84 results on '"Zheng, Q"'
Search Results
2. Programmable and robust static topological solitons in mechanical metamaterials.
- Author
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Yafei Zhang, Bo Li, Zheng, Q. S., Genin, Guy M., and Chen, C. Q.
- Abstract
Solitary, persistent wave packets called solitons hold potential to transfer information and energy across a wide range of spatial and temporal scales in physical, chemical, and biological systems. Mechanical solitons characteristically emerge either as a single wave packet or uncorrelated propagating topological entities through space and/or time, but these are notoriously difficult to control. Here, we report a theoretical framework for programming static periodic topological solitons into a metamaterial, and demonstrate its implementation in real metamaterials computationally and experimentally. The solitons are excited by deformation localizations under quasi-static compression, and arise from buckling-induced kink-antikink bands that provide domain separation barriers. The soliton number and wavelength demonstrate a previously unreported size-dependence, due to intrinsic length scales. We identify that these unanticipated solitons stem from displacive phase transitions with periodic topological excitations captured by the well-known φ
4 theory. Results reveal pathways for robust regularizations of stochastic responses of metamaterials. [ABSTRACT FROM AUTHOR]- Published
- 2019
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3. The effects of forest canopy shading and turbulence on boundary layer ozone
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Makar, P. A., primary, Staebler, R. M., additional, Akingunola, A., additional, Zhang, J., additional, McLinden, C., additional, Kharol, S. K., additional, Pabla, B., additional, Cheung, P., additional, and Zheng, Q., additional
- Published
- 2017
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4. Efficacy and safety of GLP-1 analog ecnoglutide in adults with type 2 diabetes: a randomized, double-blind, placebo-controlled phase 2 trial.
- Author
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Zhu D, Wang W, Tong G, Ma G, Ma J, Han J, Zhang X, Liu Y, Gan S, Qin H, Zheng Q, Ning J, Zhu Z, Guo M, Bu Y, Li Y, Jones CL, Fenaux M, Junaidi MK, Xu S, and Pan H
- Subjects
- Humans, Middle Aged, Male, Female, Double-Blind Method, Adult, Blood Glucose drug effects, Blood Glucose metabolism, Hypoglycemic Agents therapeutic use, Hypoglycemic Agents adverse effects, Hypoglycemic Agents administration & dosage, Aged, Treatment Outcome, Body Weight drug effects, Diabetes Mellitus, Type 2 drug therapy, Diabetes Mellitus, Type 2 blood, Glucagon-Like Peptide 1 analogs & derivatives, Glucagon-Like Peptide 1 therapeutic use, Glycated Hemoglobin metabolism
- Abstract
Glucagon-like peptide-1 (GLP-1) analogs are important therapeutics for type 2 diabetes and obesity. Ecnoglutide (XW003) is a novel, long-acting GLP-1 analog. We conducted a Phase 2, randomized, double-blind, placebo-controlled study enrolling 145 adults with T2DM. Participants were randomized to 0.4, 0.8, or 1.2 mg ecnoglutide or placebo as once-weekly injections for 20 weeks. The primary objective was to evaluate the efficacy of ecnoglutide, as measured by HbA1c change from baseline at Week 20. Secondary endpoints included body weight, glucose and lipid parameters, as well as safety. We show that, at end of treatment, the 0.4, 0.8, and 1.2 mg groups had statistically significant HbA1c reductions from baseline of -1.81%, -1.90%, and -2.39%, respectively, compared to -0.55% for placebo (P < 0.0001). At end of treatment, 71.9% of the 1.2 mg group had HbA1c ≤ 6.5% versus 9.1% on placebo, and 33.3% had body weight reductions ≥5% versus 3.0% for placebo. Ecnoglutide was generally safe and well tolerated. China Drug Trials Registry CTR20211014., (© 2024. The Author(s).)
- Published
- 2024
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5. Water-catalyzed iron-molybdenum carbyne formation in bimetallic acetylene transformation.
- Author
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Zhai X, Xue M, Zhao Q, Zheng Q, Song D, Tung CH, and Wang W
- Abstract
Transition metal carbyne complexes are of fundamental importance in carbon-carbon bond formation, alkyne metathesis, and alkyne coupling reactions. Most reported iron carbyne complexes are stabilized by incorporating heteroatoms. Here we show the synthesis of bioinspired FeMo heterobimetallic carbyne complexes by the conversion of C
2 H2 through a diverse series of intermediates. Key reactions discovered include the reduction of a μ-η2 :η2 -C2 H2 ligand with a hydride to produce a vinyl ligand (μ-η1 :η2 -CH = CH2 ), tautomerization of the vinyl ligand to a carbyne (μ-CCH3 ), and protonation of either the vinyl or the carbyne compound to form a hydrido carbyne heterobimetallic complex. Mechanistic studies unveil the pivotal role of H2 O as a proton shuttle, facilitating the proton transfer that converts the vinyl group to a bridging carbyne., (© 2024. The Author(s).)- Published
- 2024
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6. Convergent alterations in the tumor microenvironment of MYC-driven human and murine prostate cancer.
- Author
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Graham MK, Wang R, Chikarmane R, Abel B, Vaghasia A, Gupta A, Zheng Q, Hicks J, Sysa-Shah P, Pan X, Castagna N, Liu J, Meyers J, Skaist A, Zhang Y, Rubenstein M, Schuebel K, Simons BW, Bieberich CJ, Nelson WG, Lupold SE, DeWeese TL, De Marzo AM, and Yegnasubramanian S
- Subjects
- Male, Humans, Animals, Mice, Gene Expression Regulation, Neoplastic, Signal Transduction, Single-Cell Analysis, Disease Models, Animal, Cell Communication, Carcinogenesis genetics, Carcinogenesis pathology, Mice, Transgenic, RNA-Seq, Tumor Microenvironment genetics, Prostatic Neoplasms genetics, Prostatic Neoplasms pathology, Prostatic Neoplasms metabolism, Proto-Oncogene Proteins c-myc metabolism, Proto-Oncogene Proteins c-myc genetics
- Abstract
How prostate cancer cells and their precursors mediate changes in the tumor microenvironment (TME) to drive prostate cancer progression is unclear, in part due to the inability to longitudinally study the disease evolution in human tissues. To overcome this limitation, we perform extensive single-cell RNA-sequencing (scRNA-seq) and molecular pathology of the comparative biology between human prostate cancer and key stages in the disease evolution of a genetically engineered mouse model (GEMM) of prostate cancer. Our studies of human tissues reveal that cancer cell-intrinsic activation of MYC signaling is a common denominator across the well-known molecular and pathological heterogeneity of human prostate cancer. Cell communication network and pathway analyses in GEMMs show that MYC oncogene-expressing neoplastic cells, directly and indirectly, reprogram the TME during carcinogenesis, leading to a convergence of cell state alterations in neighboring epithelial, immune, and fibroblast cell types that parallel key findings in human prostate cancer., (© 2024. The Author(s).)
- Published
- 2024
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7. Systematic multi-trait AAV capsid engineering for efficient gene delivery.
- Author
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Eid FE, Chen AT, Chan KY, Huang Q, Zheng Q, Tobey IG, Pacouret S, Brauer PP, Keyes C, Powell M, Johnston J, Zhao B, Lage K, Tarantal AF, Chan YA, and Deverman BE
- Subjects
- Animals, Humans, Mice, Transduction, Genetic, Gene Transfer Techniques, Machine Learning, Genetic Therapy methods, Macaca, Hepatocytes metabolism, HEK293 Cells, Genetic Engineering methods, Dependovirus genetics, Genetic Vectors genetics, Capsid metabolism, Capsid Proteins genetics, Capsid Proteins metabolism, Liver metabolism
- Abstract
Broadening gene therapy applications requires manufacturable vectors that efficiently transduce target cells in humans and preclinical models. Conventional selections of adeno-associated virus (AAV) capsid libraries are inefficient at searching the vast sequence space for the small fraction of vectors possessing multiple traits essential for clinical translation. Here, we present Fit4Function, a generalizable machine learning (ML) approach for systematically engineering multi-trait AAV capsids. By leveraging a capsid library that uniformly samples the manufacturable sequence space, reproducible screening data are generated to train accurate sequence-to-function models. Combining six models, we designed a multi-trait (liver-targeted, manufacturable) capsid library and validated 88% of library variants on all six predetermined criteria. Furthermore, the models, trained only on mouse in vivo and human in vitro Fit4Function data, accurately predicted AAV capsid variant biodistribution in macaque. Top candidates exhibited production yields comparable to AAV9, efficient murine liver transduction, up to 1000-fold greater human hepatocyte transduction, and increased enrichment relative to AAV9 in a screen for liver transduction in macaques. The Fit4Function strategy ultimately makes it possible to predict cross-species traits of peptide-modified AAV capsids and is a critical step toward assembling an ML atlas that predicts AAV capsid performance across dozens of traits., (© 2024. The Author(s).)
- Published
- 2024
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8. C-JUN overexpressing CAR-T cells in acute myeloid leukemia: preclinical characterization and phase I trial.
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Zuo S, Li C, Sun X, Deng B, Zhang Y, Han Y, Ling Z, Xu J, Duan J, Wang Z, Yu X, Zheng Q, Xu X, Zong J, Tian Z, Shan L, Tang K, Huang H, Song Y, Niu Q, Zhou D, Feng S, Han Z, Wang G, Wu T, Pan J, and Feng X
- Subjects
- Humans, Middle Aged, Male, Female, Animals, T-Lymphocytes immunology, T-Lymphocytes metabolism, Aged, Adult, Cell Line, Tumor, Mice, Leukemia, Myeloid, Acute therapy, Leukemia, Myeloid, Acute genetics, Leukemia, Myeloid, Acute metabolism, Receptors, Chimeric Antigen metabolism, Receptors, Chimeric Antigen immunology, Receptors, Chimeric Antigen genetics, Immunotherapy, Adoptive methods, Proto-Oncogene Proteins c-jun metabolism
- Abstract
Chimeric antigen receptor (CAR) T cells show suboptimal efficacy in acute myeloid leukemia (AML). We find that CAR T cells exposed to myeloid leukemia show impaired activation and cytolytic function, accompanied by impaired antigen receptor downstream calcium, ZAP70, ERK, and C-JUN signaling, compared to those exposed to B-cell leukemia. These defects are caused in part by the high expression of CD155 by AML. Overexpressing C-JUN, but not other antigen receptor downstream components, maximally restores anti-tumor function. C-JUN overexpression increases costimulatory molecules and cytokines through reinvigoration of ERK or transcriptional activation, independent of anti-exhaustion. We conduct an open-label, non-randomized, single-arm, phase I trial of C-JUN-overexpressing CAR-T in AML (NCT04835519) with safety and efficacy as primary and secondary endpoints, respectively. Of the four patients treated, one has grade 4 (dose-limiting toxicity) and three have grade 1-2 cytokine release syndrome. Two patients have no detectable bone marrow blasts and one patient has blast reduction after treatment. Thus, overexpressing C-JUN endows CAR-T efficacy in AML., (© 2024. The Author(s).)
- Published
- 2024
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9. Robust structural superlubricity under gigapascal pressures.
- Author
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Sun T, Gao E, Jia X, Bian J, Wang Z, Ma M, Zheng Q, and Xu Z
- Abstract
Structural superlubricity (SSL) is a state of contact with no wear and ultralow friction. SSL has been characterized at contact with van der Waals (vdW) layered materials, while its stability under extreme loading conditions has not been assessed. By designing both self-mated and non-self-mated vdW contacts with materials chosen for their high strengths, we report outstanding robustness of SSL under very high pressures in experiments. The incommensurate self-mated vdW contact between graphite interfaces can maintain the state of SSL under a pressure no lower than 9.45 GPa, and the non-self-mated vdW contact between a tungsten tip and graphite substrate remains stable up to 3.74 GPa. Beyond this critical pressure, wear is activated, signaling the breakdown of vdW contacts and SSL. This unexpectedly strong pressure-resistance and wear-free feature of SSL breaks down the picture of progressive wear. Atomistic simulations show that lattice destruction at the vdW contact by pressure-assisted bonding triggers wear through shear-induced tearing of the single-atomic layers. The correlation between the breakdown pressure and material properties shows that the bulk modulus and the first ionization energy are the most relevant factors, indicating the combined structural and electronic effects. Impressively, the breakdown pressures defined by the SSL interface could even exceed the strength of materials in contact, demonstrating the robustness of SSL. These findings offer a fundamental understanding of wear at the vdW contacts and guide the design of SSL-enabled applications., (© 2024. The Author(s).)
- Published
- 2024
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10. Highly selective urea electrooxidation coupled with efficient hydrogen evolution.
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Zhan G, Hu L, Li H, Dai J, Zhao L, Zheng Q, Zou X, Shi Y, Wang J, Hou W, Yao Y, and Zhang L
- Abstract
Electrochemical urea oxidation offers a sustainable avenue for H
2 production and wastewater denitrification within the water-energy nexus; however, its wide application is limited by detrimental cyanate or nitrite production instead of innocuous N2 . Herein we demonstrate that atomically isolated asymmetric Ni-O-Ti sites on Ti foam anode achieve a N2 selectivity of 99%, surpassing the connected symmetric Ni-O-Ni counterparts in documented Ni-based electrocatalysts with N2 selectivity below 55%, and also deliver a H2 evolution rate of 22.0 mL h-1 when coupled to a Pt counter cathode under 213 mA cm-2 at 1.40 VRHE . These asymmetric sites, featuring oxygenophilic Ti adjacent to Ni, favor interaction with the carbonyl over amino groups in urea, thus preventing premature resonant C⎓N bond breakage before intramolecular N-N coupling towards N2 evolution. A prototype device powered by a commercial Si photovoltaic cell is further developed for solar-powered on-site urine processing and decentralized H2 production., (© 2024. The Author(s).)- Published
- 2024
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11. The thioredoxin system determines CHK1 inhibitor sensitivity via redox-mediated regulation of ribonucleotide reductase activity.
- Author
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Prasad CB, Oo A, Liu Y, Qiu Z, Zhong Y, Li N, Singh D, Xin X, Cho YJ, Li Z, Zhang X, Yan C, Zheng Q, Wang QE, Guo D, Kim B, and Zhang J
- Subjects
- Humans, Cell Line, Tumor, Protein Kinase Inhibitors pharmacology, Ribonucleoside Diphosphate Reductase metabolism, Ribonucleoside Diphosphate Reductase genetics, Ribonucleotide Reductases metabolism, Ribonucleotide Reductases antagonists & inhibitors, Drug Synergism, Animals, Checkpoint Kinase 1 metabolism, Checkpoint Kinase 1 antagonists & inhibitors, Oxidation-Reduction drug effects, Thioredoxins metabolism, Auranofin pharmacology, Carcinoma, Non-Small-Cell Lung drug therapy, Carcinoma, Non-Small-Cell Lung metabolism, Carcinoma, Non-Small-Cell Lung pathology, Carcinoma, Non-Small-Cell Lung genetics, Lung Neoplasms drug therapy, Lung Neoplasms metabolism, Lung Neoplasms pathology, Lung Neoplasms genetics
- Abstract
Checkpoint kinase 1 (CHK1) is critical for cell survival under replication stress (RS). CHK1 inhibitors (CHK1i's) in combination with chemotherapy have shown promising results in preclinical studies but have displayed minimal efficacy with substantial toxicity in clinical trials. To explore combinatorial strategies that can overcome these limitations, we perform an unbiased high-throughput screen in a non-small cell lung cancer (NSCLC) cell line and identify thioredoxin1 (Trx1), a major component of the mammalian antioxidant-system, as a determinant of CHK1i sensitivity. We establish a role for redox recycling of RRM1, the larger subunit of ribonucleotide reductase (RNR), and a depletion of the deoxynucleotide pool in this Trx1-mediated CHK1i sensitivity. Further, the TrxR inhibitor auranofin, an approved anti-rheumatoid arthritis drug, shows a synergistic interaction with CHK1i via interruption of the deoxynucleotide pool. Together, we show a pharmacological combination to treat NSCLC that relies on a redox regulatory link between the Trx system and mammalian RNR activity., (© 2024. The Author(s).)
- Published
- 2024
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12. An adeno-associated virus variant enabling efficient ocular-directed gene delivery across species.
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Luo S, Jiang H, Li Q, Qin Y, Yang S, Li J, Xu L, Gou Y, Zhang Y, Liu F, Ke X, Zheng Q, and Sun X
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- Animals, Mice, Rabbits, Humans, Gene Transfer Techniques, Macular Degeneration therapy, Macular Degeneration genetics, Macular Degeneration pathology, Disease Models, Animal, Capsid Proteins genetics, Capsid Proteins metabolism, Transduction, Genetic, Vascular Endothelial Growth Factor A genetics, Vascular Endothelial Growth Factor A metabolism, Mice, Inbred C57BL, Retina metabolism, Retina virology, Male, HEK293 Cells, Dependovirus genetics, Genetic Vectors genetics, Genetic Vectors administration & dosage, Genetic Therapy methods, Retinal Pigment Epithelium metabolism, Retinal Pigment Epithelium virology, Choroidal Neovascularization therapy, Choroidal Neovascularization genetics
- Abstract
Recombinant adeno-associated viruses (rAAVs) have emerged as promising gene therapy vectors due to their proven efficacy and safety in clinical applications. In non-human primates (NHPs), rAAVs are administered via suprachoroidal injection at a higher dose. However, high doses of rAAVs tend to increase additional safety risks. Here, we present a novel AAV capsid (AAVv128), which exhibits significantly enhanced transduction efficiency for photoreceptors and retinal pigment epithelial (RPE) cells, along with a broader distribution across the layers of retinal tissues in different animal models (mice, rabbits, and NHPs) following intraocular injection. Notably, the suprachoroidal delivery of AAVv128-anti-VEGF vector completely suppresses the Grade IV lesions in a laser-induced choroidal neovascularization (CNV) NHP model for neovascular age-related macular degeneration (nAMD). Furthermore, cryo-EM analysis at 2.1 Å resolution reveals that the critical residues of AAVv128 exhibit a more robust advantage in AAV binding, the nuclear uptake and endosome escaping. Collectively, our findings highlight the potential of AAVv128 as a next generation ocular gene therapy vector, particularly using the suprachoroidal delivery route., (© 2024. The Author(s).)
- Published
- 2024
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13. A patient-specific lung cancer assembloid model with heterogeneous tumor microenvironments.
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Zhang Y, Hu Q, Pei Y, Luo H, Wang Z, Xu X, Zhang Q, Dai J, Wang Q, Fan Z, Fang Y, Ye M, Li B, Chen M, Xue Q, Zheng Q, Zhang S, Huang M, Zhang T, Gu J, and Xiong Z
- Subjects
- Humans, Tumor Microenvironment, Organoids pathology, Precision Medicine methods, Lung Neoplasms genetics, Lung Neoplasms pathology
- Abstract
Cancer models play critical roles in basic cancer research and precision medicine. However, current in vitro cancer models are limited by their inability to mimic the three-dimensional architecture and heterogeneous tumor microenvironments (TME) of in vivo tumors. Here, we develop an innovative patient-specific lung cancer assembloid (LCA) model by using droplet microfluidic technology based on a microinjection strategy. This method enables precise manipulation of clinical microsamples and rapid generation of LCAs with good intra-batch consistency in size and cell composition by evenly encapsulating patient tumor-derived TME cells and lung cancer organoids inside microgels. LCAs recapitulate the inter- and intratumoral heterogeneity, TME cellular diversity, and genomic and transcriptomic landscape of their parental tumors. LCA model could reconstruct the functional heterogeneity of cancer-associated fibroblasts and reflect the influence of TME on drug responses compared to cancer organoids. Notably, LCAs accurately replicate the clinical outcomes of patients, suggesting the potential of the LCA model to predict personalized treatments. Collectively, our studies provide a valuable method for precisely fabricating cancer assembloids and a promising LCA model for cancer research and personalized medicine., (© 2024. The Author(s).)
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- 2024
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14. Atomically precise engineering of spin-orbit polarons in a kagome magnetic Weyl semimetal.
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Chen H, Xing Y, Tan H, Huang L, Zheng Q, Huang Z, Han X, Hu B, Ye Y, Li Y, Xiao Y, Lei H, Qiu X, Liu E, Yang H, Wang Z, Yan B, and Gao HJ
- Abstract
Atomically precise defect engineering is essential to manipulate the properties of emerging topological quantum materials for practical quantum applications. However, this remains challenging due to the obstacles in modifying the typically complex crystal lattice with atomic precision. Here, we report the atomically precise engineering of the vacancy-localized spin-orbit polarons in a kagome magnetic Weyl semimetal Co
3 Sn2 S2 , using scanning tunneling microscope. We achieve the step-by-step repair of the selected vacancies, leading to the formation of artificial sulfur vacancies with elaborate geometry. We find that that the bound states localized around these vacancies undergo a symmetry dependent energy shift towards Fermi level with increasing vacancy size. As the vacancy size increases, the localized magnetic moments of spin-orbit polarons become tunable and eventually become itinerantly negative due to spin-orbit coupling in the kagome flat band. These findings provide a platform for engineering atomic quantum states in topological quantum materials at the atomic scale., (© 2024. The Author(s).)- Published
- 2024
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15. Giant electric field-induced second harmonic generation in polar skyrmions.
- Author
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Wang S, Li W, Deng C, Hong Z, Gao HB, Li X, Gu Y, Zheng Q, Wu Y, Evans PG, Li JF, Nan CW, and Li Q
- Abstract
Electric field-induced second harmonic generation allows electrically controlling nonlinear light-matter interactions crucial for emerging integrated photonics applications. Despite its wide presence in materials, the figures-of-merit of electric field-induced second harmonic generation are yet to be elevated to enable novel device functionalities. Here, we show that the polar skyrmions, a topological phase spontaneously formed in PbTiO
3 /SrTiO3 ferroelectric superlattices, exhibit a high comprehensive electric field-induced second harmonic generation performance. The second-order nonlinear susceptibility and modulation depth, measured under non-resonant 800 nm excitation, reach ~54.2 pm V-1 and ~664% V-1 , respectively, and high response bandwidth (higher than 10 MHz), wide operating temperature range (up to ~400 K) and good fatigue resistance (>1010 cycles) are also demonstrated. Through combined in-situ experiments and phase-field simulations, we establish the microscopic links between the exotic polarization configuration and field-induced transition paths of the skyrmions and their electric field-induced second harmonic generation response. Our study not only presents a highly competitive thin-film material ready for constructing on-chip devices, but opens up new avenues of utilizing topological polar structures in the fields of photonics and optoelectronics., (© 2024. The Author(s).)- Published
- 2024
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16. Aggresome formation promotes ASK1/JNK signaling activation and stemness maintenance in ovarian cancer.
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Chen Y, Qiang Y, Fan J, Zheng Q, Yan L, Fan G, Song X, Zhang N, Lv Q, Xiong J, Wang J, Cao J, Liu Y, Xiong J, Zhang W, and Li F
- Subjects
- Humans, Female, Proteins metabolism, Peptides metabolism, Protein Processing, Post-Translational, Ubiquitin-Specific Proteases metabolism, MAP Kinase Signaling System, Ovarian Neoplasms genetics
- Abstract
Aggresomes are the product of misfolded protein aggregation, and the presence of aggresomes has been correlated with poor prognosis in cancer patients. However, the exact role of aggresomes in tumorigenesis and cancer progression remains largely unknown. Herein, the multiomics screening reveal that OTUD1 protein plays an important role in retaining ovarian cancer stem cell (OCSC) properties. Mechanistically, the elevated OTUD1 protein levels lead to the formation of OTUD1-based cytoplasmic aggresomes, which is mediated by a short peptide located in the intrinsically disordered OTUD1 N-terminal region. Furthermore, OTUD1-based aggresomes recruit ASK1 via protein-protein interactions, which in turn stabilize ASK1 in a deubiquitinase-independent manner and activate the downstream JNK signaling pathway for OCSC maintenance. Notably, the disruption of OTUD1-based aggresomes or treatment with ASK1/JNK inhibitors, including ibrutinib, an FDA-approved drug that was recently identified as an MKK7 inhibitor, effectively reduced OCSC stemness (OSCS) of OTUD1
high ovarian cancer cells. In summary, our work suggests that aggresome formation in tumor cells could function as a signaling hub and that aggresome-based therapy has translational potential for patients with OTUD1high ovarian cancer., (© 2024. The Author(s).)- Published
- 2024
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17. A dicarbonate solvent electrolyte for high performance 5 V-Class Lithium-based batteries.
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Zhang X, Xu P, Duan J, Lin X, Sun J, Shi W, Xu H, Dou W, Zheng Q, Yuan R, Wang J, Zhang Y, Yu S, Chen Z, Zheng M, Gohy JF, Dong Q, and Vlad A
- Abstract
Rechargeable lithium batteries using 5 V positive electrode materials can deliver considerably higher energy density as compared to state-of-the-art lithium-ion batteries. However, their development remains plagued by the lack of electrolytes with concurrent anodic stability and Li metal compatibility. Here we report a new electrolyte based on dimethyl 2,5-dioxahexanedioate solvent for 5 V-class batteries. Benefiting from the particular chemical structure, weak interaction with lithium cation and resultant peculiar solvation structure, the resulting electrolyte not only enables stable, dendrite-free lithium plating-stripping, but also displays anodic stability up to 5.2 V (vs. Li/Li
+ ), in additive or co-solvent-free formulation, and at low salt concentration of 1 M. Consequently, the Li | |LiNi0.5 Mn1.5 O4 cells using the 1 M LiPF6 in 2,5-dioxahexanedioate based electrolyte retain >97% of the initial capacity after 250 cycles, outperforming the conventional carbonate-based electrolyte formulations, making this, and potentially other dicarbonate solvents promising for future Lithium-based battery practical explorations., (© 2024. The Author(s).)- Published
- 2024
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18. Animating hydrogel knotbots with topology-invoked self-regulation.
- Author
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Zhu QL, Liu W, Khoruzhenko O, Breu J, Hong W, Zheng Q, and Wu ZL
- Abstract
Steering soft robots in a self-regulated manner remains a grand challenge, which often requires continuous symmetry breaking and recovery steps for persistent motion. Although structural morphology is found significant for robotic functions, geometric topology has rarely been considered and appreciated. Here we demonstrate a series of knotbots, namely hydrogel-based robots with knotted structures, capable of autonomous rolling and spinning/rotating motions. With symmetry broken by external stimuli and restored by self-regulation, the coupling between self-constraint-induced prestress and photothermal strain animates the knotbots continuously. Experiments and simulations reveal that nonequilibrium processes are regulated dynamically and cooperatively by self-constraints, active deformations, and self-shadowing effect of the photo-responsive gel. The active motions enable the knotbots to execute tasks including gear rotation and rod climbing. This work paves the way to devise advanced soft robots with self-regulated sustainable motions by harnessing the topology., (© 2024. The Author(s).)
- Published
- 2024
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19. Spin polarized Fe 1 -Ti pairs for highly efficient electroreduction nitrate to ammonia.
- Author
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Dai J, Tong Y, Zhao L, Hu Z, Chen CT, Kuo CY, Zhan G, Wang J, Zou X, Zheng Q, Hou W, Wang R, Wang K, Zhao R, Gu XK, Yao Y, and Zhang L
- Abstract
Electrochemical nitrate reduction to ammonia offers an attractive solution to environmental sustainability and clean energy production but suffers from the sluggish *NO hydrogenation with the spin-state transitions. Herein, we report that the manipulation of oxygen vacancies can contrive spin-polarized Fe
1 -Ti pairs on monolithic titanium electrode that exhibits an attractive NH3 yield rate of 272,000 μg h-1 mgFe -1 and a high NH3 Faradic efficiency of 95.2% at -0.4 V vs. RHE, far superior to the counterpart with spin-depressed Fe1 -Ti pairs (51000 μg h-1 mgFe -1 ) and the mostly reported electrocatalysts. The unpaired spin electrons of Fe and Ti atoms can effectively interact with the key intermediates, facilitating the *NO hydrogenation. Coupling a flow-through electrolyzer with a membrane-based NH3 recovery unit, the simultaneous nitrate reduction and NH3 recovery was realized. This work offers a pioneering strategy for manipulating spin polarization of electrocatalysts within pair sites for nitrate wastewater treatment., (© 2024. The Author(s).)- Published
- 2024
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20. Uncertainties in deforestation emission baseline methodologies and implications for carbon markets.
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Teo HC, Tan NHL, Zheng Q, Lim AJY, Sreekar R, Chen X, Zhou Y, Sarira TV, De Alban JDT, Tang H, Friess DA, and Koh LP
- Abstract
Carbon credits generated through jurisdictional-scale avoided deforestation projects require accurate estimates of deforestation emission baselines, but there are serious challenges to their robustness. We assessed the variability, accuracy, and uncertainty of baselining methods by applying sensitivity and variable importance analysis on a range of typically-used methods and parameters for 2,794 jurisdictions worldwide. The median jurisdiction's deforestation emission baseline varied by 171% (90% range: 87%-440%) of its mean, with a median forecast error of 0.778 times (90% range: 0.548-3.56) the actual deforestation rate. Moreover, variable importance analysis emphasised the strong influence of the deforestation projection approach. For the median jurisdiction, 68.0% of possible methods (90% range: 61.1%-85.6%) exceeded 15% uncertainty. Tropical and polar biomes exhibited larger uncertainties in carbon estimations. The use of sensitivity analyses, multi-model, and multi-source ensemble approaches could reduce variabilities and biases. These findings provide a roadmap for improving baseline estimations to enhance carbon market integrity and trust., (© 2023. The Author(s).)
- Published
- 2023
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21. Nonintrusive thermal-wave sensor for operando quantification of degradation in commercial batteries.
- Author
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Zeng Y, Shen F, Zhang B, Lee J, Chalise D, Zheng Q, Fu Y, Kaur S, Lubner SD, Battaglia VS, McCloskey BD, Tucker MC, and Prasher RS
- Abstract
Monitoring real-world battery degradation is crucial for the widespread application of batteries in different scenarios. However, acquiring quantitative degradation information in operating commercial cells is challenging due to the complex, embedded, and/or qualitative nature of most existing sensing techniques. This process is essentially limited by the type of signals used for detection. Here, we report the use of effective battery thermal conductivity (k
eff ) as a quantitative indicator of battery degradation by leveraging the strong dependence of keff on battery-structure changes. A measurement scheme based on attachable thermal-wave sensors is developed for non-embedded detection and quantitative assessment. A proof-of-concept study of battery degradation during fast charging demonstrates that the amount of lithium plating and electrolyte consumption associated with the side reactions on the graphite anode and deposited lithium can be quantitatively distinguished using our method. Therefore, this work opens the door to the quantitative evaluation of battery degradation using simple non-embedded thermal-wave sensors., (© 2023. The Author(s).)- Published
- 2023
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22. Nonredox trivalent nickel catalyzing nucleophilic electrooxidation of organics.
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Yan Y, Wang R, Zheng Q, Zhong J, Hao W, Yan S, and Zou Z
- Abstract
A thorough comprehension of the mechanism behind organic electrooxidation is crucial for the development of efficient energy conversion technology. Here, we find that trivalent nickel is capable of oxidizing organics through a nucleophilic attack and electron transfer via a nonredox process. This nonredox trivalent nickel exhibits exceptional kinetic efficiency in oxidizing organics that possess the highest occupied molecular orbital energy levels ranging from -7.4 to -6 eV (vs. Vacuum level) and the dual local softness values of nucleophilic atoms in nucleophilic functional groups, such as hydroxyls (methanol, ethanol, benzyl alcohol), carbonyls (formamide, urea, formaldehyde, glucose, and N-acetyl glucosamine), and aminos (benzylamine), ranging from -0.65 to -0.15. The rapid electrooxidation kinetics can be attributed to the isoenergetic channels created by the nucleophilic attack and the nonredox electron transfer via the unoccupied e
g orbitals of trivalent nickel (t2g 6 eg 1 ). Our findings are valuable in identifying kinetically fast organic electrooxidation on nonredox catalysts for efficient energy conversions., (© 2023. The Author(s).)- Published
- 2023
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23. Wide-temperature-range thermoelectric n-type Mg 3 (Sb,Bi) 2 with high average and peak zT values.
- Author
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Li JW, Han Z, Yu J, Zhuang HL, Hu H, Su B, Li H, Jiang Y, Chen L, Liu W, Zheng Q, and Li JF
- Abstract
Mg
3 (Sb,Bi)2 is a promising thermoelectric material suited for electronic cooling, but there is still room to optimize its low-temperature performance. This work realizes >200% enhancement in room-temperature zT by incorporating metallic inclusions (Nb or Ta) into the Mg3 (Sb,Bi)2 -based matrix. The electrical conductivity is boosted in the range of 300-450 K, whereas the corresponding Seebeck coefficients remain unchanged, leading to an exceptionally high room-temperature power factor >30 μW cm-1 K-2 ; such an unusual effect originates mainly from the modified interfacial barriers. The reduced interfacial barriers are conducive to carrier transport at low and high temperatures. Furthermore, benefiting from the reduced lattice thermal conductivity, a record-high average zT > 1.5 and a maximum zT of 2.04 at 798 K are achieved, resulting in a high thermoelectric conversion efficiency of 15%. This work demonstrates an efficient nanocomposite strategy to enhance the wide-temperature-range thermoelectric performance of n-type Mg3 (Sb,Bi)2 , broadening their potential for practical applications., (© 2023. The Author(s).)- Published
- 2023
- Full Text
- View/download PDF
24. Fully automatic transfer and measurement system for structural superlubric materials.
- Author
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Chen L, Lin C, Shi D, Huang X, Zheng Q, Nie J, and Ma M
- Abstract
Structural superlubricity, a state of nearly zero friction and no wear between two contact surfaces under relative sliding, holds immense potential for research and application prospects in micro-electro-mechanical systems devices, mechanical engineering, and energy resources. A critical step towards the practical application of structural superlubricity is the mass transfer and high throughput performance evaluation. Limited by the yield rate of material preparation, existing automated systems, such as roll printing or massive stamping, are inadequate for this task. In this paper, a machine learning-assisted system is proposed to realize fully automated selective transfer and tribological performance measurement for structural superlubricity materials. Specifically, the system has a judgment accuracy of over 98% for the selection of micro-scale graphite flakes with structural superlubricity properties and complete the 100 graphite flakes assembly array to form various pre-designed patterns within 100 mins, which is 15 times faster than manual operation. Besides, the system is capable of automatically measuring the tribological performance of over 100 selected flakes on Si
3 N4 , delivering statistical results for new interface which is beyond the reach of traditional methods. With its high accuracy, efficiency, and robustness, this machine learning-assisted system promotes the fundamental research and practical application of structural superlubricity., (© 2023. Springer Nature Limited.)- Published
- 2023
- Full Text
- View/download PDF
25. Author Correction: The isocyanide S N 2 reaction.
- Author
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Patil P, Zheng Q, Kurpiewska K, and Dömling A
- Published
- 2023
- Full Text
- View/download PDF
26. Biomimetic single Al-OH site with high acetylcholinesterase-like activity and self-defense ability for neuroprotection.
- Author
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Xu W, Cai X, Wu Y, Wen Y, Su R, Zhang Y, Huang Y, Zheng Q, Hu L, Cui X, Zheng L, Zhang S, Gu W, Song W, Guo S, and Zhu C
- Subjects
- Neuroprotection, Organophosphates, Acetylcholinesterase chemistry, Biomimetics
- Abstract
Neurotoxicity of organophosphate compounds (OPs) can catastrophically cause nervous system injury by inhibiting acetylcholinesterase (AChE) expression. Although artificial systems have been developed for indirect neuroprotection, they are limited to dissociating P-O bonds for eliminating OPs. However, these systems have failed to overcome the deactivation of AChE. Herein, we report our finding that Al
3+ is engineered onto the nodes of metal-organic framework to synthesize MOF-808-Al with enhanced Lewis acidity. The resultant MOF-808-Al efficiently mimics the catalytic behavior of AChE and has a self-defense ability to break the activity inhibition by OPs. Mechanism investigations elucidate that Al3+ Lewis acid sites with a strong polarization effect unite the highly electronegative -OH groups to form the enzyme-like catalytic center, resulting in superior substrate activation and nucleophilic attack ability with a 2.7-fold activity improvement. The multifunctional MOF-808-Al, which has satisfactory biosafety, is efficient in reducing neurotoxic effects and preventing neuronal tissue damage., (© 2023. The Author(s).)- Published
- 2023
- Full Text
- View/download PDF
27. The neglected role of abandoned cropland in supporting both food security and climate change mitigation.
- Author
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Zheng Q, Ha T, Prishchepov AV, Zeng Y, Yin H, and Koh LP
- Subjects
- Crops, Agricultural, Forests, Food Security, Conservation of Natural Resources, Climate Change, Agriculture
- Abstract
Despite the looming land scarcity for agriculture, cropland abandonment is widespread globally. Abandoned cropland can be reused to support food security and climate change mitigation. Here, we investigate the potentials and trade-offs of using global abandoned cropland for recultivation and restoring forests by natural regrowth, with spatially-explicit modelling and scenario analysis. We identify 101 Mha of abandoned cropland between 1992 and 2020, with a capability of concurrently delivering 29 to 363 Peta-calories yr
-1 of food production potential and 290 to 1,066 MtCO2 yr-1 of net climate change mitigation potential, depending on land-use suitability and land allocation strategies. We also show that applying spatial prioritization is key to maximizing the achievable potentials of abandoned cropland and demonstrate other possible approaches to further increase these potentials. Our findings offer timely insights into the potentials of abandoned cropland and can inform sustainable land management to buttress food security and climate goals., (© 2023. Springer Nature Limited.)- Published
- 2023
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28. The isocyanide S N 2 reaction.
- Author
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Patil P, Zheng Q, Kurpiewska K, and Dömling A
- Abstract
The S
N 2 nucleophilic substitution reaction is a vital organic transformation used for drug and natural product synthesis. Nucleophiles like cyanide, oxygen, nitrogen, sulfur, or phosphorous replace halogens or sulfonyl esters, forming new bonds. Isocyanides exhibit unique C-centered lone pair σ and π* orbitals, enabling diverse radical and multicomponent reactions. Despite this, their nucleophilic potential in SN 2 reactions remains unexplored. We have uncovered that isocyanides act as versatile nucleophiles in SN 2 reactions with alkyl halides. This yields highly substituted secondary amides through in situ nitrilium ion hydrolysis introducing an alternative bond break compared to classical amide synthesis. This novel 3-component process accommodates various isocyanide and electrophile structures, functional groups, scalability, late-stage drug modifications, and complex compound synthesis. This reaction greatly expands chemical diversity, nearly doubling the classical amid coupling's chemical space. Notably, the isocyanide nucleophile presents an unconventional Umpolung amide carbanion synthon (R-NHC(-) = O), an alternative to classical amide couplings., (© 2023. Springer Nature Limited.)- Published
- 2023
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29. Discovery and construction of surface kagome electronic states induced by p-d electronic hybridization in Co 3 Sn 2 S 2 .
- Author
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Huang L, Kong X, Zheng Q, Xing Y, Chen H, Li Y, Hu Z, Zhu S, Qiao J, Zhang YY, Cheng H, Cheng Z, Qiu X, Liu E, Lei H, Lin X, Wang Z, Yang H, Ji W, and Gao HJ
- Abstract
Kagome-lattice materials possess attractive properties for quantum computing applications, but their synthesis remains challenging. Herein, based on the compelling identification of the two cleavable surfaces of Co
3 Sn2 S2 , we show surface kagome electronic states (SKESs) on a Sn-terminated triangular Co3 Sn2 S2 surface. Such SKESs are imprinted by vertical p-d electronic hybridization between the surface Sn (subsurface S) atoms and the buried Co kagome-lattice network in the Co3 Sn layer under the surface. Owing to the subsequent lateral hybridization of the Sn and S atoms in a corner-sharing manner, the kagome symmetry and topological electronic properties of the Co3 Sn layer is proximate to the Sn surface. The SKESs and both hybridizations were verified via qPlus non-contact atomic force microscopy (nc-AFM) and density functional theory calculations. The construction of SKESs with tunable properties can be achieved by the atomic substitution of surface Sn (subsurface S) with other group III-V elements (Se or Te), which was demonstrated theoretically. This work exhibits the powerful capacity of nc-AFM in characterizing localized topological states and reveals the strategy for synthesis of large-area transition-metal-based kagome-lattice materials using conventional surface deposition techniques., (© 2023. Springer Nature Limited.)- Published
- 2023
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30. Bioinspired rotary flight of light-driven composite films.
- Author
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Wang D, Chen Z, Li M, Hou Z, Zhan C, Zheng Q, Wang D, Wang X, Cheng M, Hu W, Dong B, Shi F, and Sitti M
- Abstract
Light-driven actuators have great potential in different types of applications. However, it is still challenging to apply them in flying devices owing to their slow response, small deflection and force output and low frequency response. Herein, inspired by the structure of vine maple seeds, we report a helicopter-like rotary flying photoactuator (in response to 0.6 W/cm
2 near-infrared (NIR) light) with ultrafast rotation (~7200 revolutions per minute) and rapid response (~650 ms). This photoactuator is operated based on a fundamentally different mechanism that depends on the synergistic interactions between the photothermal graphene and the hygroscopic agar/silk fibroin components, the subsequent aerodynamically favorable airscrew formation, the jet propulsion, and the aerodynamics-based flying. The soft helicopter-like photoactuator exhibits controlled flight and steering behaviors, making it promising for applications in soft robotics and other miniature devices., (© 2023. Springer Nature Limited.)- Published
- 2023
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31. Author Correction: Ultrafast non-radiative dynamics of atomically thin MoSe 2 .
- Author
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Lin MF, Kochat V, Krishnamoorthy A, Bassman Oftelie L, Weninger C, Zheng Q, Zhang X, Apte A, Tiwary CS, Shen X, Li R, Kalia R, Ajayan P, Nakano A, Vashishta P, Shimojo F, Wang X, Fritz DM, and Bergmann U
- Published
- 2023
- Full Text
- View/download PDF
32. Anomalous polarization enhancement in a van der Waals ferroelectric material under pressure.
- Author
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Yao X, Bai Y, Jin C, Zhang X, Zheng Q, Xu Z, Chen L, Wang S, Liu Y, Wang J, and Zhu J
- Abstract
CuInP
2 S6 with robust room-temperature ferroelectricity has recently attracted much attention due to the spatial instability of its Cu cations and the van der Waals (vdW) layered structure. Herein, we report a significant enhancement of its remanent polarization by more than 50% from 4.06 to 6.36 µC cm-2 under a small pressure between 0.26 to 1.40 GPa. Comprehensive analysis suggests that even though the hydrostatic pressure suppresses the crystal distortion, it initially forces Cu cations to largely occupy the interlayer sites, causing the spontaneous polarization to increase. Under intermediate pressure, the condensation of Cu cations to the ground state and the polarization increase due cell volume reduction compensate each other, resulting in a constant polarization. Under high pressure, the migration of Cu cations to the center of the S octahedron dominates the polarization decrease. These findings improve our understanding of this fascinating vdW ferroelectric material, and suggest new ways to improve its properties., (© 2023. The Author(s).)- Published
- 2023
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33. Structure and proposed DNA delivery mechanism of a marine roseophage.
- Author
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Huang Y, Sun H, Wei S, Cai L, Liu L, Jiang Y, Xin J, Chen Z, Que Y, Kong Z, Li T, Yu H, Zhang J, Gu Y, Zheng Q, Li S, Zhang R, and Xia N
- Subjects
- Genome, Viral, Genes, Viral, Capsid Proteins genetics, DNA, DNA, Viral genetics, Bacteriophages genetics, Bacteriophages chemistry, Caudovirales genetics
- Abstract
Tailed bacteriophages (order, Caudovirales) account for the majority of all phages. However, the long flexible tail of siphophages hinders comprehensive investigation of the mechanism of viral gene delivery. Here, we report the atomic capsid and in-situ structures of the tail machine of the marine siphophage, vB_DshS-R4C (R4C), which infects Roseobacter. The R4C virion, comprising 12 distinct structural protein components, has a unique five-fold vertex of the icosahedral capsid that allows genome delivery. The specific position and interaction pattern of the tail tube proteins determine the atypical long rigid tail of R4C, and further provide negative charge distribution within the tail tube. A ratchet mechanism assists in DNA transmission, which is initiated by an absorption device that structurally resembles the phage-like particle, RcGTA. Overall, these results provide in-depth knowledge into the intact structure and underlining DNA delivery mechanism for the ecologically important siphophages., (© 2023. The Author(s).)
- Published
- 2023
- Full Text
- View/download PDF
34. Molecular mechanisms of Holliday junction branch migration catalyzed by an asymmetric RuvB hexamer.
- Author
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Rish AD, Shen Z, Chen Z, Zhang N, Zheng Q, and Fu TM
- Subjects
- DNA Helicases metabolism, Bacterial Proteins metabolism, Escherichia coli genetics, DNA metabolism, Nucleotides metabolism, Catalysis, DNA, Cruciform metabolism, Escherichia coli Proteins metabolism
- Abstract
The Holliday junction (HJ) is a DNA intermediate of homologous recombination, involved in many fundamental physiological processes. RuvB, an ATPase motor protein, drives branch migration of the Holliday junction with a mechanism that had yet to be elucidated. Here we report two cryo-EM structures of RuvB, providing a comprehensive understanding of HJ branch migration. RuvB assembles into a spiral staircase, ring-like hexamer, encircling dsDNA. Four protomers of RuvB contact the DNA backbone with a translocation step size of 2 nucleotides. The variation of nucleotide-binding states in RuvB supports a sequential model for ATP hydrolysis and nucleotide recycling, which occur at separate, singular positions. RuvB's asymmetric assembly also explains the 6:4 stoichiometry between the RuvB/RuvA complex, which coordinates HJ migration in bacteria. Taken together, we provide a mechanistic understanding of HJ branch migration facilitated by RuvB, which may be universally shared by prokaryotic and eukaryotic organisms., (© 2023. The Author(s).)
- Published
- 2023
- Full Text
- View/download PDF
35. Extreme fast charging of commercial Li-ion batteries via combined thermal switching and self-heating approaches.
- Author
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Zeng Y, Zhang B, Fu Y, Shen F, Zheng Q, Chalise D, Miao R, Kaur S, Lubner SD, Tucker MC, Battaglia V, Dames C, and Prasher RS
- Abstract
The mass adoption of electric vehicles is hindered by the inadequate extreme fast charging (XFC) performance (i.e., less than 15 min charging time to reach 80% state of charge) of commercial high-specific-energy (i.e., >200 Wh/kg) lithium-ion batteries (LIBs). Here, to enable the XFC of commercial LIBs, we propose the regulation of the battery's self-generated heat via active thermal switching. We demonstrate that retaining the heat during XFC with the switch OFF boosts the cell's kinetics while dissipating the heat after XFC with the switch ON reduces detrimental reactions in the battery. Without modifying cell materials or structures, the proposed XFC approach enables reliable battery operation by applying <15 min of charge and 1 h of discharge. These results are almost identical regarding operativity for the same battery type tested applying a 1 h of charge and 1 h of discharge, thus, meeting the XFC targets set by the United States Department of Energy. Finally, we also demonstrate the feasibility of integrating the XFC approach in a commercial battery thermal management system., (© 2023. The Author(s).)
- Published
- 2023
- Full Text
- View/download PDF
36. Robust microscale structural superlubricity between graphite and nanostructured surface.
- Author
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Huang X, Li T, Wang J, Xia K, Tan Z, Peng D, Xiang X, Liu B, Ma M, and Zheng Q
- Abstract
Structural superlubricity is a state of nearly zero friction and no wear between two contacted solid surfaces. However, such state has a certain probability of failure due to the edge defects of graphite flake. Here, we achieve robust structural superlubricity state between microscale graphite flakes and nanostructured silicon surfaces under ambient condition. We find that the friction is always less than 1 μN, the differential friction coefficient is on the order of 10
-4 , without observable wear. This is attributed to the edge warping of graphite flake on the nanostructured surface under concentrated force, which eliminate the edge interaction between the graphite flake and the substrate. This study not only challenges the traditional understanding in tribology and structural superlubricity that rougher surfaces lead to higher friction and lead to wear, thereby reducing roughness requirements, but also demonstrates that a graphite flake with a single crystal surface that does not come into edge contact with the substrate can consistently achieve robust structural superlubricity state with any non-van der Waals material in atmospheric conditions. Additionally, the study provides a general surface modification method that enables the widespread application of structural superlubricity technology in atmospheric environments., (© 2023. The Author(s).)- Published
- 2023
- Full Text
- View/download PDF
37. Lifetime over 10000 hours for organic solar cells with Ir/IrO x electron-transporting layer.
- Author
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Li Y, Huang B, Zhang X, Ding J, Zhang Y, Xiao L, Wang B, Cheng Q, Huang G, Zhang H, Yang Y, Qi X, Zheng Q, Zhang Y, Qiu X, Liang M, and Zhou H
- Abstract
The stability of organic solar cells is a key issue to promote practical applications. Herein, we demonstrate that the device performance of organic solar cells is enhanced by an Ir/IrO
x electron-transporting layer, benefiting from its suitable work function and heterogeneous distribution of surface energy in nanoscale. Notably, the champion Ir/IrOx -based devices exhibit superior stabilities under shelf storing (T80 = 56696 h), thermal aging (T70 = 13920 h), and maximum power point tracking (T80 = 1058 h), compared to the ZnO-based devices. It can be attributed to the stable morphology of photoactive layer resulting from the optimized molecular distribution of the donor and acceptor and the absence of photocatalysis in the Ir/IrOx -based devices, which helps to maintain the improved charge extraction and inhibited charge recombination in the aged devices. This work provides a reliable and efficient electron-transporting material toward stable organic solar cells., (© 2023. The Author(s).)- Published
- 2023
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- View/download PDF
38. Twisted bilayer zigzag-graphene nanoribbon junctions with tunable edge states.
- Author
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Wang D, Bao DL, Zheng Q, Wang CT, Wang S, Fan P, Mishra S, Tao L, Xiao Y, Huang L, Feng X, Müllen K, Zhang YY, Fasel R, Ruffieux P, Du S, and Gao HJ
- Abstract
Stacking two-dimensional layered materials such as graphene and transitional metal dichalcogenides with nonzero interlayer twist angles has recently become attractive because of the emergence of novel physical properties. Stacking of one-dimensional nanomaterials offers the lateral stacking offset as an additional parameter for modulating the resulting material properties. Here, we report that the edge states of twisted bilayer zigzag graphene nanoribbons (TBZGNRs) can be tuned with both the twist angle and the stacking offset. Strong edge state variations in the stacking region are first revealed by density functional theory (DFT) calculations. We construct and characterize twisted bilayer zigzag graphene nanoribbon (TBZGNR) systems on a Au(111) surface using scanning tunneling microscopy. A detailed analysis of three prototypical orthogonal TBZGNR junctions exhibiting different stacking offsets by means of scanning tunneling spectroscopy reveals emergent near-zero-energy states. From a comparison with DFT calculations, we conclude that the emergent edge states originate from the formation of flat bands whose energy and spin degeneracy are highly tunable with the stacking offset. Our work highlights fundamental differences between 2D and 1D twistronics and spurs further investigation of twisted one-dimensional systems., (© 2023. The Author(s).)
- Published
- 2023
- Full Text
- View/download PDF
39. Accelerated water activation and stabilized metal-organic framework via constructing triangular active-regions for ampere-level current density hydrogen production.
- Author
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Cheng F, Peng X, Hu L, Yang B, Li Z, Dong CL, Chen JL, Hsu LC, Lei L, Zheng Q, Qiu M, Dai L, and Hou Y
- Abstract
Two-dimensional metal-organic frameworks (MOFs) have been explored as effective electrocatalysts for hydrogen evolution reaction (HER). However, the sluggish water activation kinetics and structural instability under ultrahigh-current density hinder their large-scale industrial applications. Herein, we develop a universal ligand regulation strategy to build well-aligned Ni-benzenedicarboxylic acid (BDC)-based MOF nanosheet arrays with S introducing (S-NiBDC). Benefiting from the closer p-band center to the Fermi level with strong electron transferability, S-NiBDC array exhibits a low overpotential of 310 mV to attain 1.0 A cm
-2 with high stability in alkaline electrolyte. We speculate the newly-constructed triangular "Ni2 -S1 " motif as the improved HER active region based on detailed mechanism analysis and structural characterization, and the enhanced covalency of Ni-O bonds by S introducing stabilizes S-NiBDC structure. Experimental observations and theoretical calculations elucidate that such Ni sites in "Ni2 -S1 " center distinctly accelerate the water activation kinetics, while the S site readily captures the H atom as the optimal HER active site, boosting the whole HER activity., (© 2022. The Author(s).)- Published
- 2022
- Full Text
- View/download PDF
40. Selective activation of four quasi-equivalent C-H bonds yields N-doped graphene nanoribbons with partial corannulene motifs.
- Author
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Gao Y, Huang L, Cao Y, Richter M, Qi J, Zheng Q, Yang H, Ma J, Chang X, Fu X, Palma CA, Lu H, Zhang YY, Cheng Z, Lin X, Ouyang M, Feng X, Du S, and Gao HJ
- Abstract
Selective C-H bond activation is one of the most challenging topics for organic reactions. The difficulties arise not only from the high C-H bond dissociation enthalpies but also the existence of multiple equivalent/quasi-equivalent reaction sites in organic molecules. Here, we successfully achieve the selective activation of four quasi-equivalent C-H bonds in a specially designed nitrogen-containing polycyclic hydrocarbon (N-PH). Density functional theory calculations reveal that the adsorption of N-PH on Ag(100) differentiates the activity of the four ortho C(sp
3 ) atoms in the N-heterocycles into two groups, suggesting a selective dehydrogenation, which is demonstrated by sequential-annealing experiments of N-PH/Ag(100). Further annealing leads to the formation of N-doped graphene nanoribbons with partial corannulene motifs, realized by the C-H bond activation process. Our work provides a route of designing precursor molecules with ortho C(sp3 ) atom in an N-heterocycle to realize surface-induced selective dehydrogenation in quasi-equivalent sites., (© 2022. The Author(s).)- Published
- 2022
- Full Text
- View/download PDF
41. Condensation droplet sieve.
- Author
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Ma C, Chen L, Wang L, Tong W, Chu C, Yuan Z, Lv C, and Zheng Q
- Abstract
Large droplets emerging during dropwise condensation impair surface properties such as anti-fogging/frosting ability and heat transfer efficiency. How to spontaneously detach massive randomly distributed droplets with controlled sizes has remained a challenge. Herein, we present a solution called condensation droplet sieve, through fabricating microscale thin-walled lattice structures coated with a superhydrophobic layer. Growing droplets were observed to jump off this surface once becoming slightly larger than the lattices. The maximum radius and residual volume of droplets were strictly confined to 16 μm and 3.2 nl/mm
2 respectively. We reveal that this droplet radius cut off is attributed to the large tolerance of coalescence mismatch for jumping and effective isolation of droplets between neighboring lattices. Our work brings forth a strategy for the design and fabrication of high-performance anti-dew materials., (© 2022. The Author(s).)- Published
- 2022
- Full Text
- View/download PDF
42. Identification of a cross-neutralizing antibody that targets the receptor binding site of H1N1 and H5N1 influenza viruses.
- Author
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Li T, Chen J, Zheng Q, Xue W, Zhang L, Rong R, Zhang S, Wang Q, Hong M, Zhang Y, Cui L, He M, Lu Z, Zhang Z, Chi X, Li J, Huang Y, Wang H, Tang J, Ying D, Zhou L, Wang Y, Yu H, Zhang J, Gu Y, Chen Y, Li S, and Xia N
- Subjects
- Antibodies, Monoclonal, Antibodies, Neutralizing, Antibodies, Viral, Binding Sites, Broadly Neutralizing Antibodies, Hemagglutinin Glycoproteins, Influenza Virus, Humans, Influenza A Virus, H1N1 Subtype, Influenza A Virus, H5N1 Subtype, Influenza Vaccines, Influenza, Human, Orthomyxoviridae Infections
- Abstract
Influenza A viruses pose a significant threat globally each year, underscoring the need for a vaccine- or antiviral-based broad-protection strategy. Here, we describe a chimeric monoclonal antibody, C12H5, that offers neutralization against seasonal and pandemic H1N1 viruses, and cross-protection against some H5N1 viruses. Notably, C12H5 mAb offers broad neutralizing activity against H1N1 and H5N1 viruses by controlling virus entry and egress, and offers protection against H1N1 and H5N1 viral challenge in vivo. Through structural analyses, we show that C12H5 engages hemagglutinin (HA), the major surface glycoprotein on influenza, at a distinct epitope overlapping the receptor binding site and covering the 140-loop. We identified eight highly conserved (~90%) residues that are essential for broad H1N1 recognition, with evidence of tolerance for Asp or Glu at position 190; this site is a molecular determinant for human or avian host-specific recognition and this tolerance endows C12H5 with cross-neutralization potential. Our results could benefit the development of antiviral drugs and the design of broad-protection influenza vaccines., (© 2022. The Author(s).)
- Published
- 2022
- Full Text
- View/download PDF
43. Polygonal non-wetting droplets on microtextured surfaces.
- Author
-
Lou J, Shi S, Ma C, Zhou X, Huang D, Zheng Q, and Lv C
- Subjects
- Hydrophobic and Hydrophilic Interactions, Surface Properties, Wettability, Microfluidics, Water
- Abstract
Understanding the interactions between liquids and solids is important for many areas of science and technology. Microtextured surfaces have been extensively studied in microfluidics, DNA technologies, and micro-manufacturing. For these applications, the ability to precisely control the shape, size and location of the liquid via textured surfaces is of particular importance for the design of fluidic-based systems. However, this has been passively realized in the wetting state thanks to the pinning of the contact line, leaving the non-wetting counterpart challenging due to the low liquid affinity. In this work, confinement is imposed on droplets located on well-designed shapes and arrangements of microtextured surfaces. An active way to shape non-wetting water and liquid metal droplets into various polygons ranging from triangles, squares, rectangles, to hexagons is developed. The results suggest that energy barriers in different directions account for the movement of the contact lines and the formation of polygonal shapes. By characterizing the curvature of the liquid-vapour meniscus, the morphology of the droplet is correlated to its volume, thickness, and contact angle. The developed liquid-based patterning strategy under active regulation with low adhesion looks promising for low-cost micromanufacturing technology, DNA microarrays, and digital lab-on-a-chip., (© 2022. The Author(s).)
- Published
- 2022
- Full Text
- View/download PDF
44. Defect-mediated ripening of core-shell nanostructures.
- Author
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Zhang Q, Peng X, Nie Y, Zheng Q, Shangguan J, Zhu C, Bustillo KC, Ercius P, Wang L, Limmer DT, and Zheng H
- Subjects
- Cadmium, Crystallization, Microscopy, Electron, Transmission, Nanoparticles chemistry, Nanostructures chemistry
- Abstract
Understanding nanostructure ripening mechanisms is desirable for gaining insight on the growth and potential applications of nanoscale materials. However, the atomic pathways of nanostructure ripening in solution have rarely been observed directly. Here, we report defect-mediated ripening of Cd-CdCl
2 core-shell nanoparticles (CSN) revealed by in-situ atomic resolution imaging with liquid cell transmission electron microscopy. We find that ripening is initiated by dissolution of the nanoparticle with an incomplete CdCl2 shell, and that the areas of the Cd core that are exposed to the solution are etched first. The growth of the other nanoparticles is achieved by generating crack defects in the shell, followed by ion diffusion through the cracks. Subsequent healing of crack defects leads to a highly crystalline CSN. The formation and annihilation of crack defects in the CdCl2 shell, accompanied by disordering and crystallization of the shell structure, mediate the ripening of Cd-CdCl2 CSN in the solution., (© 2022. The Author(s).)- Published
- 2022
- Full Text
- View/download PDF
45. Coexistence of electron whispering-gallery modes and atomic collapse states in graphene/WSe 2 heterostructure quantum dots.
- Author
-
Zheng Q, Zhuang YC, Sun QF, and He L
- Abstract
The relativistic massless charge carriers with a Fermi velocity of about c/300 in graphene enable us to realize two distinct types of resonances (here, c is the speed of light in vacuum). One is the electron whispering-gallery mode in graphene quantum dots arising from the Klein tunneling of the massless Dirac fermions. The other is the atomic collapse state, which has never been observed in experiment with real atoms due to the difficulty of producing heavy nuclei with charge Z > 170; however, they can be realized near a Coulomb impurity in graphene with a charge Z ≥ 1 because of the "small" velocity of the Dirac excitations. Here we demonstrate that both the electron whispering-gallery modes and atomic collapse states coexist in graphene/WSe
2 heterostructure quantum dots due to the Coulomb-like potential near their edges. By applying a perpendicular magnetic field, we explore the evolution from the atomic collapse states to unusual Landau levels in the collapse regime., (© 2022. The Author(s).)- Published
- 2022
- Full Text
- View/download PDF
46. The Chengjiang Biota inhabited a deltaic environment.
- Author
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Saleh F, Qi C, Buatois LA, Mángano MG, Paz M, Vaucher R, Zheng Q, Hou XG, Gabbott SE, and Ma X
- Subjects
- Animals, Biological Evolution, Floods, Minerals, Rivers, Biota, Fossils
- Abstract
The Chengjiang Biota is the earliest Phanerozoic soft-bodied fossil assemblage offering the most complete snapshot of Earth's initial diversification, the Cambrian Explosion. Although palaeobiologic aspects of this biota are well understood, the precise sedimentary environment inhabited by this biota remains debated. Herein, we examine a non-weathered core from the Yu'anshan Formation including the interval preserving the Chengjiang Biota. Our data indicate that the succession was deposited as part of a delta influenced by storm floods (i.e., produced by upstream river floods resulting from ocean storms). Most Chengjiang animals lived in an oxygen and nutrient-rich delta front environment in which unstable salinity and high sedimentation rates were the main stressors. This unexpected finding allows for sophisticated ecological comparisons with other Burgess Shale-type deposits and emphasizes that the long-held view of Burgess Shale-type faunas as snapshots of stable distal shelf and slope communities needs to be revised based on recent sedimentologic advances., (© 2022. The Author(s).)
- Published
- 2022
- Full Text
- View/download PDF
47. Structures of pseudorabies virus capsids.
- Author
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Wang G, Zha Z, Huang P, Sun H, Huang Y, He M, Chen T, Lin L, Chen Z, Kong Z, Que Y, Li T, Gu Y, Yu H, Zhang J, Zheng Q, Chen Y, Li S, and Xia N
- Subjects
- Animals, Capsid, Capsid Proteins, Swine, Viral Structures, Herpesvirus 1, Suid
- Abstract
Pseudorabies virus (PRV) is a major etiological agent of swine infectious diseases and is responsible for significant economic losses in the swine industry. Recent data points to human viral encephalitis caused by PRV infection, suggesting that PRV may be able to overcome the species barrier to infect humans. To date, there is no available therapeutic for PRV infection. Here, we report the near-atomic structures of the PRV A-capsid and C-capsid, and illustrate the interaction that occurs between these subunits. We show that the C-capsid portal complex is decorated with capsid-associated tegument complexes. The PRV capsid structure is highly reminiscent of other α-herpesviruses, with some additional structural features of β- and γ-herpesviruses. These results illustrate the structure of the PRV capsid and elucidate the underlying assembly mechanism at the molecular level. This knowledge may be useful for the development of oncolytic agents or specific therapeutics against this arm of the herpesvirus family., (© 2022. The Author(s).)
- Published
- 2022
- Full Text
- View/download PDF
48. Two distinct superconducting states controlled by orientations of local wrinkles in LiFeAs.
- Author
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Cao L, Liu W, Li G, Dai G, Zheng Q, Wang Y, Jiang K, Zhu S, Huang L, Kong L, Yang F, Wang X, Zhou W, Lin X, Hu J, Jin C, Ding H, and Gao HJ
- Abstract
For iron-based superconductors, the phase diagrams under pressure or strain exhibit emergent phenomena between unconventional superconductivity and other electronic orders, varying in different systems. As a stoichiometric superconductor, LiFeAs has no structure phase transitions or entangled electronic states, which manifests an ideal platform to explore the pressure or strain effect on unconventional superconductivity. Here, we observe two types of superconducting states controlled by orientations of local wrinkles on the surface of LiFeAs. Using scanning tunneling microscopy/spectroscopy, we find type-I wrinkles enlarge the superconducting gaps and enhance the transition temperature, whereas type-II wrinkles significantly suppress the superconducting gaps. The vortices on wrinkles show a C
2 symmetry, indicating the strain effects on the wrinkles. By statistics, we find that the two types of wrinkles are categorized by their orientations. Our results demonstrate that the local strain effect with different directions can tune the superconducting order parameter of LiFeAs very differently, suggesting that the band shifting induced by directional pressure may play an important role in iron-based superconductivity., (© 2021. The Author(s).)- Published
- 2021
- Full Text
- View/download PDF
49. Bidirectional and reversible tuning of the interlayer spacing of two-dimensional materials.
- Author
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Ding Y, Zeng M, Zheng Q, Zhang J, Xu D, Chen W, Wang C, Chen S, Xie Y, Ding Y, Zheng S, Zhao J, Gao P, and Fu L
- Abstract
Interlayer spacing is expected to influence the properties of multilayer two-dimensional (2D) materials. However, the ability to non-destructively regulate the interlayer spacing bidirectionally and reversibly is challenging. Here we report the preparation of 2D materials with tunable interlayer spacing by introducing active sites (Ce ions) in 2D materials to capture and immobilize Pt single atoms. The strong chemical interaction between active sites and Pt atoms contributes to the intercalation behavior of Pt atoms in the interlayer of 2D materials and further promotes the formation of chemical bonding between Pt atom and host materials. Taking cerium-embedded molybdenum disulfide (MoS
2 ) as an example, intercalation of Pt atoms enables interlayer distance tuning via an electrochemical protocol, leading to interlayer spacing reversible and linear compression and expansion from 6.546 ± 0.039 Å to 5.792 ± 0.038 Å (~11 %). The electronic property evolution with the interlayer spacing variation is demonstrated by the photoluminescence (PL) spectra, delivering that the well-defined barrier between the multilayer and monolayer layered materials can be artificially designed., (© 2021. The Author(s).)- Published
- 2021
- Full Text
- View/download PDF
50. Cross-neutralizing antibodies bind a SARS-CoV-2 cryptic site and resist circulating variants.
- Author
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Li T, Xue W, Zheng Q, Song S, Yang C, Xiong H, Zhang S, Hong M, Zhang Y, Yu H, Zhang Y, Sun H, Huang Y, Deng T, Chi X, Li J, Wang S, Zhou L, Chen T, Wang Y, Cheng T, Zhang T, Yuan Q, Zhao Q, Zhang J, McLellan JS, Zhou ZH, Zhang Z, Li S, Gu Y, and Xia N
- Subjects
- Animals, Antibodies, Monoclonal administration & dosage, Antibodies, Monoclonal immunology, Antibodies, Monoclonal isolation & purification, Antibodies, Monoclonal metabolism, Antibodies, Viral administration & dosage, Antibodies, Viral isolation & purification, Antibodies, Viral metabolism, Binding Sites genetics, Binding Sites immunology, Broadly Neutralizing Antibodies administration & dosage, Broadly Neutralizing Antibodies isolation & purification, Broadly Neutralizing Antibodies metabolism, CHO Cells, COVID-19 epidemiology, COVID-19 immunology, COVID-19 virology, Chlorocebus aethiops, Cricetulus, Epitopes immunology, HEK293 Cells, Humans, Mice, Middle East Respiratory Syndrome Coronavirus genetics, Middle East Respiratory Syndrome Coronavirus immunology, Neutralization Tests, Pandemics prevention & control, Protein Multimerization, Receptors, Virus metabolism, SARS-CoV-2 genetics, Sf9 Cells, Spike Glycoprotein, Coronavirus genetics, Spike Glycoprotein, Coronavirus immunology, Spike Glycoprotein, Coronavirus metabolism, Vero Cells, Antibodies, Viral immunology, Broadly Neutralizing Antibodies immunology, COVID-19 therapy, Immunization, Passive methods, SARS-CoV-2 immunology
- Abstract
The emergence of numerous variants of SARS-CoV-2, the causative agent of COVID-19, has presented new challenges to the global efforts to control the COVID-19 pandemic. Here, we obtain two cross-neutralizing antibodies (7D6 and 6D6) that target Sarbecoviruses' receptor-binding domain (RBD) with sub-picomolar affinities and potently neutralize authentic SARS-CoV-2. Crystal structures show that both antibodies bind a cryptic site different from that recognized by existing antibodies and highly conserved across Sarbecovirus isolates. Binding of these two antibodies to the RBD clashes with the adjacent N-terminal domain and disrupts the viral spike. Both antibodies confer good resistance to mutations in the currently circulating SARS-CoV-2 variants. Thus, our results have direct relevance to public health as options for passive antibody therapeutics and even active prophylactics. They can also inform the design of pan-sarbecovirus vaccines., (© 2021. The Author(s).)
- Published
- 2021
- Full Text
- View/download PDF
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