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Electrochemical CO 2 reduction reaction (CO 2 RR) offers a promising approach to close the carbon cycle and reduce reliance on fossil fuels. However, traditional decoupled CO 2 RR processes involve energy-intensive CO 2 capture, conversion, and product separation, which increases operational costs. Here, we report the development of a bismuth-poly(ionic liquid) (Bi-PIL) hybrid catalyst that exhibits exceptional electrocatalytic performance for CO 2 conversion to formate. The Bi-PIL catalyst achieves over 90% Faradaic efficiency for formate over a wide potential range, even at low 15% v/v CO 2 concentrations typical of industrial flue gas. The biphenyl in PIL backbone affords hydrophobicity while maintaining high ionic conductivity, effectively mitigating the flooding issues. The PIL layer plays a crucial role as a CO 2 concentrator and co-catalyst that accelerates the CO 2 RR kinetics. Furthermore, we demonstrate the potential of Bi-PIL catalysts in a solid-state electrolyte (SSE) electrolyzer for the continuous and direct production of pure formic acid solutions from flue gas. Techno-economic analysis suggests that this integrated process can produce formic acid at a significantly reduced cost compared to the traditional decoupled approaches. This work presents a promising strategy to overcome the challenges associated with low-concentration CO 2 utilization and streamline the production of valuable liquid fuels and chemicals from CO 2 ., (© 2024 Wiley‐VCH GmbH.)

Creating fluorophores that meet the Broadcast Service Television 2020 (BT.2020) standard is a significant achievement. In this paper, we present an innovative strategy that could revolutionize the development of high-performance narrowband fluorophores for ultra-high-definition displays. Our approach combines classic multi-resonance BN-doped fragments with naphthalene, creating two novel narrowband bright green quasi-fluorescent emitters, NT-2B and NT-3B. When tested in dilute toluene, these molecules exhibit emission peaks at 510 and 511 nm with extremely narrow FWHM values of 15 and 14 nm, respectively. Both molecules also demonstrate conventional fluorescence properties with high photoluminescence quantum yields (PLQYs) of up to 85%. Notably, OLEDs containing NT-2B achieve a peak EQE of approximately 30% and at a doping concentration of 5 wt.%, OLEDs based on NT-2B achieve a CIEy value of roughly 0.75, closely matching the BT.2020 standard., (© 2024 Wiley‐VCH GmbH.)

Herein, we propose a regional functionalization molecular design strategy that enables independent control of distinct pivotal parameters through different molecule segments. Three novel multiple resonances thermally activated delayed fluorescence (MR-TADF) emitters A-BN, DA-BN, and A-DBN, have been successfully synthesized by integrating highly rigid and three-dimensional adamantane-containing spirofluorene units into the MR framework. These molecules form two distinctive functional parts: part 1 comprises a boron-nitrogen (BN)-MR framework with adjacent benzene and fluorene units forming a central luminescent core characterized by an exceptionally rigid planar geometry, allowing for narrow FWHM values; part 2 includes peripheral mesitylene, benzene, and adamantyl groups, creating a unique three-dimensional "umbrella-like" conformation to mitigate intermolecular interactions and suppress exciton annihilation. The resulting A-BN, DA-BN, and A-DBN exhibit remarkably narrow FWHM values ranging from 18 to 14 nm and near-unity photoluminescence quantum yields. Particularly, OLEDs based on DA-BN and A-DBN demonstrate outstanding efficiencies of 35.0 % and 34.3 %, with FWHM values as low as 22 nm and 25 nm, respectively, effectively accomplishing the integration of high color purity and high device performance., (© 2024 Wiley-VCH GmbH.)

Nitrogen (N 2 ) conversion to ammonia (NH 3 ) in a mild condition is a big chemical challenge. The whole-cell diazotrophs based biological NH 3 synthesis is one of the most promising strategies. Herein, the first attempt of photoelectrochemical-microbial (PEC-MB) biohybrid is contributed for artificial N 2 fixation, where Azotobacter vinelandii (A. vinelandii) is interfaced directly with polydopamine encapsulated nickel oxide (NiO) nanosheets (NiO@PDA). By virtue of excellent bio-adhesive activity, high conductivity, and good biocompatibility of PDA layer, abundant A. vinelandii are effectively adsorbed on NiO@PDA to form NiO@PDA/A. vinelandii biohybrid, and the rationally designed biohybrid achieved a record-high NH 3 production yield of 1.85   µmol h -1 /10 8 cells (4.14 µmol h -1 cm -2 ). In addition, this biohybrid can operate both under illumination with a PEC model or in dark with an electrocatalytic (EC) model to implement long-term and successional NH 3 synthesis. The enhancement mechanism of NH 3 synthesis in NiO@PDA/A. vinelandii biohybrid can be ascribed to the increase of nicotinamide adenine dinucleotide-hydrogen (NADH) and adenosine 5-triphosphate (ATP) concentrations and over expression of nitrogen-fixing genes of nifH, nifD and nifK in nitrogenase. This innovative PEC-MB biohybrid strategy sheds light on the fundamental mechanism and establishes proof of concept of biotic-abiotic photosynthetic systems for sustainable chemical production., (© 2024 Wiley‐VCH GmbH.)

Arboviruses, transmitted by medical arthropods, pose a serious health threat worldwide. During viral infection, Post Translational Modifications (PTMs) are present on both host and viral proteins, regulating multiple processes of the viral lifecycle. In this study, a mammalian E3 ubiquitin ligase WWP2 (WW domain containing E3 ubiquitin ligase 2) is identified, which interacts with the NS1 protein of Zika virus (ZIKV) and mediates K63 and K48 ubiquitination of Lys 265 and Lys 284, respectively. WWP2-mediated NS1 ubiquitination leads to NS1 degradation via the ubiquitin-proteasome pathway, thereby inhibiting ZIKV infection in mammalian hosts. Simultaneously, it is found Su(dx), a protein highly homologous to host WWP2 in mosquitoes, is capable of ubiquitinating NS1 in mosquito cells. Unexpectedly, ubiquitination of NS1 in mosquitoes does not lead to NS1 degradation; instead, it promotes viral infection in mosquitoes. Correspondingly, the NS1 K265R mutant virus is less infectious to mosquitoes than the wild-type (WT) virus. The above results suggest that the ubiquitination of the NS1 protein confers different adaptations of ZIKV to hosts and vectors, and more importantly, this explains why NS1 K265-type strains have become predominantly endemic in nature. This study highlights the potential application in antiviral drug and vaccine development by targeting viral proteins' PTMs., (© 2024 The Author(s). Advanced Science published by Wiley‐VCH GmbH.)

The complexity of the multielement interaction in high-entropy alloys (HEAs) may provide more active sites to adapt different catalytic reaction steps in oxygen evolution reaction (OER). Investigating the correlation between structure and performance of HEAs electrocatalysts is both essential and challenging. In this work, FeCoNiCrMo x HEA nanoparticles are successfully fabricated utilizing a unique nanofabrication method called inert gas condensation. With the increase of high-valence metal component Mo, the atomic structure amorphization and electronic structure reconstruction are unveiled. According to the X-ray photoelectron spectroscopy valence spectra, the d-band center of FeCoNiCrMo x is ascending, and thus enhancing the adsorption energy. Synchrotron pair distribution function analysis reflects the degree of structural disorder and reveals a robust correlation with the intrinsic OER activities of the electrocatalysts. FeCoNiCrMo 1.0 high-entropy metallic glass nanoparticles exhibit an outstanding OER performance with an ultralow overpotential of 294.5 mV at a high current density of 100 mA cm -2 . This work brings fundamental and practical insights into the modulation mechanism of metal components of HEAs catalysts for developing OER., (© 2024 Wiley‐VCH GmbH.)

Visualization of training effectiveness is critical to patients' confidence and eventual rehabilitation. Here, an innovative magnetoinductive pressure sensor is proposed for monitoring hand rehabilitation in stroke hemiplegic patients. It couples the giant magneto and stress-impedance effects of a square spiral amorphous wire with the giant magnetoelastic effect of a polymer magnet (NdFeB@PDMS). The addition of the magnetoelastic layer results in a sensitivity improvement of 178%, a wide sensing range (up to 1 MPa), fast response/recovery times (40 ms), and excellent mechanical robustness (over 15 000 cycles). Further integration with an LC oscillation circuit enables frequency adjustment into the MHz range resulting in a sensitivity of 6.6% kPa -1 and outstanding linearity (R 2 =  0.99717) over a stress range of up to 100 kPa. When attached to a commercial split-fingerboard, the sensor is capable of dynamically monitoring the force in each finger, providing a reading of the rehabilitation process. Unlike conventional inductive sensors, the sensor is based on an inductive force-responsive material (amorphous wire), which significantly boosts the sensitivity. The approach also demonstrates the potential of magnetoelasticity in static pressure sensing, which is highly sensitive to dynamic pressure only through electromagnetic induction. This makes it more suitable for long-term and continuous human health monitoring., (© 2024 Wiley‐VCH GmbH.)

Hypoxic tumor microenvironment (TME) hampers the application of oxygen (O 2 )-dependent photodynamic therapy (PDT) in solid tumors. To address this problem, a biomimetic nanotheranostics (named MMCC@EM) is developed for optical molecular imaging-escorted self-oxygenation PDT. MMCC@EM is synthesized by encapsulating chlorin e6 (Ce6) and catalase (CAT) in metal-organic framework (MOF) nanoparticles with erythrocyte membrane (EM) camouflage. Based on the biomimetic properties of EM, MMCC@EM efficiently accumulates in tumor tissues. The enriched MMCC@EM achieves TME-activatable drug release, thereby releasing CAT and Ce6, and this process can be monitored through fluorescence (FL) imaging. In addition, endogenous hydrogen peroxide (H 2 O 2 ) will be decomposed by CAT to produce O 2 , which can be reflected by the measurement of intratumoral oxygen concentration using photoacoustic (PA) imaging. Such self-oxygenation nanotheranostics effectively mitigate tumor hypoxia and improve the generation of singlet oxygen ( 1 O 2 ). The 1 O 2 disrupts mitochondrial function and triggers caspase-3-mediated cellular apoptosis. Furthermore, MMCC@EM triggers immunogenic cell death (ICD) effect, leading to an increased infiltration of cytotoxic T lymphocytes (CTLs) into tumor tissues. As a result, MMCC@EM exhibits good therapeutic effects in 4T1-tumor bearing mice under the navigation of FL/PA duplex imaging., (© 2024 Wiley‐VCH GmbH.)

An optimal cancer chemotherapy regimen should effectively address the drug resistance of tumors while eliciting antitumor-immune responses. Research has shown that non-apoptotic cell death, such as pyroptosis and ferroptosis, can enhance the immune response. Despite this, there has been limited investigation and reporting on the mechanisms of oncosis and its correlation with immune response. Herein, we designed and synthesized a Ru(II) complex that targeted the nucleus and mitochondria to induce cell oncosis. Briefly, the Ru(II) complex disrupts the nucleus and mitochondria DNA, which active polyADP-ribose polymerase 1, accompanied by ATP consumption and porimin activation. Concurrently, mitochondrial damage and endoplasmic reticulum stress result in the release of Ca 2+ ions and increased expression of Calpain 1. Subsequently, specific pore proteins porimin and Calpain 1 promote cristae destruction or vacuolation, ultimately leading to cell membrane rupture. The analysis of RNA sequencing demonstrates that the Ru(II) complex can initiate the oncosis-associated pathway and activate both innate and adaptive immunity. In vivo experiments have confirmed that oncosis promotes dendritic cell maturation and awakens adaptive cytotoxic T lymphocytes but also activates the innate immune by inducing the polarization of macrophages towards an M1 phenotype., (© 2024 Wiley-VCH GmbH.)

Multi-component copolymerized donors (MCDs) have gained significant interest and have been rapidly developed in flexible organic solar cells (f-OSCs) in recent years. However, ensuring the power conversion efficiency (PCE) of f-OSCs while retaining ideal mechanical properties remains an enormous challenge. The fracture strain (FS) value of typical high-efficiency blend films is generally less than 8 %, which is far from the application standards of wearable photovoltaic devices. Therefore, we developed a series of novel MCDs after meticulous molecular design. Among them, the consistent MCD backbone and end-capped functional group formed a highly conjugated molecular plane, and the solubilization and mechanical properties were effectively optimized by modifying the proportion of solubilized alkyl chains. Consequently, due to the formation of entangled structures with a frozen blend film morphology considerably improved the high ductility of the active layer, P1 0.8 /P2 0.2 -TCl exhibited efficient PCE in rigid (18.53 %) and flexible (17.03 %) OSCs, along with excellent FS values (16.59 %) in pristine films, meanwhile, the outstanding FS values of 25.18 % and 12.3 % were achieved by P1 0.6 /P2 0.4 -TCl -based pristine and blend films, respectively, which were one of the highest records achieved by end-capped MCD-based binary OSCs, demonstrating promising application to synchronize the realization of high-efficiency and mechanically ductile flexible OSCs., (© 2024 Wiley-VCH GmbH.)

One of the central focuses in self-assembly is precisely controlling the self-assembly pathway so that the target molecules can be produced exclusively. Trans-1,2-cyclohexanediamine contains two amino units that form a 60° angle when projected on a plane. This angle naturally favors the formation of triangular products in most cases when trans-1,2-cyclohexanediamine is used as a bisamino building block in the synthesis of macrocycles and tubes. Here, we synthesized a slightly bent tetraformyl precursor bearing a central dibenzothiophene moiety, whose 3,7-positions are functionalized with two m-phthalaldehyde units. We observed that combining this tetraformyl building block with trans-1,2-cyclohexanediamine yielded a quadrangular tube when the concentrations of the precursors were relatively high. Both experimental measurements and theoretical calculations indicate that the formation of this unlikely occurring quadrangular product was driven by the intramolecular C-H···π interactions between the dibenzothiophene building blocks within the tube framework. This driving force, however, was disturbed in the triangular tube, a smaller counterpart whose formation was considered previously much more thermodynamically favored. These results improved our fundamental understanding on how to create those products whose syntheses are considered difficult or impossible, by modulating the intramolecular driving forces., (© 2024 Wiley‐VCH GmbH.)

Mortality rates due to lung cancer are high worldwide. Although PD-1 and PD-L1 immune checkpoint inhibitors boost the survival of patients with non-small-cell lung cancer (NSCLC), resistance often arises. The Warburg Effect, which causes lactate build-up and potential lysine-lactylation (Kla), links immune dysfunction to tumor metabolism. The role of non-histone Kla in tumor immune microenvironment and immunotherapy remains to be clarified. Here, global lactylome profiling and metabolomic analyses of samples from patients with NSCLC is conducted. By combining multi-omics analysis with in vitro and in vivo validation, that intracellular lactate promotes extracellular lipolysis through lactyl-APOC2 is revealed. Mechanistically, lactate enhances APOC2 lactylation at K70, stabilizing it and resulting in FFA release, regulatory T cell accumulation, immunotherapy resistance, and metastasis. Moreover, the anti-APOC2 K70-lac antibody that sensitized anti-PD-1 therapy in vivo is developed. This findings highlight the potential of anti lactyl-APOC2-K70 approach as a new combination therapy for sensitizing immunotherapeutic responses., (© 2024 The Author(s). Advanced Science published by Wiley‐VCH GmbH.)

Hepatocellular carcinoma (HCC) hematogenous dissemination is a leading cause of HCC-related deaths. The inflammatory facilitates this process by promoting the adhesion and invasion of tumor cells in the circulatory system. But the contribution of hemodynamics to this process remains poorly understood due to the lack of a suitable vascular flow model for investigation. This study develops a vascular flow model to examine the impact of hemodynamics on endothelial inflammation-mediated HCC metastasis. This work finds the increasing shear stress will reduce the recruitment of HCC cells by disturbing adhesion forces between endothelium and HCC cells. However, this reduction will be restored by the inflammation. When applying high FSS (4-6 dyn cm -2 ) to the inflammatory endothelium, there will be a 4.8-fold increase in HCC cell adhesions compared to normal condition. Nevertheless, the increase fold of cell adhesions is inapparent, around 1.5-fold, with low and medium FSS. This effect can be attributed to the FSS-induced upregulation of ICAM-1 and VCAM-1 of the inflammatory endothelium, which serve to strengthen cell binding forces. These findings indicate that hemodynamics plays a key role in HCC metastasis during endothelial inflammation by regulating the expression of adhesion-related factors., (© 2024 Wiley‐VCH GmbH.)

Chemodynamic therapy (CDT) has emerged as a promising approach for treating infected diabetic wounds, while reliable imaging technology for simultaneous monitoring of ROS and therapeutic processes is still a formidable challenge. Herein, smart covalent organic framework (COF) nanoreactors (COF NRs) are constructed by hyaluronic acid (HA) packaged glucose oxidase (GOx) covalently linked Fe-COF for diabetic wound healing. Upon the breakdown of the HA protective layer, GOx consumes glucose to produce gluconic acid and hydrogen peroxide (H 2 O 2 ), resulting in decreased local pH and H 2 O 2 supplementation. Density functional theory (DFT) calculations show that Fe-COF has high catalytic activity towards H 2 O 2 , leading to in situ generation of hydroxyl radicals (·OH) for sterilization, and the localized downregulation of glucose effectively improved the microenvironment of diabetic wounds. Meanwhile, based on the near-infrared photothermal imaging of oxidized 3,3',5,5'-tetramethylbenzidine (oxTMB), the authors showed that TMB can be applied for the point-of-care testing of ·OH and glucose, and assessing the sterilization progress in vivo. More significantly, the facile photothermal signaling strategy can be extended to monitor various ROS-mediated therapeutic systems, enabling accurate prediction of treatment outcomes., (© 2024 Wiley‐VCH GmbH.)

The unique catalytic activities of high-entropy alloys (HEAs) emerge from the complex interaction among different elements in a single-phase solid solution. As a "green" nanofabrication technique, inert gas condensation (IGC) combined with laser source opens up a highly efficient avenue to develop HEA nanoparticles (NPs) for catalysis and energy storage. In this work, the novel N-doped non-noble HEA NPs are designed and successfully prepared by IGC. The N-doping effects of HEA NPs on oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) are systematically investigated. The results show that N-doping is conducive to improving the OER, but unfavorable for HER activity. The FeCoNiCrN NPs achieve an overpotential of 269.7 mV for OER at a current density of 10 mA cm -2 in 1.0 M KOH solution, which is among the best reported values for non-noble HEA catalysts. The effects of the differences in electronegativity, ionization energy and electron affinity energy among mixed elements in N-doped HEAs are discussed as inducing electron transfer efficiency. Combined with X-ray photoelectron spectroscopy and the extended X-ray absorption fine structure analysis, an element-design strategy in N-doped HEAs electrocatalysts is proposed to improve the intrinsic activity and ameliorate water splitting performance., (© 2023 Wiley‐VCH GmbH.)

DNA strand displacement reactions are vital for constructing intricate nucleic acid circuits, owing to their programmability and predictability. However, the scarcity of effective methods for eliminating circuit leakages has hampered the construction of circuits with increased complexity. Herein, a versatile strategy is developed that relies on a spatially controlled proximity split tweezer (PST) switch to transduce the biomolecular signals into the independent oligonucleotides. Leveraging the double-stranded rigidity of the tweezer works synergistically with the hindering effect of the hairpin lock, effectively minimizing circuit leakage compared with sequence-level methods. In addition, the freely designed output strand is independent of the target binding sequence, allowing the PST switch conformation to be modulated by nucleic acids, small molecules, and proteins, exhibiting remarkable adaptability to a wide range of targets. Using this platform, established logical operations between different types of targets for multifunctional transduction are successfully established. Most importantly, the platform can be directly coupled with DNA catalytic circuits to further enhance transduction performance. The uniqueness of this platform lies in its design straightforwardness, flexibility, scalable intricacy, and system compatibility. These attributes pave a broad path toward nucleic acid-based development of sophisticated transduction networks, making them widely applied in basic science research and biomedical applications., (© 2023 Wiley‐VCH GmbH.)

How Nature synthesizes enantiomerically pure substances from achiral or racemic resources remains a mystery. In this study, we aimed to emulate this natural phenomenon by constructing chiral tetrahedral cages through self-assembly, achieved by condensing two achiral compounds-a trisamine and a trisaldehyde. The occurrence of intercomponent CH⋅⋅⋅π interactions among the phenyl building blocks within the cage frameworks results in twisted conformations, imparting planar chirality to the tetrahedrons. In instances where the trisaldehyde precursor features electron-withdrawing ester side chains, we observed that the intermolecular CH⋅⋅⋅π forces are strong enough to prevent racemization. To attain enantioselective self-assembly, a chiral amine was introduced during the imine formation process. The addition of three equivalents of chiral amino mediator to one equivalent of the achiral trisaldehyde precursor formed a trisimino intermediate. This chiral compound was subsequently combined with the achiral trisamino precursor, leading to an imine exchange reaction that releasing the chiral amino mediator and formation of the tetrahedral cage with an enantiomeric excess (ee) of up to 75 %, exclusively composed of achiral building blocks. This experimental observation aligns with theoretical calculations based on the free energies of related cage structures. Moreover, since the chiral amine was not consumed during the imine exchange cycle, it enabled the enantioselective self-assembly of the tetrahedral cage for multiple cycles when new batches of the achiral trisaldehyde and trisamino precursors were successively added., (© 2024 Wiley‐VCH GmbH.)

Cattle and the draught force provided by its skeletal muscle have been integral to agro-ecosystems of agricultural civilization for millennia. However, relatively little is known about the cattle muscle functional genomics (including protein coding genes, non-coding RNA, etc.). Circular RNAs (circRNAs), as a new class of non-coding RNAs, can be effectively translated into detectable peptides, which enlightened us on the importance of circRNAs in cattle muscle physiology function. Here, RNA-seq, Ribosome profiling (Ribo-seq), and peptidome data are integrated from cattle skeletal muscle, and detected five encoded peptides from circRNAs. It is further identified and functionally characterize a 907-amino acids muscle-specific peptide that is named circNEB-peptide because derived by the splicing of Nebulin (NEB) gene. This peptide localizes to the nucleus and cytoplasm and directly interacts with SKP1 and TPM1, key factors regulating physiological activities of myoblasts, via ubiquitination and myoblast fusion, respectively. The circNEB-peptide is found to promote myoblasts proliferation and differentiation in vitro, and induce muscle regeneration in vivo. These findings suggest circNEB-peptide is an important regulator of skeletal muscle regeneration and underscore the possibility that more encoding polypeptides derived by RNAs currently annotated as non-coding exist., (© 2023 The Authors. Advanced Science published by Wiley-VCH GmbH.)

Despite widespread use of the deuterium isotope effect, selective deuterium labeling of chemical molecules remains a major challenge. Herein, a facile and general electrochemically driven, organic mediator enabled deuteration of styrenes with deuterium oxide (D 2 O) as the economical deuterium source was reported. Importantly, this transformation could be suitable for various electron rich styrenes mediated by triphenylphosphine (TPP). The reaction proceeded under mild conditions without transition-metal catalysts, affording the desired products in good yields with excellent D-incorporation (D-inc, up to >99 %). Mechanistic investigations by means of isotope labeling experiments and cyclic voltammetry tests provided sufficient support for this transformation. Notably, this method proved to be a powerful tool for late-stage deuteration of biorelevant compounds., (© 2023 Wiley-VCH GmbH.)

Herein, an electrochemically driven NiH-catalyzed reductive coupling of alkyl halides and alkyl alkenes for the construction of Csp 3 -Csp 3 bonds is firstly reported. Notably, alkyl halides serve dual function as coupling substrates and as hydrogen sources to generate NiH species under electrochemical conditions. The tunable nature of this reaction is realized by introducing an intramolecular coordinating group to the substrate, where the product can be easily adjusted to give the desired branched products. The method proceeds under mild conditions, exhibits a broad substrate scope, and affords moderate to excellent yields with over 70 examples, including late-stage modification of natural products and drug derivatives. Mechanistic insights offer evidence for an electrochemically driven coupling process. The sp 3 -carbon-halogen bonds can be activated through single electron transfer (SET) by the nickel catalyst in its low valence state, generated by cathodic reduction, and the generation of NiH species from alkyl halides is pivotal to this transformation., (© 2023 Wiley-VCH GmbH.)

Topologically disordered metallic glass nanoparticles (MGNPs) with highly active and tailorable surface chemistries have immense potential for functional uses. The synthesis of free-standing MGNPs is crucial and intensively pursued because their activity strongly depends on their exposed surfaces. Herein, a novel laser-evaporated inert-gas condensation method is designed and successfully developed for synthesizing free-standing MGNPs without substrates or capping agents, which is implemented via pulse laser-induced atomic vapor deposition under an inert helium atmosphere. In this way, the metallic atoms vaporized from the targets collide with helium atoms and then condense into short-range-order (SRO) clusters, which mutually assemble to form the MGNPs. Using this method, free-standing Pd 40 Ni 40 P 20 MGNPs with a spherical morphology are synthesized, which demonstrates satisfactory electrocatalytic activity and durability in oxygen reduction reactions. Moreover, local structure investigations using synchrotron pair distribution function techniques reveal the transformation of SRO cluster connection motifs of the MGNPs from face-sharing to edge-sharing modes during cyclic voltammetry cycles, which enhances the electrochemical stability by blocking crystallization. This approach provides a general strategy for preparing free-standing MGNPs with high surface activities, which may have widespread functional applications., (© 2023 Wiley-VCH GmbH.)

Five osmium(II) polypyridyl complexes of the general formula [Os(4,7-diphenyl-1,10-phenanthroline) 2 L] 2+ were synthesized as photosensitizers for photodynamic therapy by varying the nature of the ligand L. Thanks to the pronounced π-extended structure of the ligands and the heavy atom effect provided by the osmium center, these complexes exhibit a high absorption in the near-infrared (NIR) region (up to 740 nm), unlike related ruthenium complexes. This led to a promising phototoxicity in vitro against cancer cells cultured as 2D cell layers but also in multicellular tumor spheroids upon irradiation at 740 nm. The complex [Os(4,7-diphenyl-1,10-phenanthroline) 2 (2,2'-bipyridine)] 2+ was found to be the most efficient against various cancer cell lines, with high phototoxicity indexes. Experiments on CT26 tumor-bearing BALB/c mice also indicate that the Os II complexes could significantly reduce tumor growth following 740 nm laser irradiation. The high phototoxicity in the biological window of this structurally simple complex makes it a promising photosensitizer for cancer treatment., (© 2023 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.)

Phase-junction nanocomposites, made of nanograins with the same composition but different phases, offer a platform to optimize the physiochemical performance of materials. Herein, we demonstrate a straightforward strategy to synthesize Cu 2-x S phase-junction nanocomposites by retaining surface 1-dodecanethiol (DDT) ligands, in contrast to the traditional method that strips the ligands. As a result, phase junctions between a conventional monoclinic (m) phase and an unconventional metastable tetragonal (t) phase are obtained. The significantly improved power factor is obtained due to the doping of the t-phase. The phase-junction interfaces reduce thermal conductivity. Finally, surface regulation of phase junctions pushes the peak zT to 2.1 at 932 K, being the highest reported for environment-friendly metal sulfides. This work provides a paradigm to optimize thermoelectric performance by controlling phase junctions through surface-ligand tuning., (© 2022 Wiley-VCH GmbH.)

Carbon dioxide (CO 2 ) is an abundant, inexpensive, renewable C1 resource and the main component of greenhouse gas, thereby the research for its sustainable and efficient conversion has received notable attention in recent years. Electrochemical organic synthesis, as a green and efficient synthetic method, is convinced to be an ideal approach for CO 2 utilization. In this review, recent advances in electrocarboxylation with CO 2 were summarized through different reaction types, which would disclose the great potential of electrocarboxylation in green organic synthesis., (© 2022 Wiley-VCH GmbH.)

Metallic glasses (MGs), with high density of low coordination sites and high Gibbs free energy state, are novel promising and competitive candidates in the family of electrochemical catalysts. However, it remains a grand challenge to modify the properties of MGs by control of the disordered atomic structure. Recently, nanostructured metallic glasses (NGs), consisting of amorphous nanometer-sized grains connected by amorphous interfaces, have been reported to exhibit tunable properties compared to the MGs with identical chemical composition. Here, it is demonstrated that electrodeposited Ni-P NG is characterized by an extremely high energy state due to its heterogeneous structure, which significantly promotes the catalytic performance. Moreover, the Ni-P NG with a heterogeneous structure is a perfect precursor for the fabrication of unique honey-like nanoporous structure, which displays superior catalytic performance in the urea oxidation reaction (UOR). Specifically, modified Ni-P NG requires a potential of mere 1.36 V at 10 mA cm -2 , with a Tafel slope of 13 mV dec -1 , which is the best UOR performance in Ni-based alloys. The present work demonstrates that the nanostructurization of MGs provides a universal and effective pathway to upgrade the energy state of MGs for the design of high-performance catalysts in energy conversion., (© 2022 Wiley-VCH GmbH.)

Photocatalytic water splitting for hydrogen evolution is one of the most promising methods to mitigate environmental and energy-related issues. In this study, manganese cadmium sulfide (Mn x Cd 1-x S) solid solution is used to construct a p-n heterostructure with NiCo 2 O 4 through a hydrothermal method. The Mn 0.25 Cd 0.75 S/NiCo 2 O 4 composites are used for photocatalytic hydrogen evolution reaction, and the optimal hydrogen rate with 40 mg of Mn 0.25 Cd 0.75 S/NiCo 2 O 4 40 mg (MCS/NCO 40) is 61159 μmol g -1  h -1 , which is about 16.3 times than that of pure Mn 0.25 Cd 0.75 S. After combining with NiCo 2 O 4 , the light absorption scale, the separation efficiency of photogenerated carriers, and the reaction kinetics are enhanced. Moreover, the band offset of MCS/NCO composites is calculated by the core level alignment method, demonstrating the formation of a p-n heterostructure. The built-in electric field from the p-n heterostructure drives charge transfer and enhances separation efficiency, which results in improved photocatalytic performance., (© 2022 Wiley-VCH GmbH.)

The development of minimally invasive cardiac patches, either as hemostatic dressing or treating myocardial infarction, is of clinical significance but remains a major challenge. Designing such patches often requires simultaneous consideration of several material attributes, including bioabsorption, non-toxicity, matching the mechanic properties of heart tissues, and working efficiently in wet and dynamic environments. Using genetically engineered multi-domain proteins, a printed bi-layer proteinaceous hydrogel patch for heart failure treatments is reported. The intrinsic self-healing nature of hydrogel materials physically enables seamless interfacial integration of two disparate hydrogel layers and functionally endows the cardiac patches with the combinatorial advantages of each layer. Leveraging the biocompatibility, structural stability, and tunable drug release properties of the bi-layer hydrogel, promising effects of hemostasis, fibrosis reduction, and heart function recovery on mice is demonstrated with two myocardium damage models. Moreover, this proteinaceous patch is proved biodegradable in vivo without any additive inflammations. In conclusion, this work introduces a promising new type of minimally invasive patch based on genetically modified double-layer protein gel for treating heart-related injuries or diseases., (© 2022 Wiley-VCH GmbH.)

Topological semimetals provide new opportunities for exploring novel thermoelectric phenomena, owing to their exotic and nontrivial electronic structure topology around the Fermi surface. Herein, the discovery of large transverse and longitudinal magneto-thermoelectric (MTE) effects in Mg 3 Bi 2 is reported and predicted to be a type-II nodal-line semimetal in the absence of spin-orbit coupling (SOC). The maximum transverse power factor is 2182 μW m -1 K -2 at 13.5 K and 6 Tesla. The longitudinal power factor reaches up to 3043 μW m -1 K -2 , which is 20 times higher than that in a zero-strength magnetic field and is also comparable to state-of-the-art MTE materials. By compensating the Mg loss in Mg-rich conditions for tuning the carrier concentration close to intrinsic state, the sample fabricated in this study exhibits a large linear non-saturating magnetoresistance of 940% under a field of 14 Tesla. Using density functional calculations, the authors attribute the underlying mechanism to the parent linear-dispersed nodal-line electronic structure without SOC and the anisotropic Fermi surface shape with SOC, highlighting the essential role of high carrier mobility and open electron orbits in the moment space. This work offers a new avenue toward highly efficient MTE materials through defect engineering in polycrystalline topological semimetals., (© 2022 Wiley-VCH GmbH.)

Marine biofouling is one of the most significant challenges hindering practical uranium extraction from seawater. Single atoms have been widely used in catalytic applications because of their remarkable redox property, implying that the single atom is highly capable of catalyzing the generation of reactive oxygen species (ROS) and acts as an anti-biofouling substance for controlling biofouling. In this study, the Co single atom loaded polyacrylamidoxime (PAO) material, PAO-Co, is fabricated based on the binding ability of the amidoxime group to uranyl and cobalt ions. Nitrogen and oxygen atoms from the amidoxime group stabilize the Co single atom. The fabricated PAO-Co exhibits a broad range of antimicrobial activity against diverse marine microorganisms by producing ROS, with an inhibition rate up to 93.4%. The present study is the first to apply the single atom for controlling biofouling. The adsorbent achieves an ultrahigh uranium adsorption capacity of 9.7 mg g -1 in biofouling-containing natural seawater, which decreased only by 11% compared with that in biofouling-removed natural seawater. These findings indicate that applying single atoms would be a promising strategy for designing biofouling-resistant adsorbents for uranium extraction from seawater., (© 2022 The Authors. Advanced Science published by Wiley-VCH GmbH.)

An adaptive coordination structure is vital for selective uranium extraction from seawater. By strategy of molecular imprinting, uranyl is introduced into a multivariate metal-organic framework (MOF) during the synthesis process to guide the in situ construction of proper nanocage structure for targeting uranyl binding. Except for the coordination between uranium with four oxygen from the materials, the axial oxygen of uranyl also forms hydrogen bonds with hydrogen from the phenolic hydroxyl group, which enhances the binding affinity of the material to uranyl. Attributing to the high binding affinity, the adsorbent shows high uranium binding selectivity to uranyl against not only the interfering metal ions, but also the carbonate group that coordinates with uranyl to form [UO 2 (CO) 3 ] 4- in seawater. In natural seawater, the adsorbent realizes a high uranium adsorption capacity of 7.35 mg g -1 , together with an 18.38 times higher selectivity to vanadium., (© 2021 Wiley-VCH GmbH.)

The detection of environmental uranyl is attracting increasing attention. However, the available detection strategies mainly depend on the selective recognition of uranyl, which is subject to severe interference by coexisting metal ions. Herein, based on the unique uranyl-triggered photocleavage property, the protein BSA is labelled with fluorescent molecules that exhibit an aggregation-induced emission effect for uranyl detection. Uranyl-triggered photocleavage causes the separation of the fluorescent-molecule-labelled protein fragments, leading to attenuation of the emission fluorescence, which is used as a signal for uranyl detection. This detection strategy shows high selectivity for uranyl and an ultralow detection limit of 24 pM with a broad detection range covering five orders of magnitude. The detection method also shows high reliability and stability, making it a promising technique for practical applications in diverse environments., (© 2022 Wiley-VCH GmbH.)

Herein, we disclose a straightforward, robust, and simple route to access β-substituted desaturated cyclic amines via an electrochemically driven desaturative β-functionalization of cyclic amines. This transformation is based on multiple single-electron oxidation processes using catalytic amounts of ferrocene. The reaction proceeds in the absence of stoichiometric amounts of electrolyte under mild conditions, affording the desired products with high chemo- and regioselectivity. The reaction was tolerant of a broad range of substrates and also enables late-stage β-C(sp 3 )-H acylation of potentially valuable products. Preliminary mechanistic studies using cyclic voltammetry reveal the key role of ferrocene as a redox mediator in the reaction., (© 2021 Wiley-VCH GmbH.)

Chronic airway inflammation mediated by CD8 + T lymphocytes contributes to the pathogenesis of Chronic obstructive pulmonary disease (COPD). Deciphering the fingerprint of the chronic inflammation orchestrated by CD8 + T cells may allow the development of novel approaches to COPD management. Here, the expression of IL-27 and IFN-γ + CD8 + Tc1 cells were evaluated in patients with COPD and in cigarette smoke-exposed mice. The production of IL-27 by marrow-derived dendritic cells (mDCs) in response to cigarette smoke extract (CSE) was assessed. The role of IL-27 in IFN-γ + CD8 + Tc1 cells was explored. We demonstrated that elevated IL-27 was accompanied by an exaggerated IFN-γ + CD8 + Tc1 response in a smoking mouse model of emphysema. We noted that lung dendritic cells were one of the main sources of IL-27 during chronic cigarette smoke exposure. Moreover, CSE directly induced the production of IL-27 by mDCs in vitro. IL-27 negatively regulated the differentiation of IFN-γ + CD8 + Tc1 cells isolated from cigarette smoke-exposed mice in a STAT1- and STAT3-independent manner. Systemic administration of recombinant IL-27 attenuated IFN-γ + CD8 + Tc1 response in the late phase of cigarette smoke exposure. Our results uncovered that IL-27 negatively regulates IFN-γ + CD8 + Tc1 response in the late stage of chronic cigarette smoke exposure, which may provide a new strategy for the anti-inflammatory treatment of smoking-related COPD/emphysema., (© 2021 Wiley-VCH GmbH.)

Noble-metal-free composites with good photocatalytic property are of great interest. Here, CeO 2 nanorods composites loaded with amorphous Fe(OH) 3 cocatalyst were designed and prepared via a secondary water bath at 100 °C. The as-synthesized CeO 2 /amorphous Fe(OH) 3 composites exhibited superior light photocatalytic activities compared to pure CeO 2 , especially the sample with a loading time of 60 min. The photocatalytic oxygen generation rate could reach to 357.2 μmol h -1  g -1 , and the average apparent quantum yield (AQY) was 24.67 %, which was a 5.5-fold increase compared to the CeO 2 sample. The improvement of photocatalytic performance could be ascribed to three main reasons: First, loading the amorphous Fe(OH) 3 enlarged the specific surface area and passivated the surface of the pristine CeO 2 . Second, the amorphous Fe(OH) 3 ,which acted as a cocatalyst, provided many active sites, and reduced the reaction activation energy. Thirdly, the maximum interface with intimate contact between CeO 2 and amorphous Fe(OH) 3 cocatalyst accelerated the photogenerated charge separation efficiency and thus improved the photocatalytic performance of CeO 2 in photocatalytic water oxidation., (© 2021 Wiley-VCH GmbH.)

Resistance to sorafenib severely hinders its effectiveness against hepatocellular carcinoma (HCC). Cancer stemness is closely connected with resistance to sorafenib. Methods for reversing the cancer stemness remains one of the largest concerns in research and the lack of such methods obstructs current HCC therapeutics. Ubiquitin-specific protease 22 (USP22) is reported to play a pivotal role in HCC stemness and multidrug resistance (MDR). Herein, a galactose-decorated lipopolyplex (Gal-SLP) is developed as an HCC-targeting self-activated cascade-responsive nanoplatform to co-delivery sorafenib and USP22 shRNA (shUSP22) for synergetic HCC therapy. Sorafenib, entrapped in the Gal-SLPs, induced a reactive oxygen species (ROS) cascade and triggered rapid shUSP22 release. Thus, Gal-SLPs dramatically suppressed the expression of USP22. The downregulation of USP22 suppresses multidrug resistance-associated protein 1 (MRP1) to induce intracellular sorafenib accumulation and hampers glycolysis of HCC cells. As a result, Gal-SLPs efficiently inhibit the viability, proliferation, and colony formation of HCC cells. A sorafenib-insensitive patient-derived xenograft (PDX) model is established and adopted to evaluate in vivo antitumor effect of Gal-SLPs. Gal-SLPs exhibit potent antitumor efficiency and biosafety. Therefore, Gal-SLPs are expected to have great potential in the clinical treatment of HCC., Competing Interests: The authors declare no conflict of interest., (© 2021 The Authors. Advanced Science published by Wiley‐VCH GmbH.)

Electrochemical sensing performance is often compromised by electrode biofouling (e.g., proteins nonspecific binding) in complex biological fluids; however, the design and construction of a robust biointerface remains a great challenge. Herein, inspired by nature, we demonstrate a robust polydopamine-engineered biointerfacing, to tailing zwitterionic molecules (i.e., sulfobetaine methacrylate, SBMA) through Michael Addition. The SBMA-PDA biointerface can resist proteins nonspecific binding in complex biological fluids while enhancing interfacial electron transfer and electrochemical stability of the electrode. In addition, this sensing interface can be integrated with tissue-implantable electrode for in vivo analysis with improved sensing performance, preserving ca. 92.0% of the initial sensitivity after 2 h of implantation in brain tissue, showing low acute neuroinflammatory responses and good stability both in normal and in Parkinson's disease (PD) rat brain tissue., (© 2020 Wiley-VCH GmbH.)

Temperature sensors play a significant role in biology, chemistry, and engineering, especially those that can work accurately in a noninvasive manner. We adopted a photoinduced post-synthetic copolymerization strategy to realize a membranous ratiometric luminescent thermometer based on the emissions of two lanthanide ions. This novel mixed-lanthanide polyMOF membrane exhibits not only the integrity and temperature sensing behaviour of the Ln-MOF powder but also excellent mechanical properties, such as flexibility, elasticity, and processability. Moreover, the polyMOF membrane shows remarkable stability under harsh conditions, including high humidity, strong acid and alkali (pH 0-14), which allowed the mapping of temperature distributions in extreme circumstances. This work highlights a simple strategy for polyMOF membrane formation and pushes forward the further practical application of Ln-MOF-based luminescent thermometers in various fields and conditions., (© 2020 Wiley-VCH GmbH.)

The unique three-dimensional structure of spidrion determines the outstanding mechanical properties of the spider silk fiber. Inspired by the similarity of the three-dimensional structure of superb-uranyl binding protein (SUP) to that of spidroin, a dual-SUP (DSUP) chimeric protein fiber with high tensile strength is designed. The DSUP hydrogel fiber exhibits a loofah-shape structure by the cross-interaction of the protein nanofiber. Full exposure of abundant functional uranyl-binding sites in the stretchable loofah-shape hydrogel protein fiber give the DSUP fiber a groundbreaking uranium extraction capacity of 17.45 mg g -1 with an ultrashort saturation time of 3 days in natural seawater. This work reports the design of an adsorbent with ultrahigh uranium extraction capacity and explores a strategy for fabricating artificial high-strength functional non-spidroin protein fiber., (© 2020 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Monolayer organic crystals have attracted considerable attention due to their extraordinary optoelectronic properties. Solution self-assembly on the surface of water is an effective approach to fabricate monolayer organic crystals. However, due to the difficulties in controlling the spreading of organic solution on the water surface and the weak intermolecular interaction between the organic molecules, large-area growth of monolayer organic crystals remains a great challenge. Here, a graphene quantum dots (GQDs)-induced self-assembly method for centimeter-sized growth of monolayer organic crystals on a GQDs solution surface is reported. The spreading area of the organic solution can be readily controlled by tuning the pH value of the GQDs solution. Meanwhile, the π-π stacking interaction between the GQDs and the organic molecules can effectively reduce the nucleation energy of the organic molecules and afford a cohesive force to bond the crystals, enabling large-area growth of monolayer organic crystals. Using 2,7-didecyl benzothienobenzothiopene (C 10 -BTBT) as an examples, centimeter-sized monolayer C 10 -BTBT crystal with uniform molecular packing and crystal orientation is attained. Organic field-effect transistors based on the monolayer C 10 -BTBT crystals exhibit a high mobility up to 2.6 cm 2 V -1 s -1 , representing the highest mobility value for solution-assembled monolayer organic crystals. This work provides a feasible route for large-scale fabrication of monolayer organic crystals toward high-performance organic devices., (© 2020 Wiley‐VCH GmbH.)

The efficient backbone-directed self-assembly of cyclic metalla[3]catenanes by the combination of tetrachloroperylenediimide (TCPDI)-based dinuclear rhodium(III) clips and 4,4'-diazopyridine or 4,4'-dipyridylethylene ligands is realized in a single-step strategy. The topology and coordination geometry of the cyclic metalla[3]catenanes are characterized by NMR spectroscopy, ESI-TOF-MS spectrometry, UV/Vis-NIR spectroscopy, and X-ray diffraction studies. The most remarkable feature of the formed cyclic metalla[3]catenane is that it contains π-aggregates (ca. 2.6 nm) incorporating six TCPDIs. Further studies revealed that cyclic metalla[3]catenanes can be converted reversibly to their corresponding sodium adducts and precursor building blocks, respectively. This strategy opens the possibility of generating unique supramolecular structures from discrete functional π-aggregates with precise arrangements., (© 2020 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Exploitation and utilization of sustainable energy sources has increasingly become the common theme of global social development, which has promoted tremendous development of energy conversion devices/technologies. Owing to excellent and unique optical/electrical properties, carbon dots (CDs) have attracted extensive research interest for numerous energy conversion applications. Strong absorption, downconversion photoluminescence, electron acceptor/donor characteristics, and excellent electron conductivity endow CDs with enormous potential for applications in optoelectronic devices. Furthermore, excellent electron transfers/transport capacities and easily manipulable structural defects of CDs offer distinct advantages for electrocatalytic applications. Recent advances in CD-based energy conversion applications, including optoelectronic devices such as light-emitting diodes and solar cells, and electrocatalytic reactions including the hydrogen evolution reaction, oxygen evolution reaction, oxygen reduction reaction, and carbon dioxide reduction reaction, are summarized. Finally, current challenges and future prospects for CD-based energy conversion applications are proposed, highlighting the importance of controllable structural design and modifications., (© 2020 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

The crosslink-enhanced emission effect was first proposed to explore the strong luminescence of nonconjugated polymer dots possessing only either non-emissive or weakly emissive sub-luminophores. Interesting phenomena in recent research indicate such enhancement caused by extensive crosslinking appears in diverse luminescent polymers with sub-luminophores (electron-rich heteroatomic moieties) or luminophores (conjugated π domains). This enhancement can promote the emission from nonluminous to luminous, from weakly luminous to strongly luminous, and even convert the pathway of radiative transitions. The concept of the crosslink-enhanced emission effect should be updated and extended to an in-depth spatial effect, such as electron overlap and energy splitting in confined domains by effective crosslinking, more than initial immobilization. This Minireview outlines the development of the crosslink-enhanced emission effect from the perspective of the detailed classification, inherent mechanism and applicable systems. An outlook on the further exploration and application of this theory are also proposed., (© 2020 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.)

GSTP1 has been considered to be a marker for malignancy in many tissues. However, the existing GST fluorescent probes are unfavorable for in vivo imaging because of the limited emission wavelength or insufficient fluorescence enhancement (six-fold). The limited fluorescence enhancement of GST fluorescent probes is mainly ascribed to the high background signals resulting from the spontaneous reaction between GSH and the probes. In this work, a highly specific GST probe with NIR emission has been successfully developed through optimization of the essential unit of the probe to repress the spontaneous reaction. The novel GST probe exhibits over 100-fold fluorescence enhancement upon incubation with GSTP1/GSH and high selectivity over other potential interference. In addition, the probe has been proved to be capable of tracking endogenous GST in A549 cells. Finally, the in vivo imaging results demonstrate that the probe can be used for effective imaging of endogenous GST activity in subcutaneous tumor mouse with high contrast., (© 2020 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Vibralactone is isolated from the basidiomycete fungus Boreostereum vibrans as one of the strongest lipase inhibitors. Its unusual β-lactone-fused bicycle is derived from an aryl ring moiety by an oxidative ring-expansion prior to an intramolecular cyclization. Herein, we report the discovery of the cyclase VibC which belongs to the α/β-hydrolase superfamily and is involved in the vibralactone biosynthesis. Biochemical and crystal studies suggest that VibC may catalyze an aldol or an electrocyclic reaction initiated by the Ser-His-Asp catalytic triad. For the aldol and pericyclic chemistry in living cells, VibC is a unique hydrolase performing the carbocycle formation of an oxepinone to a fused bicyclic β-lactone. This presents a naturally occurring, new enzymatic reaction in both aldol and hydrolase (bio)chemistry that will guide future exploitation of these enzymes in synthetic biology for chemical-diversity expansion of natural products., (© 2020 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Needle placement is important for many clinical interventions, such as tissue biopsy, regional anesthesia and drug delivery. It is essential to visualize the spatial position of the needle and the target tissue during the interventions using appropriate imaging techniques. Based on the contrast of optical absorption, photoacoustic imaging is well suited for the guidance of interventional procedures. However, conventional photoacoustic imaging typically provides two-dimensional (2D) slices of the region of interest and could only visualize the needle and the target when they are within the imaging plane of the probe at the same time. This requires great alignment skill and effort. To ease this problem, we developed a 3D interventional photoacoustic imaging technique by fast scanning a linear array ultrasound probe and stitching acquired image slices. in vivo sentinel lymph node biopsy experiment shows that the technique could precisely locate a needle and a sentinel lymph node in a tissue volume while a perfusion experiment demonstrates that the technique could visualize the 3D distribution of injected methylene blue dye underneath the skin at high temporal and spatial resolution. The proposed technique provides a practical way for photoacoustic image-guided interventions., (© 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Industrial applications of Pt-based oxygen-reduction-reaction (ORR) catalysts are limited by high cost and low stability. Here, facile large-scale synthesis of sub-3-nm ordered Pt 3 In clusters on commercial carbon black as ORR catalyst that alleviates both these shortcomings is reported. As-prepared Pt 3 In/C exhibits a mass activity of 0.71 mA mg -1 and a specific area activity of 0.91 mA cm -2 at 0.9 V vs reversible hydrogen electrode, which are 4.1 and 2.7 times the corresponding values of commercial Pt/C catalysts. The as-prepared ordered Pt 3 In/C catalyst is also remarkably stable with negligible activity and structural decay after 20 000 accelerated electrochemical durability cycles, due to its ordered structure. Density-functional-theory calculations demonstrate that ordered-Pt 3 In is more energetically favorable for ORR than the commercial Pt/C catalysts because ∆ G O is closer to the peak of the volcano plot after ordered incorporation of indium atoms., Competing Interests: The authors declare no conflict of interest., (© 2019 The Authors. Published by WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim.)

The design and development of low-cost, highly efficient, and stable electrocatalysts to take the place of noble-metal catalysts for the oxygen evolution reaction (OER) remain a significant challenge. Herein, the synthesis of yolk-shell-structured binary transition metal phosphide Co x Fe 1-x P with different Co/Fe ratios by phosphidation of a cobalt ferrite precursor is reported. The as-synthesized Co x Fe 1-x P catalysts were used for the OER. All yolk-shell Co x Fe 1-x P catalysts with different Co/Fe ratios showed much better performance than the corresponding solid catalyst. The formation of Co oxides on the catalyst surface during OER and the optimal Co/Fe ratio were found to be critical to their activity. Among the as-prepared Co x Fe 1-x P catalysts, that with a Co/Fe ratio of 0.47/0.53 (Co 0.47 Fe 0.53 P) exhibited the best performance. Co 0.47 Fe 0.53 P has an overpotential of 277 mV at a current density of 10 mA cm -2 , a Tafel slope of 37 mV dec -1 , and superior stability in alkaline medium. The outstanding performance is partly ascribed to the transfer of valence electrons from Co to P and Fe. The Co 0.47 Fe 0.53 P matrix with excellent conductivity and Fe phosphate that is stable on the surface of the catalyst are also helpful for the OER performance. In addition, the yolk-shell structure of Co 0.47 Fe 0.53 P increases the contact area between electrolyte and catalyst. These characteristics of Co 0.47 Fe 0.53 P greatly improve its OER performance. This optimized binary transition metal phosphide provides a new approach for the design of nonprecious-metal electrocatalysts., (© 2019 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Despite the various synthesis methods to obtain carbon dots (CDs), the bottom-up methods are still the most widely administrated route to afford large-scale and low-cost synthesis. However, as CDs are developed with increasing reports involved in producing many CDs, the structure and property features have changed enormously compared with the first generation of CDs, raising classification concerns. To this end, a new classification of CDs, named carbonized polymer dots (CPDs), is summarized according to the analysis of structure and property features. Here, CPDs are revealed as an emerging class of CDs with distinctive polymer/carbon hybrid structures and properties. Furthermore, deep insights into the effects of synthesis on the structure/property features of CDs are provided. Herein, the synthesis methods of CDs are also summarized in detail, and the effects of synthesis conditions of the bottom-up methods in terms of the structures and properties of CPDs are discussed and analyzed comprehensively. Insights into formation process and nucleation mechanism of CPDs are also offered. Finally, a perspective of the future development of CDs is proposed with critical insights into facilitating their potential in various application fields., Competing Interests: The authors declare no conflict of interest., (© 2019 The Authors. Published by WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim.)

In this work, a novel biomimetic surface-attachable initiator is successfully synthesized by the conjugation of 3,4-dihydroxyphenylacetic acid and thermal 2,2'-azobis(2-methylpropionamide) dihydrochloride (V-50). The synthesized initiator (DOPV) can adhere to various material surfaces in a mussel-inspired way and initiate the surface grafting polymerization. Hydrogel coatings are facilely prepared by the thermal-initiated radical copolymerization of antimicrobial polyhexamethylene guanidine and antifouling polyethylene glycol oligomers. The developed hydrogel coatings not only show antimicrobial activity toward gram-negative and gram-positive bacteria but also demonstrate protein resistance, antibiofilm efficacy, hemocompatibility, and low cytotoxicity in vitro. Most importantly, the hydrogel coatings reveal excellent antimicrobial efficacy with a log reduction above 5 in a rodent subcutaneous infection model. These results demonstrate the potential fabrication of bio-functional coatings for biomedical devices or implants through an inexpensive, facile, and environmentally friendly mussel-inspired technique., (© 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)