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Abstract H2O2 photosynthesis represents an appealing approach for sustainable and decentralized H2O2 production. Unfortunately, current reactions are mostly carried out in laboratory-scale single-phase batch reactors, which have a limited H2O2 production rate (

Abstract The synthesis of multi-carbon (C2+) fuels via electrocatalytic reduction of CO, H2O using renewable electricity, represents a significant stride in sustainable energy storage and carbon recycling. The foremost challenge in this field is the production of extended-chain carbon compounds (Cn, n ≥ 3), wherein elevated *CO coverage (θco) and its subsequent multiple-step coupling are both critical. Notwithstanding, there exists a “seesaw” dynamic between intensifying *CO adsorption to augment θco and surmounting the C-C coupling barrier, which have not been simultaneously realized within a singular catalyst yet. Here, we introduce a facilely synthesized lattice-strain-stabilized nitrogen-doped Cu (LSN-Cu) with abundant defect sites and robust nitrogen integration. The low-coordination sites enhance θco and concurrently, the compressive strain substantially fortifies nitrogen dopants on the catalyst surface, promoting C-C coupling activity. The n-propanol formation on the LSN-Cu electrode exhibits a 54% faradaic efficiency and a 29% half-cell energy efficiency. Moreover, within a membrane electrode assembly setup, a stable n-propanol electrosynthesis over 180 h at a total current density of 300 mA cm−2 is obtained.

Abstract The proton exchange membrane water electrolyzer (PEMWE), crucial for green hydrogen production, is challenged by the scarcity and high cost of iridium‐based materials. Cobalt oxides, as ideal electrocatalysts for oxygen evolution reaction (OER), have not been extensively applied in PEMWE, due to extremely high voltage and poor stability at large current density, caused by complicated structural variations of cobalt compounds during the OER process. Thus, the authors sought to introduce chromium into a cobalt spinel (Co3O4) catalyst to regulate the electronic structure of cobalt, exhibiting a higher oxidation state and increased Co–O covalency with a stable structure. In‐depth operando characterizations and theoretical calculations revealed that the activated Co–O covalency and adaptable redox behavior are crucial for facilitating its OER activity. Both turnover frequency and mass activity of Cr‐doped Co3O4 (CoCr) at 1.67 V (vs RHE) increased by over eight times than those of as‐synthesized Co3O4. The obtained CoCr catalyst achieved 1500 mA cm−2 at 2.17 V and exhibited notable durability over extended operation periods – over 100 h at 500 mA cm−2 and 500 h at 100 mA cm−2, demonstrating promising application in the PEMWE industry.

Abstract Organic photovoltaics have attracted worldwide interest due to their unique advantages in developing low-cost, lightweight, and flexible power sources. Functional molecular design and synthesis have been put forward to accelerate the discovery of ideal organic semiconductors. However, it is extremely expensive to conduct experimental screening of the wide organic compound space. Here we develop a framework by combining a deep learning model (graph neural network) and an ensemble learning model (Light Gradient Boosting Machine), which enables rapid and accurate screening of organic photovoltaic molecules. This framework establishes the relationship between molecular structure, molecular properties, and device efficiency. Our framework evaluates the chemical structure of the organic photovoltaic molecules directly and accurately. Since it does not involve density functional theory calculations, it makes fast predictions. The reliability of our framework is verified with data from previous reports and our newly synthesized organic molecules. Our work provides an efficient method for developing new organic optoelectronic materials.

Abstract Polymer nanocomposites with nanoparticles dispersed in polymer matrices have attracted extensive attention due to their significantly improved overall performance, in which the nanoparticle-polymer interface plays a key role. Understanding the structures and properties of the interfacial region, however, remains a major challenge for polymer nanocomposites. Here, we directly observe the presence of two interfacial polymer layers around a nanoparticle in polar polymers, i.e., an inner bound polar layer (~10 nm thick) with aligned dipoles and an outer polar layer (over 100 nm thick) with randomly orientated dipoles. Our results reveal that the impacts of the local nanoparticle surface potential and interparticle distance on molecular dipoles induce interfacial polymer layers with different polar molecular conformations from the bulk polymer. The bilayer interfacial features lead to an exceptional enhancement in polarity-related properties of polymer nanocomposites at ultralow nanoparticle loadings. By maximizing the contribution of inner bound polar layer via a nanolamination design, we achieve an ultrahigh dielectric energy storage density of 86 J/cm3, far superior to state-of-the-art polymers and nanocomposites.

Well-defined metastable phase nanostructures are a core issue for catalyst design. Here, the authors report metastable monoclinic phase IrO2 nanoribbons obtained via a molten-alkali mechanochemical method, which exhibit intrinsic high performance towards the acidic oxygen evolution reaction.

The construction of well-ordered nanoarrays, particularly invoking metastable material phases, remains a challenge. Here, authors prepared a well-ordered, rhodium nanoarray on two-dimensional, metastable rhodium oxide to enhance hydrogen evolution electrocatalysis.

While water electrolysis devices represent a technology for renewable energy, there are few stable catalysts that survive the acidic conditions. Here, authors enhance acidic oxygen evolution by introducing strong Brønsted acid sites into RuO2 to accelerate bridging-oxygen-assisted deprotonation.

Guided by high-throughput computational screening, we report the preparation of hydrogen-bonded cobaltoporphyrin frameworks and demonstrate the achievement of high activity and selectivity for electrochemical H2O2 production in acid.

Abstract Catalytic reactions are surface‐sensitive processes. Fabrication of homogeneous metastable metals can be used to promote phase‐dependent catalytic performance; however, this has been a challenging task. Herein, homogeneous metastable hexagonal close‐packed (hcp) Ir is epitaxially grown onto metastable phase hcp Ni, as demonstrated using spherical aberration electron microscopy. The as‐fabricated metastable hcp Ir exhibits high intrinsic activity for the alkaline hydrogen evolution reaction (HER). In particular, metastable hcp Ir delivers a low overpotential of 17 mV at 10 mA cm−2 and presents a high specific activity of 8.55 mA cm−2 and a high turnover frequency of 38.26 s−1 at −0.07 V versus the reversible hydrogen electrode. Owing to its epitaxially grown structure, metastable hcp Ir is highly stable. Theoretical calculations reveal that metastable hcp Ir promotes H2O adsorption and fast H2O dissociation, which contributes to its remarkable HER activity. Findings can elucidate the crystal phase‐controlled synthesis of advanced noble metal nanomaterials for the fundamental catalytic applications.

Mature corn grains is an important food ration for residents in our country, but its edible flavor quality was rarely reported. The volatile organic components (VOCs) in whole grain powder with different treatment of 5 high-quality yellow grain maize varieties were detected with gas chromatography-mass spectrometry (GC-MS), the results showed that a total of 101 species of VOCs were identified, but only 60~70 species were found in a single variety. These VOCs could be divided into 12 categories, of which, the number of esters, alkanes and ketones were more, followed by alcohols, aldehydes and amides. When the composition of VOCs were analyzed, it was also found that there were about 20 species of components with high content at the level of over 106 peak area, which constituted 80% of the total volatile substances content, in these high content components, 13 were co-owned which were present in all samples, and 4~16 were specific which varied among varieties. There were two species of high content components at the level of 107 peak area，n-dodecane and tert-butanol were identified, which were considered to be important volatile substances in corn. The detection results also showed that the relative total content of VOCs in the samples distributed from 36.660 to 68.001 mg/kg. When they were compared each other, it was also found that the total content of VOCs was significantly different among varieties and samples, including different storage time and packages. The content of aroma substances in newly harvested grains was the highest. The ears or grains was stored naturally 1 year, its VOCs lost about 1/5. While the whole powder was stored naturally 1 year, its VOCs lost nearly a third. But the powder being stored in vacuum bags and under the low temperature 3 years, the loss of VOCs was slightly. These results suggested that the aroma substances content in corn was a variety characteristic. Excellent varieties and special production areas could effectively increase the kinds and the content of aroma substances in grains. Storage time and storage conditions could significantly affect the quality of aroma. Storage under the conditions of low temperature and vacuum could effectively maintain the quality of aroma. These results provided important reference data for quality evaluation of high quality edible corn.

Catalytic hydrogenolysis of end-of-life polyolefins can produce value-added liquid fuels and therefore holds great promises in plastic waste reuse and environmental remediation. The major challenge limiting the recycling economic benefit is the severe methanation (usually >20%) induced by terminal C–C cleavage and fragmentation in polyolefin chains. Here, we overcome this challenge by demonstrating that Ru single-atom catalyst can effectively suppress methanation by inhibiting terminal C–C cleavage and preventing chain fragmentation that typically occurs on multi-Ru sites. The Ru single-atom catalyst supported on CeO2 shows an ultralow CH4 yield of 2.2% and a liquid fuel yield of over 94.5% with a production rate of 314.93 gfuels gRu−1 h−1 at 250 °C for 6 h. Such remarkable catalytic activity and selectivity of Ru single-atom catalyst in polyolefin hydrogenolysis offer immense opportunities for plastic upcycling.

The electrochemical conversion of carbon monoxide (CO) to value-added chemical products is promising for carbon utilization and CO removal. Herein we explored the potential of two-dimensional metal-embedded polyphthalocyanines (MPPcs) for electro-catalytic CO reduction reaction (CORR) by computational approach. The CrPPc, MnPPc, CoPPc, and MoPPc are initially screened out as the candidates. Then the optimal reaction pathways and corresponding potential determining steps (PDS) are determined by calculating free energies of all the possible intermediates. Based on our results, the CrPPc, MnPPc, and MoPPc could efficiently reduce CO into methane (CH4), among which the CrPPc exhibits the highest performance.

Ni-based single-atom catalysis (Ni-SAC) has been experimentally reported with superior performance in reducing CO2 to CO. However, due to the ambiguities in its structures, the active sites of Ni-SAC that are responsible for superior performance have not yet been resolved. This work investigates the CO2 reduction reaction (CO2RR) mechanism on Ni-SAC by carrying out quantum mechanics (QM) simulation to consider both solvation effects. After exploring multiple possible combinations of N, S, and C, we distinguish a Ni-SAC site with two C, one S, and one N, representing the best performance. The predicted formation energy is closely consistent with experimental onset potential. Our prediction also suggests further improvement by finely tuning the electronics state of metal sites by changing the SAC support.

Identifying new, active material phases provides a promising avenue in the development of efficient catalysts. Here, authors demonstrate a metastable 1T-phase IrO2 metallene oxide as an oxygen evolution electrocatalyst in acidic electrolytes.

Abstract Over past two decades, organic photovoltaics (OPVs) with unique advantages of low cost and flexibility meet significant development opportunities and the official world record for the power conversion efficiency (PCE) of organic solar cells (OSCs) has reached to 17.3%. Traditionally, efficiency breakthrough need the constant input of intensive labor and time. The artificial intelligence, as a rising interdisciplinary, brings certainly a revolution in research methods. In this review, we introduce a state‐of‐art theoretical methodology of the synergy of high‐throughput screening and machine learning (ML) in accelerating the discovery of high‐efficient OSC materials. We present key details, rules and experience in database construction, selection of molecular features, fast‐screening calculations, models training and their predication capabilities. Meanwhile, three typical ML frameworks are concluded to reveal the structure‐property‐efficiency relationship, suggesting that this theoretical methodology can train powerful models with just molecular configurations and theoretical calculations for molecular design and efficiency improvements.

Abstract Here, we report a density functional theory (DFT)-based high-throughput screening method to successfully identify a type of alloy nanoclusters as the electrocatalyst for hydrogen evolution reaction (HER). Totally 7924 candidates of Cu-based alloy clusters of Cu55-n M n (M = Co, Ni, Ru, and Rh) are optimized and evaluated to screening for the promising catalysts. By comparing different structural patterns, Cu-based alloy clusters prefer the core–shell structures with the dopant metal in the core and Cu as the shell atoms. Generally speaking, the HER performance of the Cu-based nanoclusters can be significantly improved by doping transition metals, and the active sites are the bridge sites and three-fold sites on the outer-shell Cu atoms. Considering the structural stability and the electrochemical activity, core–shell CuNi alloy clusters are suggested to be the superior electrocatalyst for hydrogen evolution. A descriptor composing of surface charge is proposed to efficiently evaluate the HER activity of the alloy clusters supported by the DFT calculations and machine-learning techniques. Our screening strategy could accelerate the pace of discovery for promising HER electrocatalysts using metal alloy nanoclusters.

Developing organic photoluminescent materials with high emission efficiencies in the solid state under a water atmosphere is important for practical applications. Here, the authors report the formation of intra- and intermolecular hydrogen bonds in a tautomerizable Schiff base and intercalation of water in the crystal lattice leading to a luminescent organic hydrate.

Tea is an important beverage crop with a large and heterozygous genome. Here, the authors assemble the genome of the cultivar Longjing 43 and conduct a population genetics study to reveal divergent selection for disease resistance and flavor between the two variety groups.

Abstract Background The growth process of the tea plant (Camellia sinensis) includes vegetative growth and reproductive growth. The reproductive growth period is relatively long (approximately 1.5 years), during which a large number of nutrients are consumed, resulting in reduced tea yield and quality, accelerated aging, and shortened economic life of the tea plant. The formation of unisexual and sterile flowers can weaken the reproductive growth process of the tea plant. To further clarify the molecular mechanisms of pistil deletion in the tea plant, we investigated the transcriptome profiles in the pistil-deficient tea plant (CRQS), wild tea plant (WT), and cultivated tea plant (CT) by using RNA-Seq. Results A total of 3683 differentially expressed genes were observed between CRQS and WT flower buds, with 2064 upregulated and 1619 downregulated in the CRQS flower buds. These genes were mainly involved in the regulation of molecular function and biological processes. Ethylene synthesis–related ACC synthase genes were significantly upregulated and ACC oxidase genes were significantly downregulated. Further analysis revealed that one of the WIP transcription factors involved in ethylene synthesis was significantly upregulated. Moreover, AP1 and STK, genes related to flower development, were significantly upregulated and downregulated, respectively. Conclusions The transcriptome analysis indicated that the formation of flower buds with pistil deletion is a complex biological process. Our study identified ethylene synthesis, transcription factor WIP, and A and D-class genes, which warrant further investigation to understand the cause of pistil deletion in flower bud formation.

Separating molecules or ions with sub-Angstrom scale precision is important but technically challenging. Here, the authors demonstrate that precise solute-solute separation can be achieved using polyamide membranes formed via surfactant-assembly regulated interfacial polymerization.

An understanding of the spectrum–property relationship of perovskite solar cells when illuminated by light‐emitting diodes that are used for indoor applications is necessary. Herein, it is aimed to explore the influences of correlated‐color temperatures on a MAPbI3‐based device under low‐light conditions. Given an irradiance of approximately 3 W m−2 (or ≈1000 lx), a maximum free carrier generation rate of 1.0 × 1021 m−3 s−1 was found. Additionally, power conversion efficiencies (PCEs) up to 31.97%, 30.36%, and 28.98% with maximum power outputs of 13.66, 13.02, and 16.09 μW could be reached at 3000, 4000, and 6500 K, respectively. Additional increases in the PCEs were observed when high‐energy blue light (in a range of 400–550 nm) was excluded during the current–voltage sweeps. In combination with the surface photovoltage measurements, intense blue light (under 6500 K) had a minimal influence on the photoinduced charge separation signals when compared to those caused by 3000 and 4000 K light. As a solar cell, the PCE reached as high as 34.52%, which corresponded to 73.08% of the thermodynamic limit of its bandgap at 3000 K.

Summary: It is challenging to realize high efficiency and stability in perovskite photovoltaics simultaneously. Here, we show supramolecular chemistry using macrocyclic crown ether to prepare high-performance metal-halide perovskite films. Multiple cooperative supramolecular interactions between perovskites and crown ether are built, and superior defect passivation is achieved. A thin crystalline capping layer on top of perovskites is constructed to synergistically passivate the perovskite surface defects and protect the underlying films from environmental damage. The capping layer is confirmed to be a unique two-dimensional (2D) crystal with a highly ordered, high-crystallinity lamellae structure and face-sharing lead-halide octahedral organization, providing surface protection on the perovskite matrix. Lead-halide perovskite solar cells (PSCs) with supramolecular passivation and a 2D crystal interlayer demonstrated remarkable photovoltaic efficiency and stability improvements, offering a 21.5% efficiency and improved environmental stabilities under moisture, ultraviolet (UV) irradiation, and thermal stress. Our work provides a strategy to achieve efficient and stable lead-halide perovskite-based devices by crown ether-induced supramolecular passivation and 2D crystal interlayer protection.

Electrocatalytic water splitting for hydrogen and oxygen generation provides an attractive path to obtain clean energy, but the half reaction of oxygen evolution remains the bottleneck for the progress. Here, the authors show single atom tungsten doped ultrathin α-Ni(OH)2 exhibits enhanced performance in electrocatalytic water oxidation.

Dithienopicenocarbazole (DTPC), as the kernel module in A-D-A non-fullerene acceptors (NFA), has been reported for its ultra-narrow bandgap, high power conversion efficiency, and extremely low energy loss. To further improve the photovoltaic performance of DTPC-based acceptors, molecular engineering of end-capped groups could be an effective method according to previous research. In this article, a class of acceptors were designed via bringing terminal units with an enhanced electron-withdrawing ability to the DTPC central core. Their geometrical structures, frontier molecular orbitals, absorption spectrum, and intramolecular charge transfer and energy loss have been systematically investigated on the basis of density functional theory (DFT) and time-dependent density functional theory (TD-DFT) calculations. Surprisingly, NFA 4 highlights the dominance for its increased open circuit voltages while NFA 2, 7, and 8 exhibit great potential for their enhanced charge transfer and lower energy loss, corresponding to a higher short-circuit current density. Our results also manifest that proper modifications of the terminal acceptor with extensions of π-conjugation might bring improved outcomes for overall properties. Such a measure could become a feasible strategy for the synthesis of new acceptors, thereby facilitating the advancement of organic solar cells.

The D genome progenitor of bread wheat, Aegilops tauschii Cosson (DD, 2n = 2x = 14), which is naturally distributed in Central Eurasia, ranging from northern Syria and Turkey to western China, is considered a potential genetic resource for improving bread wheat. In this study, the chloroplast (cp) genomes of 17 Ae. tauschii accessions were reconstructed. The cp genome sizes ranged from 135,551 bp to 136,009 bp and contained a typical quadripartite structure of angiosperms. Within these genomes, we identified a total of 124 functional genes, including 82 protein-coding genes, 34 transfer RNA genes and eight ribosomal RNA genes, with 17 duplicated genes in the IRs. Although the comparative analysis revealed that the genomic structure (gene order, gene number and IR/SC boundary regions) is conserved, a few variant loci were detected, predominantly in the non-coding regions (intergenic spacer regions). The phylogenetic relationships determined based on the complete genome sequences were consistent with the hypothesis that Ae. tauschii populations in the Yellow River region of China originated in South Asia not Xinjiang province or Iran, which could contribute to more effective utilization of wild germplasm resources. Furthermore, we confirmed that Ae. tauschii was derived from monophyletic speciation rather than hybrid speciation at the cp genome level. We also identified four variable genomic regions, rpl32-trnL-UAG, ccsA-ndhD, rbcL-psaI and rps18-rpl20, showing high levels of nucleotide polymorphisms, which may accordingly prove useful as cpDNA markers in studying the intraspecific genetic structure and diversity of Ae. tauschii.

It is highly desirable, while still challenging, to obtain noble metal nanocrystals with custom capping ligands, because their colloidal synthesis relies on specific capping ligands for the shape control while conventional ligand exchange processes suffer from “the strong replaces the weak” limitation, which greatly hinders their applications. Herein, we report a general and effective ligand exchange approach that can replace the native capping ligands of noble metal nanocrystals with virtually any type of ligands, producing flexibly tailored surface properties. The key is to use diethylamine with conveniently switchable binding affinity to the metal surface as an intermediate ligand. As a strong ligand, it in its original form can effectively remove the native ligands; while protonated, it loses its binding affinity and facilitates the adsorption of new ligands, especially weak ones, onto the metal surface. By this means, the irreversible order in the conventional ligand exchange processes could be overcome. The efficacy of the strategy is demonstrated by mutual exchange of the capping ligands among cetyltrimethylammonium, citrate, polyvinylpyrrolidone, and oleylamine. This novel strategy significantly expands our ability to manipulate the surface property of noble metal nanocrystals and extends their applicability to a wide range of fields, particularly biomedical applications.

Lithium-sulfur (Li-S) batteries can provide far higher energy density than currently commercialized lithium ion batteries, but challenges remain before it they are used in practice. One of the challenges is the shuttle effect that originates from soluble intermediates, like lithium polysulfides. To address this issue, we report a novel laminar composite, N,O-carboxymethyl chitosan-reduced graphene oxide (CC-rGO), which is manufactured via the self-assembly of CC onto GO and subsequent reduction of GO under an extreme condition of 1 Pa and −50 °C. The synthesized laminar CC-rGO composite is mixed with acetylene black (AB) and coated on a commercial polypropylene (PP) membrane, resulting in a separator (CC-rGO/AB/PP) that can not only completely suppress the polysulfides penetration, but also can accelerate the lithium ion transportation, providing a Li-S battery with excellent cyclic stability and rate capability. As confirmed by theoretic simulations, this unique feature of CC-rGO is attributed to its strong repulsive interaction to polysulfide anions and its benefit for fast lithium ion transportation through the paths paved by the heteroatoms in CC.

Radialenes have distinct structural, electronic and chemical properties from other hydrocarbons, but their synthesis remains a challenge. Here, the authors report a copper catalyzed one-step synthetic protocol of [4]radialene via the cyclotetramerization of phenylacetylene molecules upon thermal activation.

Abstract Janus kinase 2 (JAK2) has been regarded as an essential target for the treatment of myeloproliferative neoplasms (MPNs). BBT594 and CHZ868, Type-II inhibitors of JAK2, illustrate satisfactory efficacy in preclinical MPNs and acute lymphoblastic leukemia (ALL) models. However, the L884P mutation of JAK2 abrogates the suppressive effects of BBT594 and CHZ868. In this study, conventional molecular dynamics (MD) simulations, umbrella sampling (US) simulations and MM/GBSA free energy calculations were employed to explore how the L884P mutation affects the binding of BBT594 and CHZ868 to JAK2 and uncover the resistance mechanism induced by the L884P mutation. The results provided by the US and MD simulations illustrate that the L884P mutation enhances the flexibility of the allosteric pocket and alters their conformations, which amplify the conformational entropy change (−TΔS) and weaken the interactions between the inhibitors and target. Additionally, the structural analyses of BBT594 and CHZ868 in complex with the WT JAK2 illustrate that the drug tail with strong electronegativity and small size located in the allosteric pocket of JAK2 may enhance anti-resistance capability. In summary, our results highlight that both of the changes of the conformational entropies and enthalpies contribute to the L884P-induced resistance in the binding of two Type-II inhibitors into JAK2 kinase.

Using first-principles calculations, we have investigated the electronic and optical properties of MoSe2 with Se vacancies (SVSe, α-DVSe, and β-DVSe) and further repaired by halogen atoms (F, Cl, Br and I). For the MoSe2 with Se vacancies, Cl, Br and I atoms can occupy the Se vacancies and form three bonds with the neighboring Mo atoms, but F atom only can form two F-Mo bonds with the lowest adsorption energies due to its smaller atomic radius. Halogen atoms possess one more electron than Se atom, which results in a local magnetic moment of 1µB for single vacancy and 2µB for double vacancies. The MoSe2 with Se vacancies exhibits n-type doping semiconductor, which agrees well with the experimental observations. After halogen atoms doping in the defective site, the defective levels shift from electron donor levels to the electron acceptor levels, and finally reduces the n-type doping from the defective structure through a p-doping process. Compared to the defective MoSe2, absorption enhancement around low energy area of 0∼3 eV is observed in the halogen-repaired MoSe2 structures. Our results provide new insights in structural repairing of the transition metal dichalcogenides and promote their remarkable properties for applications in optoelectronics.

Design of hydrogen evolution catalysts needs to balance the hydrogen adsorption energy to facilitate easy adsorption and desorption. Here, the authors report a composite catalyst where hydrogen adsorption occurs on rhodium and desorbs from silicon which has a lower adsorption energy.

Clustering methods have been widely applied to the fault diagnosis of mechanical system, but the characteristic that the number of cluster needs to be determined in advance limits the application range of the method. In this paper, a novel clustering method combining the adaptive resonance theory (ART) with the similarity measure based on the Yu’s norm is presented and applied to the fault diagnosis of rolling element bearings, which can be adaptive to generate the number of cluster by the vigilance parameter test. Time-domain features, frequency-domain features, and time series model parameters are extracted to demonstrate the fault-related information about the bearings, and then considering the irrelevance or redundancy of some features many salient features are selected by an improved distance discriminant technique and input into the proposed clustering method to diagnose the faults of bearings. The experiment results confirmed that the proposed clustering method can diagnose the fault categories accurately and has better diagnosis performance compared with fuzzy ART and Self-Organizing Feature Map (SOFM).

By using first-principles calculations, we investigate the structural stability of nitrogen-doped (N-doped) graphene with graphitic-N, pyridinic-N and pyrrolic-N, and the transition metal (TM) atoms embedded into N-doped graphene. The structures and energetics of TM atoms from Sc to Ni embedded into N-doped graphene are studied. The TM atoms at N4V 2 forming a 4N-centered structure shows the strongest binding and the binding energies are more than 7 eV. Finally, we investigate the catalytic performance of N-doped graphene with and without TM embedding for O2 dissociation, which is a fundamental reaction in fuel cells. Compared to the pyridinic-N, the graphitic-N is more favorable to dissociate O2 molecules with a relatively low reaction barrier of 1.15 eV. However, the catalytic performance on pyridinic-N doped structure can be greatly improved by embedding TM atoms, and the energy barrier can be reduced to 0.61 eV with V atom embedded. Our results provide the stable structure of N-doped graphene and its potential applications in the oxygen reduction reactions.

Tyrosine kinases are regarded as excellent targets for chemical drug therapy of carcinomas. However, under strong purifying selection, drug resistance usually occurs in the cancer cells within a short term. Many cases of drug resistance have been found to be associated with secondary mutations in drug target, which lead to the attenuated drug-target interactions. For example, recently, an acquired secondary mutation, G2032R, has been detected in the drug target, ROS1 tyrosine kinase, from a crizotinib-resistant patient, who responded poorly to crizotinib within a very short therapeutic term. It was supposed that the mutation was located at the solvent front and might hinder the drug binding. However, a different fact could be uncovered by the simulations reported in this study. Here, free energy surfaces were characterized by the drug-target distance and the phosphate-binding loop (P-loop) conformational change of the crizotinib-ROS1 complex through advanced molecular dynamics techniques, and it was revealed that the more rigid P-loop region in the G2032R-mutated ROS1 was primarily responsible for the crizotinib resistance, which on one hand, impaired the binding of crizotinib directly, and on the other hand, shortened the residence time induced by the flattened free energy surface. Therefore, both of the binding affinity and the drug residence time should be emphasized in rational drug design to overcome the kinase resistance.

Nanoscale particles have become promising materials in many fields, such as cancer therapeutics, diagnosis, imaging, drug delivery, catalysis, as well as biosensors. In order to stimulate and facilitate these applications, there is an urgent need for the understanding of the interaction mode between the nano-particles and proteins. In this study, we investigate the orientation and adsorption between several enzymes (cytochrome c, RNase A, lysozyme) and 4 nm/11 nm silica nanoparticles (SNPs) by using molecular dynamics (MD) simulation. Our results show that three enzymes are adsorbed onto the surfaces of both 4 nm and 11 nm SNPs during our MD simulations and the small SNPs induce greater structural stabilization. The active site of cytochrome c is far away from the surface of 4 nm SNPs, while it is adsorbed onto the surface of 11 nm SNPs. We also explore the influences of different groups (-OH, -COOH, -NH2 and CH3) coated onto silica nanoparticles, which show significantly different impacts. Our molecular dynamics results indicate the selective interaction between silicon nanoparticles and enzymes, which is consistent with experimental results. Our study provides useful guides for designing/modifying nanomaterials to interact with proteins for their bio-applications.

In recent years, numerous single-atom catalysts (SACs) have emerged and showed superior catalytic performance. Although different substrates lead to diverse activity, the substrate-dependent catalytic mechanism is still unrevealed. In this work, by taking the CO oxidation reaction as a representative, we have investigated the substrate-dependent catalytic activity of single-atom Pt using different inorganic perovskites (ABO3) as the substrates. It is found that the interaction between the single atom Pt and substrates plays a crucial role in determining the catalytic activity, and the stronger interaction of Pt with the substrates could stabilize the active centre towards a significantly lower energy barrier for CO oxidation. Furthermore, a simple descriptor of the angle of adsorbed CO is proposed to estimate the reaction barrier. The larger tilt angle of the adsorbed CO represents the relatively stronger adsorption strength of CO with Pt, resulting in a higher energy barrier for CO oxidation. Finally, Pt-SrNiO3 and Pt-SrAgO3 are screened out as promising SACs for the CO oxidation reaction with low barriers of 0.64 eV and 0.71 eV, respectively. Therefore, the catalytic performance of single-atom Pt catalysts could be efficiently regulated by the substrates to achieve high stability and activity. [ABSTRACT FROM AUTHOR]