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Optimizing high-coordination shell of Co-based single-atom catalysts for efficient ORR and zinc-air batteries

Journal of Energy Chemistry 2024年第8期95卷 306-314,I0007页

作者： Yugang Qi Qing liang Kexin Song Xinyan zhou Meiqi Liu Wenwen Li fuxi Liu zhou Jiang Xu Zou Zhongjun Chen Wei Zhang Weitao Zheng Key Laboratory of Automobile Materials MOE School of Materials Science&Engineering Electron Microscopy Centerand International Center of Future ScienceJilin Provincial International Cooperation Key Laboratory of High-Efficiency Clean Energy MaterialsJilin UniversityChangchun 130012JilinChina Institute of High Energy Physics Chinese Academy of SciencesBeijing 100049China

Atom-level modulation of the coordination environment for single-atom catalysts(SACs)is considered as an effective strategy for elevating the catalytic *** the MNxsite,breaking the symmetrical geometry and charge distribution by introducing relatively weak electronegative atoms into the first/second shell is an efficient way,but it remains challenging for elucidating the underlying mechanism of ***,a practical strategy was reported to rationally design single cobalt atoms coordinated with both phosphorus and nitrogen atoms in a hierarchically porous carbon derived from metal-organic frameworks.X-ray absorption spectrum reveals that atomically dispersed Co sites are coordinated with four N atoms in the first shell and varying numbers of P atoms in the second shell(denoted as Co-N/P-C).The prepared catalyst exhibits excellent oxygen reduction reaction(ORR)activity as well as zinc-air battery *** introduction of P atoms in the Co-SACs weakens the interaction between Co and N,significantly promoting the adsorption process of ^(*)OOH,resulting in the acceleration of reaction kinetics and reduction of thermodynamic barrier,responsible for the increased intrinsic *** discovery provides insights into an ultimate design of single-atom catalysts with adjustable electrocatalytic activities for efficient electrochemical energy conversion.

关键词： Electrocatalytic Oxygen reduction reaction Single atom catalyst Shell coordination optimization

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Research on Quantitative Identification of Three-Dimensional Connectivity of Fractured-Vuggy Reservoirs

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Energy Engineering 2024年第5期121卷 1195-1207页

作者： Xingliang Deng Peng Cao Yintao Zhang Yuhui zhou Xiao Luo liang Wang Exploration and Development Research Institute PetroChina Tarim Oilfield CompanyKorla841000China PetroChina Hangzhou Research Institute of Geology Hangzhou310023China School of Petroleum Engineering Yangtze UniversityWuhan430100China

The fractured-vuggy carbonate oil resources in the western basin of China are extremely *** connectivity of carbonate reservoirs is complex,and there is still a lack of clear understanding of the development and topological structure of the pore space in fractured-vuggy ***,effective prediction of fractured-vuggy reservoirs is *** view of this,this work employs adaptive point cloud technology to reproduce the shape and capture the characteristics of a fractured-vuggy *** identify the complex connectivity among pores,fractures,and vugs,a simplified one-dimensional connectivity model is established by using the meshless connection element method(CEM).Considering that different types of connection units have different flow characteristics,a sequential coupling calculation method that can efficiently calculate reservoir pressure and saturation is *** automatic history matching,the dynamic production data is fitted in real-time,and the characteristic parameters of the connection unit are *** results show that the three-dimensional connectivity model of the fractured-vuggy reservoir built in this work is as close as 90%of the fine grid model,while the dynamic simulation efficiency is much higher with good accuracy.

关键词： Fractured-vuggy reservoir three-dimensional connectivity connection unit dynamic prediction automatic history matching

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Electronic-scale assessment of high-temperature oxidation mechanisms in a novel Fe-based alloy

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Journal of Iron and Steel Research(International) 2024年第4期31卷 982-997页

作者： Wei-di Luo Ting-ping Hou Xuan liang Dong Zhang Heng-fu Lin Yu Li Tian-liang Zhao Cheng-yang Hu Serhii Yershov Kai-ming Wu The State Key Laboratory of Refractories and Metallurgy.Wuhan University of Science and Technology.Wuhan 430081 HubeiChina Hubei Province Key Laboratory of Systems Science in Meallurgial Process Wuhan University of Science and Technology.Wuhan 430081.Hubei.China International Research Institute for Steel Technology Wuhan University of Science and Technology.Wuhan 430081.HubeiChina Collaborative Innovation Center for Advanced Steels w uhan University of Science and Technology.Wuhan 430081.HuleiChina

The development of alloys with high antioxidation performance is limited by the ambiguous details of the oxidation ***,based on the structures of internal oxides detected by high-resolution transmission electron microscopy,a hybrid method combining first-principles calculation,climb image nudged elastic band method and quasi-harmonic Debye model has been implemented to explain the oxidation mechanism with an emphasis on the origin of delamination and *** results showed that the delamination of oxides corresponds to the acceleration of diffusion of Cr element caused by lamellar *** reduction in the cracking occurrence at high temperature mainly results from the smaller bulk modulus of ***,the stronger chemical bonds promoted by lamellar structures also correspond to the higher crackingresistance.

关键词： Oxidation Crystal structure Diffusion Cracking-First-principles calculation

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Fate of organophosphate esters from the Northwestern Pacific to the Southern Ocean:Occurrence,distribution,and fugacity model simulation

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Journal of Environmental Sciences 2024年第3期137卷 347-357页

作者： Tengda Shi Ruijing Li Jie fu Chao Hou Hui Gao Guanjie Cheng Haibo Zhang Shuaichen Jin liang Kong Guangshui Na College of Marine Technology and Environment Dalian Ocean UniversityDalian 116023China Laboratory for coastal marine eco-environment process and carbon sink of Hainan province/Yazhou Bay Innovation Institute Hainan Tropical Ocean UniversitySanya 572022China National Marine Environmental Monitoring Center Dalian 116023China College of Marine Ecology and Environment Shanghai Ocean UniversityShanghai 201306China NCS Testing Technology Co. Ltd.Beijing 10081China

Eleven organophosphate esters(OPEs)in the air and seawater were investigated from the northwestern Pacific Ocean to the Southern Ocean during the 2018 Chinese 34th Antarctic Scientific *** concentration of total OPEs ranged from 164.82 to 3501.79 pg/m~3in air and from 4.54 to 70.09 ng/L in *** halogenated OPEs,tri(chloropropyl)phosphate(TCPP)and tri(2-chloroethyl)phosphate(TCEP),were generally more abundant than the non-halogenated OPEs.A levelⅢfugacity model was developed to simulate the transfer and fate of seven OPEs in the air and seawater regions of the central Ross *** model results indicate that OPEs are transferred from the air to the seawater in the central Ross Sea in summer,during which the Ross Sea acts as a final OPE *** and wet deposition dominated the processes involving OPE transfer to *** OPE degradation process was also found to be more pervasive in the atmosphere than in the seawater *** findings highlights the importance of long-range transport of OPEs and their air–seawater interface behavior in the Antarctic.

关键词： Organophosphate esters(OPEs) Long-range transport fugacity model Antarctic Fate

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Hierarchical crystalline-amorphous nanocomposites with high strength and large deformability enabled by elemental diffusion

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Journal of Materials Science & Technology 2024年第4期171卷 150-161页

作者： Liqiang Wang Heyi Wang Xin zhou Huangliu fu James Utama Surjadi Shuo Qu Xu Song Rong Fan Yang Lu Department of Mechanical Engineering City University of Hong KongHong KongChina Nano-Manufacturing Laboratory(NML) Shenzhen Research Institute of City University of Hong KongShenzhen 518057China Chengdu Research Institute City University of Hong KongChengdu 610200China Shenyang National Laboratory for Materials Science Institute of Metal ResearchChinese Academy of SciencesShenyang 110016China Department of Mechanical and Automation Engineering The Chinese University of Hong KongHong KongChina Department of Mechanical Engineering The University of Hong KongHong KongChina

Amorphous/nanocrystalline dual-phase structures have recently emerged as an effective way for over-coming the strength-ductility trade-offand breaking the limitation of the reverse Hall-Petch ***,we proposed a new strategy to develop a hierarchical and interconnected amorphous-crystalline nanocomposite arising from the nanoscale elemental interdiffusion and oxygen adsorption behavior dur-ing thermal treatment *** nanocomposite consisted of a three-dimensional(3D)hierarchical network structure where the crystalline phase(Cr-Co-Ni-Al)was embedded into the Al-O-based amor-phous phase network with critical feature sizes encompassing three orders of magnitude(from microm-eter to nanometer scale).It can achieve ultrahigh compression yield strength of-3.6 GPa with large homogeneous deformation of over 50%*** massive interstitial atoms induced lattice distortion and hierarchical amorphous phase boundary contributed to the strength *** situ Uniaxial compression inside a transmission electron microscope(TEM)revealed that the exceptional deformability of the nanocomposites resulted from the homogenous plastic flow of nano-sized amorphous phase and the plastic co-deformation behavior restricted by the nano-architected dual-phase *** proposed dual-phase synthesis approach can outperform conventional nanolaminates design strategies in terms of the mechanical properties achievable while providing a pathway to easily tune the microstructure of these nanolaminates.

关键词： Nanolaminates Dual-phase nanocomposites In situ transmission electron microscopy Multi-component alloy

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Stability of bedded rock slopes subjected to hydro-fluctuation and associated strength deterioration

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Journal of Rock Mechanics and Geotechnical Engineering 2024年第8期16卷 3233-3257页

作者： Bin Xu Xinrong Liu Yue liang Xiaohan zhou Zuliang Zhong School of River and Ocean Engineering Chongqing Jiaotong UniversityChongqing400074China School of Civil Engineering Chongqing UniversityChongqing400045China

Reservoir-induced earthquakes(RIEs)occur frequently in the Three Gorges Reservoir Area(TGRA)and the rock mass strength of the hydro-fluctuation belt(HFB)deteriorates severely due to the reservoirinduced seismic *** models of typical bedded rock slopes(BRSs),***(GIS),moderately(MIS),and steeply(SIS)inclined slopes,were proposed according to field *** dynamic response mechanism and stability of the BRSs,affected by the rock mass deterioration of the HFB,were investigated by the shaking table test and the universal distinct element code(UDEC)***,the amplification coefficient of the peak ground acceleration(PGA)of the slope was gradually attenuated under multiple seismic loads,and the acceleration response showed obvious“surface effect”and“elevation effect”in the horizontal and vertical directions,***“S-type”cubic function and“steep-rise type”exponential function were used to characterize the cumulative damage evolution of the slope caused by microseismic waves(low seismic waves)and high seismic waves,*** to the dynamic responses of the acceleration,cumulative displacement,rock pressure,pore water pressure,damping ratio,natural frequency,stability coefficient,and sliding velocity of the slope,the typical evolution processes of the dynamic cumulative damage and instability failure of the slope were generalized,and the numerical and experimental results were *** the dynamic effects of the slope height(SH),slope angle(SA),bedding plane thickness(BPT),dip angle of the bedding plane(DABP),dynamic load amplitude(DLA),dynamic load frequency(DLF),height of water level of the hydro-fluctuation belt(HWLHFB),degradation range of the hydro-fluctuation belt(DRHFB),and degradation shape of the hydro-fluctuation belt(DSHFB),the sensitivity of factors influencing the slope dynamic stability using the orthogonal analysis method(OAM)was DLA>DRHFB>SA>SH>DLF>HWLHFB>DSHFB>DABP>BPT.

关键词： Bedded rock slopes Hydro-fluctuation belt Shaking table test UDEC simulation Dynamic response mechanism

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In-situ synthesis of quantum dots in the nucleus of live cells

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National Science Review 2024年第3期11卷 172-182页

作者： Yusi Hu Zhi-Gang Wang Haohao fu Chuanzheng zhou Wensheng Cai Xueguang Shao Shu-Lin Liu Dai-Wen Pang State Key Laboratory of Medicinal Chemical Biology Frontiers Science Centre for New Organic MatterTianjin Key Laboratory of Biosensing and Molecular Recognition Research Centre for Analytical Sciences College of Chemistry School of Medicine and Frontiers Science Centre for Cell Responses Nankai University Haihe Laboratory of Sustainable Chemical Transformations

The cell nucleus is the main site for the storage and replication of genetic material, and the synthesis of substances in the nucleus is rhythmic, regular and strictly regulated by physiological processes. However,whether exogenous substances, such as nanoparticles, can be synthesized in situ in the nucleus of live cells has not been reported. Here, we have achieved in-situ synthesis of CdSxSe1-xquantum dots（QDs） in the nucleus by regulation of the glutathione（GSH） metabolic pathway. High enrichment of GSH in the nucleus can be accomplished by the addition of GSH with the help of the Bcl-2 protein. Then, high-valence Se is reduced to low-valence Se by glutathione-reductase-catalyzed GSH, and interacts with the Cd precursor formed through Cd and thiol-rich proteins, eventually generating QDs in the nucleus. Our work contributes to a new understanding of the syntheses of substances in the cell nucleus and will pave the way for the development of advanced ‘supercells’.

关键词： glutathione live cell nucleus quantum dot intracellular synthesis

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3D printing encouraging desired in-situ polypyrrole seed-polymerization for ultra-high energy density supercapacitors

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Journal of Energy Chemistry 2024年第8期95卷 117-125,I0004页

作者： Tiantian zhou Shangwen Ling Shuxian Sun Ruoxin Yuan Ziqin Wu Mengyuan fu Hanna He Xiaolong Li Chuhong Zhang State Key Laboratory of Polymer Materials Engineering Polymer Research InstituteSichuan UniversityChengdu 610065SichuanChina

The tireless pursuit of supercapacitors with high energy density entails the parallel advancement of wellsuited electrode materials and elaborately engineered ***(PPy)emerges as an exceedingly conductive polymer and a prospective pseudocapacitive materials for supercapacitors,yet the inferior cyclic stability and unpredictable polymerization patterns severely impede its real-world ***,for the first time,an innovative seed-induced in-situ polymerization assisted 3D printing strategy is proposed to fabricate PPy-reduced graphene oxide/poly(vinylidene difluoride-cohexafluoropropylene)(PVDF-HFP)(PPy-rGO/PH)electrodes with controllable polymerization behavior and exceptional areal mass *** preferred active sites uniformly pre-planted on the 3D-printed graphene substrates serve as reliable seeds to induce efficient polypyrrole deposition,achieving an impressive mass loading of 185.6 mg cm^(-2)(particularly 79.2 mg cm^(-2)for polypyrrole)and a superior areal capacitance of 25.2 F cm^(-2)at 2 mA cm^(-2)for a 12-layer *** agreement with theses appealing features,an unprecedented areal energy density of 1.47 mW h cm^(-2)for a symmetrical device is registered,a rarely achieved value for other PPy/rGO-based *** work highlights a promising route to preparing high energy density energy storage modules for real-world applications.

关键词： 3D printing Seed-induced polymerization Supercapacitor Polypyrrole High energy density

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Green manuring relocates microbiomes in driving the soil functionality of nitrogen cycling to obtain preferable grain yields in thirty years

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Science China(Life Sciences) 2024年第3期67卷 596-610页

作者： Guopeng zhou Kunkun Fan Songjuan Gao Danna Chang Guilong Li Ting liang Hai liang Shun Li Jiudong Zhang Zongxian Che Weidong Cao State Key Laboratory of Efficient Utilization of Arid and Semi-arid Arable Land in Northern China/Institute of Agricultural Resources and Regional Planning Chinese Academy of Agricultural SciencesBeijing 100081China State Key Laboratory of Soil and Sustainable Agriculture Institute of Soil ScienceChinese Academy of SciencesNanjing 210008China College of Resources and Environmental Sciences Nanjing Agricultural UniversityNanjing 210095China Institute of Soil&Fertilizer and Resource&Environment Jiangxi Academy of Agricultural SciencesNanchang 330200China Institute of Soil and Fertilizer and Water-saving Agriculture Gansu Academy of Agricultural SciencesLanzhou 730070China

Fertilizers are widely used to produce more food, inevitably altering the diversity and composition of soil organisms. The role of soil biodiversity in controlling multiple ecosystem services remains unclear, especially after decades of fertilization. Here, we assess the contribution of the soil functionalities of carbon(C), nitrogen(N), and phosphorus(P) cycling to crop production and explore how soil organisms control these functionalities in a 33-year field fertilization experiment. The long-term application of green manure or cow manure produced wheat yields equivalent to those obtained with chemical N, with the former providing higher soil functions and allowing the functionality of N cycling(especially soil N mineralization and biological N fixation) to control wheat production. The keystone phylotypes within the global network rather than the overall microbial community dominated the soil multifunctionality and functionality of C,N, and P cycling across the soil profile(0–100 cm). We further confirmed that these keystone phylotypes consisted of many metabolic pathways of nutrient cycling and essential microbes involved in organic C mineralization, N_(2)O release, and biological N fixation. The chemical N, green manure, and cow manure resulted in the highest abundances of amoB, nifH, and GH48 genes and Nitrosomonadaceae,Azospirillaceae, and Sphingomonadaceae within the keystone phylotypes, and these microbes were significantly and positively correlated with N_(2)O release, N fixation, and organic C mineralization, respectively. Moreover, our results demonstrated that organic fertilization increased the effects of the network size and keystone phylotypes on the subsoil functions by facilitating the migration of soil microorganisms across the soil profiles and green manure with the highest migration rates. This study highlights the importance of the functionality of N cycling in controlling crop production and keystone phylotypes in regulating soil functions, an

关键词： soil biodiversity soil multifunctionality element cycling keystone phylotypes

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Bimetallic NiCoP catalysts anchored on phosphorus-doped lignin-based carbon for robust oxygen evolution performance

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Rare Metals 2024年第7期43卷 3084-3095页

作者： Ling-Ying-Zi Xiong Bo-Wen Liu Lei Du Yue-Kuan zhou Xu-liang Lin Huan Wang Guangdong Engineering Technology Research Center for Sensing Materials & Devices Guangzhou Key Laboratory of Sensing Materials & DevicesSchool of Chemistry and Chemical EngineeringGuangzhou University School of Chemical Engineering and Light Industry Guangdong University of Technology Guangdong Provincial Laboratory of Chemistry and Fine Chemical Engineering Jieyang Center Sustainable Energy and Environment Thrust Function HubThe Hong Kong University of Science and Technology (Guangzhou) Division of Emerging Interdisciplinary Areas Department of Mechanical and Aerospace EngineeringThe Hong Kong University of Science and Technology State Key Lab of Pulp and Paper Engineering South China University of Technology

Oxygen evolution reaction（OER） catalysts are the key core materials that determine the performance of fuel cells,metal-air batteries,electrolytic water decomposition,and other *** this work,a green lignin-based non-precious metal OER catalyst was prepared by a simple ***,c arboxylated lignin was used to complex Ni and Co in situ,and then they were placed with sodium hypophosphite in the same tube furnace for upstream and downstream high-temperature calcination to construct a lignin carbon-based Ni-Co bimetallic OER catalyst（NiCoP@C）.The synthesized catalyst is a porous bimetallic phosphide with a three-dimensional network structure and high-density electrochemical active ***@C exhibited favorable catalytic activity for the oxygen evolution reaction（OER） with overpotential of 280 mV at 10 mA·cm-2and a Tafel slope of 77 mV·***,it exhibited remarkable durability during *** functional theory（DFT） calculations revealed that by leveraging the distinctive structure of transition metal phosphide nanoparticles incorporated into a reticulated substrate,the NiCoP@C catalyst offered an increased number of active sites for OER catalysis,significantly enhancing its stability during practical *** present study broadens the utilization pathways of biomass to "turn waste into treasure," aligning the development concept of green sustainable development.

关键词： Oxygen evolution reaction Lignin Carbon-based catalyst Nickel–cobalt bimetal Metal phosphide

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