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Multiscale simulations of surface adsorption characteristics of amino acids on zinc metal anode

Journal of energy Chemistry 2023年第12期87卷 153-161,I0006页

作者： Yufan Xia Zijian Hong Linming Zhou Shuang Chen Zhen Luo Shoutong Jin Yuhui Huang Yinzhu Jiang Yongjun Wu School of materials Science and Engineering Zhejiang UniversityHangzhou 310027ZhejiangChina ZJU-Hangzhou Global Scientific and Technological Innovation center Zhejiang UniversityHangzhou 311215ZhejiangChina state key laboratory of Silicon and Advanced Semiconductor materials Zhejiang UniversityHangzhou 310027ZhejiangChina research Institute of Zhejiang University-Taizhou Zhejiang UniversityTaizhou 318000ZhejiangChina

Aqueous zinc-ion batteries(ZIBs) are considered promising power sources for grid storage,but they face several issues,including dendrite growth,corrosion,hydrogen evolution,etc.,which are related to the Zn metal/liquid electrolyte interface.To address these challenges,many researchers have focused on modifying the Zn anode with surface adsorption.However,the underlying mechanism between the Zn surface and adsorbed/protective molecules has not been thoroughly explored.In this study,we built a multiscale simulation platform that integrates state-of-art simulation methods to comprehensively investigate the adsorption process of amino acids on the Zn metal surface.Our major finding is that adsorption sites,adsorbate–surface angle,and average distance are critical parameters for the stability and strength of surface adsorption.Additionally,ab initio molecular dynamics reveal the kinetics of the surface adsorption and molecule reorientation processes.Specifically,it can be discovered that the amino acids prefer to align parallel to the Zn metal surface,leading to better surface protection against corrosion and preventing dendrite growth.These findings pave the way for an in-depth understanding of the surface adsorption process,as well as providing concrete design principles for stable Zn metal anodes.

关键词： Zn-ion battery First-principles calculations Surface adsorption Ab initio molecular dynamics

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Ordering in liquid and its heredity impact on phase transformation of Mg-Al-Ca alloys

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镁合金学报(英文) 2023年第6期11卷 2006-2017页

作者： Jiang You Cheng Wang Shun-Li Shang Yipeng Gao Hong Ju Hong Ning Yi Wang Hui-Yuan Wang Zi-Kui Liu state key laboratory of Automotive Simulation and Control&School of materials Science and Engineering Jilin UniversityNanling Campus No.5988 enmin StreetChangchun 130025China International center of Future Science Jilin UniversityChangchun 130012China Department of materials Science and Engineering The Pennsylvania State UniversityUniversity ParkPA 16802United States of America

It is a long-sought goal to achieve desired mechanical properties through tailoring phase formation in alloys,especially for complicated multi-phase alloys.In fact,unveiling nucleation of competitive crystalline phases during solidification hinges on the nature of liquid.Here we employ ab initio molecular dynamics simulations(AIMD)to reveal liquid configuration of the Mg-Al-Ca alloys and explore its effect on the transformation of Ca-containing Laves phase from Al2Ca to Mg_(2)Ca with increasing Ca/Al ratio(rCa/Al).There is structural similarity between liquid and crystalline phase in terms of the local arrangement environment,and the connection schemes of polyhedras.The forming signature of Mg_(2)Ca,as hinted by the topological and chemical short-range order originating from liquid,ascends monotonically with increasing rCa/Al.However,Al_(2)Ca crystal-like order increase at first and then decrease at the crossover of rCa/Al=0.74,corresponding to experimental composition of phase transition from Al_(2)Ca to Mg_(2)Ca.The origin of phase transformation across different compositions lies in the dense packing of atomic configurations and preferential bonding of chemical species in both liquid and solid.The present finding provides a feasible scenario for manipulating phase formation to achieve high performance alloys by tailoring the crystal-like order in liquid.

关键词： Liquid alloy Solidification Crystalembryo Short-rangeorder Ab initio molecular dynamics

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Compositional engineering of HKUST-1/sulfidized NiMn-LDH on functionalized MWCNTs as remarkable bifunctional electrocatalysts for water splitting

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Carbon energy 2023年第12期5卷 1-20页

作者： Mengshan Chen Reza Abazari Soheila Sanati Jing Chen Mingyuzhi Sun Cunhong Bai Alexander M.Kirillov Yingtang Zhou Guangzhi Hu Zhejiang key laboratory of Petrochemical environmental Pollution Control National Engineering Research Center for Marine AquacultureMarine Science and Technology CollegeZhejiang Ocean UniversityZhoushanChina Department of Chemistry Faculty of ScienceUniversity of MaraghehMaraghehIran state key laboratory of High-Efficiency Utilization of Coal and Green Chemical Engineering College of Chemistry and Chemical EngineeringNingxia UniversityYinchuanChina Departamento de Engenharia Química Centro de Química EstruturalInstitue of Molecular SciencesInstituto Superior TécnicoUniversidade de LisboaLisbonPortugal School of Ecology and environmental Science Institute for Ecological Research and Pollution Control of Plateau LakesYunnan UniversityKunmingChina

Water-splitting reactions such as the hydrogen evolution reaction(HER)and the oxygen evolution reaction(OER)typically require expensive noble metal-based electrocatalysts.This has motivated researchers to develop novel,cost-effective electrocatalytic systems.In this study,a new multicomponent nanocomposite was assembled by combining functionalized multiwalled carbon nanotubes,a Cu-based metal–organic framework(MOF)(HKUST-1 or HK),and a sulfidized NiMn-layered double hydroxide(NiMn-S).The resulting nanocomposite,abbreviated as MW/HK/NiMn-S,features a unique architecture,high porosity,numerous electroactive Cu/Ni/Mn sites,fast charge transfer,excellent structural stability,and conductivity.At a current density of 10 mA cm-2,this dual-function electrocatalyst shows remarkable performance,with ultralow overpotential values of 163 mV(OER)or 73 mV(HER),as well as low Tafel slopes(57 and 75 mV dec-1,respectively).Additionally,its high turnover frequency values(4.43 s-1 for OER;3.96 s-1 for HER)are significantly superior to those of standard noble metal-based Pt/C and IrO2 systems.The synergistic effect of the nanocomposite's different components is responsible for its enhanced electrocatalytic performance.A density functional theory study revealed that the multi-interface and multicomponent heterostructure contribute to increased electrical conductivity and decreased energy barrier,resulting in superior electrocatalytic HER/OER activity.This study presents a novel vision for designing advanced electrocatalysts with superior performance in water splitting.Various composites have been utilized in water-splitting applications.This study investigates the use of the MW/HK/NiMn-S electrocatalyst for water splitting for the first time to indicate the synergistic effect between carbon-based materials along with layered double hydroxide compounds and porous compounds of MOF.The unique features of each component in this composite can be an interesting topic in the field of water splitting.

关键词： bifunctional electrocatalyst electroactive sites multicomponent synergic effect water splitting

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Recyclable Fenton-like catalyst based on zeolite Y supported ultrafine,highly-dispersed Fe_2O_3 nanoparticles for removal of organics under mild conditions

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中国化学快报：英文版 2019年第2期30卷 324-330页

作者： Xuanyu Yang Xiaowei Cheng Ahmed A.Elzatahry Jinyang Chen Abdulaziz Alghamdi Yonghui Deng Department of Chemistry State Key Laboratory of Molecular Engineering of Polymers Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials iChEM (Collaborative Innovation Center of Chemistry for Energy Materials) Fudan University materials Science and Technology Program College of Arts and Sciences Qatar University School of environmental and Chemical Engineering Shanghai University Department of Chemistry College of Science King Saud University state key Lab of Transducer Technology Shanghai Institute of Microsystem and Information Technology Chinese Academy of Sciences

A versatile wet impregnation method was employed to conveniently and controllably deposit Fe_2O_3 nanoparticles on zeolites including commercial Y, mordenite and ZSM-5 with the similar framework Si/Al ratios and crystal sizes, respectively. The ultrafine Fe_2O_3 nanoparticles in size of 5 nm can be highly dispersed on zeolite Y matrix due to its much better wettability than ZSM-5 and mordenite. By using the obtained Fe_2O_3/zeolite composite as the heterogeneous Fenton-like catalysts, the degradation of phenol as a model reaction was systematically investigated, including the zeolite supports, particle size and dispersion of Fe_2O_3, and reaction conditions of H_2O_2 concentration, temperature, and pH value. The catalyst based on zeolite Y with Fe loading of 9% exhibited the best phenol degradation efficiency (> 90%)in neutral pH within 2 h. Its high catalytic activity in Fenton reaction can be attributed to the bifunctional properties of strong surface BrФnsted acidity and high reactivity of octahedral Fe^(3+) in the highlydispersed ultrafine Fe_2O_3 nanoparticles in size of 5 nm, which were the primary active centers to quickly decompose H_2O_2 into hydroxyl radicals. Since phenol degradation can be performed under mild conditions of ambient temperature (283-323 K) and a wide pH range (4.0-7.0), the catalysts can be easily recovered for recyclable use with stable degradation activity, which own the immense potential in deep treatment of organic pollutants in industrial wastewater.

关键词： Fenton-like reaction Zeolite Fe2O3 nanoparticles Highly-dispersed Phenol degradation

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Nonequilibrium molecular dynamics for accelerated computation of ion–ion correlated conductivity beyond Nernst–Einstein limitation

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npj Computational materials 2023年第1期9卷 1796-1803页

作者： Ryoma Sasaki Bo Gao Taro Hitosugi Yoshitaka Tateyama School of materials and Chemical Technology Tokyo Institute of Technology2-12-1 OokayamaMeguroTokyo 152-8552Japan center for Green research on energy and environmental materials National Institute for Material Science1-1 NamikiTsukubaIbaraki 305-0044Japan Department of Chemistry The University of Tokyo7-3-1 HongoBunkyoTokyo 113-0033Japan

Condensed matters with high ionic conductivities are crucial in various solid devices such as solid-state batteries. The conduction ischaracterized by the cooperative ionic motion associated with the high carrier density. However, the high cost of computingcorrelated ionic conductivities has forced almost all ab initio molecular dynamics (MD) to rely on the Nernst–Einstein dilute-solutionapproximation, which ignores the cross-correlation effect. Here we develop a chemical color-diffusion nonequilibrium MD (CCD-NEMD) method, which enables to calculate the correlated conductivities with fewer sampling steps than the conventional MD. ThisCCD-NEMD is demonstrated to well evaluate the conductivities in the representative solid electrolyte bulk Li10GeP2S12 andLi_(7)La_(3)Zr_(2)O_(12). We also applied CCD-NEMD to the grain boundary of Li_(7)La_(3)Zr_(2)O_(12) and demonstrated its applicability for calculatinginterfacial local conductivities, which is essential for investigating grain boundaries and composite electrolytes. CCD-NEMD canprovide further accurate understanding of ionics with ionic correlations and promote developing solid devices.

关键词： dynamics Nernst steps

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Multiple evaluations of atmospheric behavior between Criegee intermediates and HCHO: Gas-phase and air-water interface reaction

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Journal of environmental Sciences 2023年第5期127卷 308-319页

作者： Tianlei Zhang Mingjie Wen Chao Ding Yongqi Zhang Xiaohui Ma Zhuqing Wang Makroni Lily Junhai Liu Rui Wang Institute of Theoretical and Computational Chemistry Shaanxi Key Laboratory of CatalysisSchool of Chemical&Environment ScienceShaanxi University of TechnologyHanzhong 723001China School of environmental Science and Engineering Institute of Environmental Health and Pollution ControlGuangdong University of TechnologyGuangzhou 510006China Shandong key laboratory of Biophysics Institute of BiophysicsDezhou UniversityDezhou 253023China environmental research Institute Shandong UniversityQingdao 266237China Qinba Mountains of Bio-Resource Collaborative Innovation center of Southern Shaanxi Province Shaanxi University of TechnologyHanzhong 723001China

Given the high abundance of water in the atmosphere,the reaction of Criegee intermediates(CIs)with(H_(2)O)_(2) is considered to be the predominant removal pathway for CIs.However,recent experimental findings reported that the reactions of CIs with organic acids and carbonyls are faster than expected.At the same time,the interface behavior between CIs and carbonyls has not been reported so far.Here,the gas-phase and air-water interface behavior between Criegee intermediates and HCHO were explored by adopting high-level quantum chemical calculations and Born-Oppenheimer molecular dynamics(BOMD)simulations.Quantum chemical calculations evidence that the gas-phase reactions of CIs+HCHO are submerged energy or low energy barriers processes.The rate ratios speculate that the HCHO could be not only a significant tropospheric scavenger of CIs,but also an inhibitor in the oxidizing ability of CIs on SO_(x) in dry and highly polluted areas with abundant HCHO concentration.The reactions of CH_(2)OO with HCHO at the droplet’s surface follow a loop structure mechanism to produce i)SOZ(■),ii)BHMP(HOCH_(2)OOCH_(2)OH),and iii)HMHP(HOCH_(2)OOH).Considering the harsh reaction conditions between CIs and HCHO at the interface(i.e.,the two molecules must be sufficiently close to each other),the hydration of CIs is still their main atmospheric loss pathway.These results could help us get a better interpretation of the underlying CIs-aldehydes chemical processes in the global polluted urban atmospheres.

关键词： Criegee intermediates HCHO Atmospheric behavior Air-water interface Chemical processes

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Solvation Structure and dynamics of Mg(TFSI)_(2) Aqueous Electrolyte

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energy & environmental materials 2022年第1期5卷 295-304页

作者： Zhou Yu Taylor R.Juran Xinyi Liu Kee Sung Han Hui Wang Karl T.Mueller Lin Ma Kang Xu Tao Li Larry A.Curtiss Lei Cheng materials Science Division Argonne National LaboratoryLemont IL 60439USA Joint center for energy Storage research(JCESR) Lemont IL 60439USA Department of Physics Binghamton UniversityState University of New York4400 Vestal Parkway EastBinghamton NY 13902USA Department of Chemistry and Biochemistry Northern Illinois UniversityDeKalb IL 60115USA Physical and Computational Sciences Directorate Pacific Northwest National LaboratoryRichland WA 99352USA energy&Environment Directorate Pacific Northwest National LaboratoryRichland WA 99352USA energy Storage Branch Energy and Biotechnology DivisionSensor and Electronics DirectorateU.S.Army Research LaboratoryAdelphi MD 20783USA Department of Chemistry and Biochemistry Northern Illinois University DeKalb IL 60115 USA X-ray Science Division Argonne National laboratory Lemont IL 60439 USA

Using ab initio molecular dynamics(AIMD)simulations,classical molecular dynamics(CMD)simulations,small-angle X-ray scattering(SAXS),and pulsed-field gradient nuclear magnetic resonance(PFG-NMR),the solvation structure and ion dynamics of magnesium bis(trifluoromethanesulfonyl)imide(Mg(TFSI)_(2))aqueous electrolyte at 1,2,and 3 m concentrations are investigated.From AIMD and CMD simulations,the first solvation shell of an Mg;ion is found to be composed of six water molecules in an octahedral configuration and the solvation shell is rather rigid.The TFSI^(-)ions prefer to stay in the second solvation shell and beyond.Meanwhile,the comparable diffusion coefficients of positive and negative ions in Mg(TFSI)_(2)aqueous electrolytes have been observed,which is mainly due to the formation of the stable[Mg(H_(2)O_(6))_(2)]^(+)complex,and,as a result,the increased effective Mg ion size.Finally,the calculated correlated transference numbers are lower than the uncorrelated ones even at the low concentration of 2 and 3 m,suggesting the enhanced correlations between ions in the multivalent electrolytes.This work provides a molecular-level understanding of how the solvation structure and multivalency of the ion affect the dynamics and transport properties of the multivalent electrolyte,providing insight for rational designs of electrolytes for improved ion transport properties.

关键词： Mg(TFSI)_(2)aqueous electrolyte molecular dynamics simulation pulsed-field gradient nuclear magnetic resonance small-angle X-ray scattering ion dynamics

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Extraordinary Compatibility to Mass Loading and Rate Capability of Hierarchically Porous Carbon Nanorods Electrode Derived from the Waste Tire Pyrolysis Oil

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energy & environmental materials 2022年第4期5卷 1238-1250页

作者： Shengping Li Zipan Yang Mingzhen Wu Chenggen Xu Xilu Zhang Rundan Lin Xuejie Wang Lu Zhao Dong Sun Xinlong Ma Jinsen Gao state key laboratory of Heavy Oil Processing China University of PetroleumChangpingBeijing 102249China

The conversion of waste tire pyrolysis oil(WTPO)into S-doped porous carbon nanorods(labeled as WPCNs)with hierarchical pore structure is realized by a simple template-directed approach.The specific surface area of as-obtained porous carbon nanorods can reach up to 1448 m^(2) g^(−1) without the addition of any activating agent.As the capacitive electrode,WPCNs possess the extraordinary compatibility to capacitance,different electrolyte systems as well as long-term cycle life even at a commercial-level areal mass loading(10 mg cm^(−2)).Besides,only an extremely small capacitance fluctuation is observed under the extreme circumstance(−40 to 80℃),reflecting the excellent high-and low-temperature performance.The relationship between the pore structure and capacitive behavior is analyzed by comparing WPCNs with mesopores-dominated asphalt-derived porous carbon nanorods(APCNs)and micropores-dominated activated carbon.The molecular dynamics simulation further reveals the ion diffusion and transfer ability of the as-prepared carbon materials under different pore size distribution.The total ion flow(NT)of WPCNs calculated by the simulation is obviously larger than APCNs and the N_(T) ratio between them is similar with the experimental average capacitance ratio.Furthermore,this work also provides a valuable strategy to prepare the electrode material with high capacitive energy storage ability through the high value-added utilization of WTPO.

关键词： compatibility high-and low-temperature performance high areal mass loading porous carbon nanorods waste tire pyrolysis oil

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Macroscopic assembled graphene nanofilms based room temperature ultrafast mid-infrared photodetectors

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InfoMat 2022年第6期4卷 129-140页

作者： Li Peng Lixiang Liu Sichao Du Srikrishna Chanakya Bodepudi Lingfei Li Wei Liu Runchen Lai Xiaoxue Cao Wenzhang Fang Yingjun Liu Xinyu Liu Jianhang Lv Muhammad Abid Junxue Liu Shengye Jin Kaifeng Wu Miao-Ling Lin Xin Cong Ping-Heng Tan Haiming Zhu Qihua Xiong Xiaomu Wang Weida Hu Xiangfeng Duan Bin Yu Zhen Xu Yang Xu Chao Gao MOE key laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and EngineeringInternational Research Center for X PolymersZhejiang UniversityHangzhouChina School of Micro-nanoelectronics State Key Laboratory of Silicon MaterialsHangzhou Global Scientific and Technological Innovation CenterZJU-UIUC Joint InstituteZhejiang UniversityHangzhouChina state key laboratory of molecular reaction dynamics and dynamics Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalianChina state key laboratory of Superlattices and Microstructures Institute of SemiconductorsChinese Academy of SciencesBeijingChina Department of Chemistry Zhejiang UniversityHangzhouChina Division of Physics and Applied Physics School of Physical and Mathematical SciencesNanyang Technological UniversitySingaporeSingapore National laboratory of Solid state Microstructures Collaborative Innovation Center of Advanced MicrostructureSchool of Electronic Science and EngineeringNanjing UniversityNanjingChina state key laboratory of Infrared Physics Shanghai Institute of Technical PhysicsChinese Academy of SciencesShanghaiChina Department of Chemistry and Biochemistry California Nanosystems InstituteUniversity of CaliforniaLos AngelesCaliforniaUSA

Graphene with linear energy dispersion and weak electron-phonon interaction is highly anticipated to harvest hot electrons in a broad wavelength range.However,the limited absorption and serious backscattering of hot-electrons result in inadequate quantum yields,especially in the mid-infrared range.Here,we report a macroscopic assembled graphene(nMAG)nanofilm/silicon heterojunction for ultrafast mid-infrared photodetection.The assembled Schottky diode works in 1.5-4.0μm at room temperature with fast response(20-30 ns,rising time,4 mm2 window)and high detectivity(1.61011 to 1.9109 Jones from 1.5 to 4.0μm)under the pulsed laser,outperforming single-layer-graphene/silicon photodetectors by 2-8 orders.These performances are attributed to the greatly enhanced photo-thermionic effect of electrons in nMAG due to its high light absorption(~40%),long carrier relaxation time(~20 ps),low work function(4.52 eV),and suppressed carrier number fluctuation.The nMAG provides a long-range platform to understand the hot-carrier dynamics in bulk 2D materials,leading to broadband and ultrafast MIR active imaging devices at room temperature.

关键词： graphene nanofilm heterojunction macro-assembly mid-infrared photodetector photothermionic effect

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Photocatalysis:an overview of recent developments and technological advancements

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Science China Chemistry 2020年第2期63卷 149-181页

作者： Yuanxing Fang Yun Zheng Taofang Yong Chen Yaodong Zhu Qing Liang Hua Sheng Zhaosheng Li Chuncheng Chen Xinchen Wang state key laboratory of Photocatalysis on energy and Environment College of ChemistryFuzhou UniversityFuzhou 350116China key laboratory of molecular Designing and Green Conversions Fujian Province UniversityCollege of Materials Science and EngineeringHuaqiao UniversityXiamen 361021China Collaborative Innovation center of Advanced Microstructures National Laboratory of Solid State MicrostructuresCollege of Engineering and Applied SciencesNanjing UniversityNanjing 210093China key laboratory of Photochemistry CAS Research/Education Center for Excellence in Molecular SciencesInstitute of ChemistryChinese Academy of SciencesBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China

Photocatalysis,which is the catalyzation of redox reactions via the use of energy obtained from light sources,is a topic that has garnered a lot of attention in recent years as a means of addressing the environmental and economic issues plaguing society today.Of particular interest are photosynthesis can potentially mimic a variety of vital reactions,many of which hold the key to develop sustainable energy economy.In light of this,many of the technological and procedural advancements that have recently occurred in the field are discussed in this review,namely those linked to:(1)photocatalysts made from metal oxides,nitride,and sulfides;(2)photocatalysis via polymeric carbon nitride(PCN);and(3)general advances and mechanistic insights related to TiO2-based catalysts.The challenges and opportunities that have arisen over the past few years are discussed in detail.Basic concepts and experimental procedures which could be useful for eventually overcoming the problems associated with photocatalysis are presented herein.

关键词： photocatalysis carbon nitride metal oxides metal nitride metal sulfide mechanism TiO2

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