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Toward a comprehensive hypothesis of oxygen-evolution reaction in the presence of iron and gold

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Journal of energy Chemistry 2024年第2期89卷 172-183,I0005页

作者： Negah Hashemi Jafar Hussain Shah Cejun Hu Subhajit Nandy Pavlo Aleshkevych Sumbal Farid Keun Hwa Chae Wei xie Taifeng Liu Junhu Wang Mohammad Mahdi Najafpour Department of Chemistry Institute for Advanced Studies in Basic Sciences(IASBS)Zanjan 45137-66731Iran center for Advanced Mössbauer Spectroscopy Mössbauer Effect Data CenterDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina Key Lab of Advanced energy Materials Chemistry(Ministry of Education) Renewable Energy Conversion and Storage CenterCollege of ChemistryNankai UniversityTianjin 300071China Advanced Analysis center Korea Institute of Science and TechnologySeoul 02792Republic of Korea Institute of Physics Polish Academy of SciencesWarsaw 02-668Poland National and Local joint Engineering research center for Applied Technology of Hybrid Nanomaterials Henan UniversityKaifeng 475004HenanChina center of Climate Change and Global Warming Institute for Advanced Studies in Basic Sciences(IASBS)Zanjan 45137-66731Iran research center for Basic sciences&Modern Technologies(RBST) Institute for Advanced Studies in Basic Sciences(IASBS)Zanjan 45137-66731Iran

This study investigates the effects of Fe on the oxygen-evolution reaction(OER)in the presence of Au.Two distinct areas of OER were identified:the first associated with Fe sites at low overpotential(~330 mV),and the second with Au sites at high overpotential(~870 mV).Various factors such as surface Fe concentration,electrochemical method,scan rate,potential range,concentration,method of adding K_(2)Fe O_(4),nature of Fe,and temperature were varied to observe diverse behaviors during OER for Fe O_(x)H_(y)/Au.Trace amounts of Fe ions had a significant impact on OER,reaching a saturation point where the activity did not increase further.Strong electronic interaction between Fe and Au ions was indicated by x-ray photoelectron spectroscopy(xPS)and electron paramagnetic resonance(EPR)analyses.In situ visible spectroscopy confirmed the formation of Fe O_(4)^(2-)during OER.In situ Mossbauer and surfaceenhanced Raman spectroscopy(SERS)analyses suggest the involvement of Fe-based species as intermediates during the rate-determining step of OER.A lattice OER mechanism based on Fe O_(x)H_(y)was proposed for operation at low overpotentials.Density functional theory(DFT)calculations revealed that Fe oxide,Fe-oxide clusters,and Fe doping on the Au foil exhibited different activities and stabilities during OER.The study provides insights into the interplay between Fe and Au in OER,advancing the understanding of OER mechanisms and offering implications for the design of efficient electrocatalytic systems.

关键词： DFT calculation Fe/Au electrocatalysis Mechanism Oxygen evolution Water oxidation

Insights into the kinetics–morphology relationship of 1-, 2-, and 3D TiNb_(2)O_(7) anodes for Li-ion storage

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Nano research 2024年第4期17卷 2770-2780页

作者： Wenlei xu Yaolin xu Veronika Grzimek Andrea Martin Thorsten Schultz Patrícia ARusso Yan Lu Norbert Koch Nicola Pinna Department of Chemistry IRIS Adlershof and the Center for the Science of Materials BerlinHumboldt-Universität zu BerlinBrook-Taylor-Str.212489 BerlinGermany Department of Electrochemical energy storage Helmholtz-Zentrum Berlin für Materialien und EnergieHahn-Meitner-Platz 114109 BerlinGermany Institut für Physik and IRIS Adlershof Humboldt-Universität zu BerlinBrook-Taylor-Str.212489 BerlinGermany joint research Group of Molecular Systems Helmholtz-Zentrum Berlin für Materialien und Energie12489 BerlinGermany

Understanding the influence of electrode material’s morphology on electrochemical behavior is of great significance for the development of rechargeable batteries,however,such studies are often limited by the inability to precisely control the morphology of electrode materials.Herein,nanostructured titanium niobium oxides(TiNb_(2)O_(7))with three different morphologies(one-dimensional(1D),two-dimensional(2D),and three-dimensional(3D))were synthesized via a facile microwave-assisted solvothermal method.The influence of the morphological dimension of TiNb_(2)O_(7) as electrode material on the electrochemical performance in Li-ion batteries(LIBs)and the underlying correlation with the electrochemical kinetics were studied in detail.2D TiNb_(2)O_(7)(TNO-2D)shows a superior rate capability and cycling stability,associated with improved kinetics for charge transfer and Li-ion diffusion,compared to the 1D and 3D materials.Operando x-ray diffraction measurements reveal the structural stability and crystallographic evolution of TNO-2D upon lithiation and delithiation and correlate the Li-ion diffusion kinetics with the lattice evolution during battery charge and discharge.Moreover,carbon-coated TNO-2D achieves enhanced rate capability(205 mAh·g^(-1) at 50 C)and long-term cycling stability(87%after 1000 cycles at 5 C).This work provides insights into the rational morphology design of electrode materials for accelerated charge transfer and enhanced fast-charging capability,pushing forward the development of electrode materials for high-power rechargeable batteries in future energy storage.

关键词： morphological dimension electrochemical kinetics lithium-ion batteries TiNb_(2)O_(7) structural evolution

Understanding fluorine-free electrolytes via small-angle x-ray scattering

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Journal of energy Chemistry 2022年第7期31卷 340-346,I0009页

作者： Kun Qian Zhou Yu Yuzi Liu David J.Gosztola Randall E.Winans Lei Cheng Tao Li Department of Chemistry and Biochemistry Northern Illinois UniversityDeKalbIL 60115USA Materials science division and joint center for energy storage research Argonne National LaboratoryLemontIL 60439USA center for Nanoscale Materials Argonne National LaboratoryLemontIL 60439USA x-ray science division and joint center for energy storage research Argonne National LaboratoryLemontIL 60439USA

Fluorine-free electrolytes have attracted great attention because of its low-cost and environmental friendliness. However, so far, little is known about the solution structures of these electrolytes. Here,we compare the solvation phenomenon of sodium tetraphenylborate(NaBPh_(4)) salt dissolved in organic solvents of propylene carbonate(PC), 1,2-dimethoxyethane(DME), acetonitrile(ACN) and tetrahydrofuran(THF). Small-angle x-ray scattering(SAxS) reveals a unique two-peak structural feature in this saltconcentrated PC electrolyte, while solutions using other solvents only have one scattering peak.Molecular dynamics(MD) simulations further reveal that there are anion-based clusters in addition to the short-range charge ordering in the concentrated NaBPh4/PC electrolyte. Raman spectroscopy confirms the existence of considerable contact ion pairs(CIPs). This work emphasizes the importance of global and local structural analysis, which will provide valuable clues for understanding the structureperformance relationship of electrolytes.

关键词： Fluorine-free electrolytes Sodium-ion batteries Small-angle x-ray scattering Solvation structures Sodium tetraphenylborate

Roadmap for rechargeable batteries:present and beyond

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science China Chemistry 2024年第1期67卷 13-42页

作者： Sen xin xu Zhang Lin Wang Haijun Yu xin Chang Yu-Ming Zhao Qinghai Meng Pan xu Chen-Zi Zhao Jiahang Chen Huichao Lu xirui Kong Jiulin Wang Kai Chen Gang Huang xinbo Zhang Yu Su Yao xiao Shu-Lei Chou Shilin Zhang Zaiping Guo Aobing Du Guanglei Cui Gaojing Yang Qing Zhao Liubing Dong Dong Zhou Feiyu Kang Hu Hong Chunyi Zhi Zhizhang Yuan xianfeng Li Yifei Mo Yizhou Zhu Dongfang Yu xincheng Lei Jianxiong Zhao Jiayi Wang Dong Su Yu-Guo Guo Qiang Zhang Jun Chen Li-Jun Wan CAS Key Laboratory of Molecular Nanostructure and Nanotechnology CAS Research/Education Center for Excellence in Molecular SciencesBeijing National Laboratory for Molecular Sciences(BNLMS)Institute of ChemistryChinese Academy of Sciences(CAS)Beijing 100190China University of Chinese Academy of sciences.Beijing 100049 China Institute of Advanced Battery Materials and Devices Faculty of Materials and ManufacturingBeijing University of TechnologyBeijing 100124China Key Laboratory of Advanced Functional Materials Ministry of EducationBeijing University of TechnologyBeijing 100124China Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology Department of Chemical EngineeringTsinghua UniversityBeijing 100084China State Key Laboratory of Chemistry and Utilization of Carbon-Based energy Resources College of ChemistryXinjiang UniversityUrumqi 830046China Department of Chemical Engineering Shanghai Jiao Tong UniversityShanghai 200240China State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChangchun 130022China Institute for Carbon Neutralization College of Chemistry and Materials EngineeringWenzhou UniversityWenzhou 325035China School of Chemical Engineering and Advanced Materials The University of AdelaideAdelaide 5000Australia Qingdao Industrial energy storage research Institute Qingdao Institute of Bioenergy and Bioprocess TechnologyChinese Academy of SciencesQingdao 266101China Frontiers science center for New Organic Matter Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education)College of ChemistryNankai UniversityTianjin 300071China College of Chemistry and Materials science Jinan UniversityGuangzhou 511443China Tsinghua Shenzhen International Graduate School Tsinghua UniversityShenzhen 518055China Department of Materials science and Engineering City University of Hong KongHong Kong 999077China division of energy storage Dalian National Laboratory for Clean Energy(DNL)Dalian Institute of Chem

Rechargeable batteries currently hold the largest share of the electrochemical energy storage market,and they play a major role in the sustainable energy transition and industrial decarbonization to respond to global climate change.Due to the increased popularity of consumer electronics and electric vehicles,lithium-ion batteries have quickly become the most successful rechargeable batteries in the past three decades,yet growing demands in diversified application scenarios call for new types of rechargeable batteries.Tremendous efforts are made to developing the next-generation post-Li-ion rechargeable batteries,which include,but are not limited to solid-state batteries,lithium–sulfur batteries,sodium-/potassium-ion batteries,organic batteries,magnesium-/zinc-ion batteries,aqueous batteries and flow batteries.Despite the great achievements,challenges persist in precise understandings about the electrochemical reaction and charge transfer process,and optimal design of key materials and interfaces in a battery.This roadmap tends to provide an overview about the current research progress,key challenges and future prospects of various types of rechargeable batteries.New computational methods for materials development,and characterization techniques will also be discussed as they play an important role in battery research.

关键词： energy storage rechargeable batteries battery materials electrochemistry

A Novel Layered Double Hydroxide and Dodecyl Alcohol Assisted PCM Composite with High Latent Heat storage Capacity and Thermal Conductivity

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Journal of Thermal science 2024年第2期33卷 537-547页

作者： AL-AHMED Amir SARI Ahmet KHAN Firoz AL-RASHEIDI Masoud Hekimoğlu Gökhan AFZAAL Mohammad A.ALSULAMI Ahmed DAFALLA Hatim SALHI Billel A.ALSULAIMAN Fahad Interdisciplinary research center for Renewable energy and Power Systems(IRC-REPS) King Fahd University of Petroleum&MineralsDhahran31261Saudi Arabia Department of Metallurgical and Material Engineering Karadeniz Technical UniversityTrabzon61080Turkey Maths and Natural sciences division Higher Colleges of TechnologyP.O.Box 7947SharjahUnited Arab Emirates Department of Mechanical Engineering King Fahd University of Petroleum&MineralsDhahran31261Saudi Arabia Core research Facilities King Fahd University of Petroleum&MineralsDhahran31261Saudi Arabia Interdisciplinary research center for Membranes and Water Security King Fahd University of Petroleum&MineralsDhahran31261Saudi Arabia

Dodecyl alcohol(DDA) is a promising solid-liquid phase change material(PCM) due to its favorable latent heat storage(LHS) characteristics.However,the leakage issue of PCM in a melted state during the heating period and low thermal conductivity restricts its utilization potential in thermal energy storage(TES) practices.Within the same context,the present work aims to overcome the leakage issue and improve the thermal conductivity of the DDA.With this in mind,a novel leak-proof layered double hydroxide(LDH)/DDA composite PCM is proposed through a solution-based impregnation method.The leak-proof impregnation ratio of the DDA impregnated within the cavities of the synthesized Al/Fe-LDH was determined to be 60%.Detailed morphological,physicochemical,and thermal properties of the fabricated composite were studied by scanning electron microscopy(SEM),Fourier transforms infrared(FTIR) spectroscopy,x-ray diffraction(xRD)spectroscopy,differential scanning calorimetry(DSC),thermalgravimetric analysis(TGA),and thermal cycling study.The results show that the LDH/DDA composite has a suitable phase change temperature(about 20℃) for passive solar thermal management of building envelopes.This composite PCM showed high LHS enthalpy(about136 J/g),good thermal stability,and cycling LHS reliability.It also showed nearly 152% higher thermal conductivity compared to that of pure DDA,ultimately reducing the melting and solidification time of the pure DDA by 44.9% and 45.5%,respectively.

关键词： dodecyl alcohol layered double hydroxide composite PCM thermal conductivity thermal energy storage(TES)

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

Association of daily sitting time and leisure-time physical activity with body fat among U.S.adults

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Journal of Sport and Health science 2024年第2期13卷 195-203页

作者： Jingwen Liao Min Hu Kellie Imm Clifton J.Holmes Jie Zhu Chao Cao Lin Yang Guangdong Provincial Key Laboratory of Physical Activity and Health Promotion Guangzhou Sport UniversityGuangzhou 510500China Scientific research center Guangzhou Sport UniversityGuangzhou 510500China division of Epidemiology&Genetics Department of Population and Public Health SciencesKeck School of Medicine of the University of Southern CaliforniaLos AngelesCA 90033USA Program in Physical Therapy Washington University School of MedicineSt.LouisMO 63110USA center for Human Nutrition Washington University School of MedicineSt.LouisMO 63110USA Department of Plastic and Reconstructive Surgery Shanghai East HospitalTongji UniversityShanghai 200070China Department of Cancer Epidemiology and Prevention research Alberta Health ServicesCalgary T2S 3C3Canada Department of Oncology and Community Health sciences University of CalgaryCalgary T2N 1N4Canada

Background:Prolonged sitting and reduced physical activity lead to low energy expenditures.However,little is known about the joint impact of daily sitting time and physical activity on body fat distribution.We investigated the independent and joint associations of daily sitting time and physical activity with body fat among adults.Methods:This was a cross-sectional analysis of U.S.nationally representative data from the National Health and Nutrition Examination Survey2011-2018 among adults aged 20 years or older.Daily sitting time and leisure-time physical activity(LTPA)were self-reported using the Global Physical Activity Questionnaire.Body fat(total and trunk fat percentage)was determined via dual x-ray absorptiometry.Results:Among 10,808 adults,about 54.6%spent 6 h/day or more sitting;more than one-half reported no LTPA(inactive)or less than 150 min/week LTPA(insufficiently active)with only 43.3%reported 150 min/week or more LTPA(active)in the past week.After fully adjusting for sociodemographic data,lifestyle behaviors,and chronic conditions,prolonged sitting time and low levels of LTPA were associated with higher total and trunk fat percentages in both sexes.When stratifying by LTPA,the association between daily sitting time and body fat appeared to be stronger in those who were inactive/insuufficiently active.In the joint analyses,inactive/insuufficiently active adults who reported sitting more than 8 h/day had the highest total(female:3.99%(95%confidence interval(95%CI):3.09%-4.88%);male:3.79%(95%CI:2.75%-4.82%))and trunk body fat percentages(female:4.21%(95%CI:3.09%-5.32%);male:4.07%(95%CI:2.95%-5.19%))when compared with those who were active and sitting less than 4 h/day.Conclusion:Prolonged daily sitting time was associated with increased body fat among U.S.adults.The higher body fat associated with 6 h/day sitting may not be offset by achieving recommended levels of physical activity.

关键词： Adults Body fat distribution Physical activity Sitting time

Microscopic Understanding of the Ionic Networks of“Water-in-Salt”Electrolytes

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energy Material Advances 2021年第1期2021卷 342-350页

作者： xinyi Liu Zhou Yu Erik Sarnello Kun Qian Soenke Seifert Randall E.Winans Lei Cheng Tao Li Department of Chemistry and Biochemistry Northern Illinois UniversityUSA Materials science division Argonne National LaboratoryUSA joint center for energy storage research Argonne National LaboratoryUSA x-ray science division Argonne National LaboratoryUSA

“Water-in-salt”electrolytes with excellent electrochemical and physical properties have been extensively investigated.However,the structural understanding of the lithium bis(trifluoromethane sulfonyl)imide(LiTFSI)in water is still lacking.Here,we perform synchrotron x-ray scattering to systemically study the structural variation of TFSI anions in an aqueous solution under a variety of concentrations and temperatures.There are two different solvation structures in the solution:TFSI-solvated structure and TFSI-network.As the concentration increases,the TFSI-solvated structure gradually disappears while the TFSI-network gradually forms.Even at relatively low concentrations,the TFSI-network can be observed.Our experimental results show that these two structures can coexist at a particular concentration,and temperature changes will lead to one structure’s formation or disappearance.Also,the TFSI-network is the key to obtain a stable electrochemical window under relatively high temperatures.

关键词： structure lithium methane

MOF-Transformed In_(2)O_(3-x)@C Nanocorn Electrocatalyst for Efficient CO_(2)Reduction to HCOOH

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Nano-Micro Letters 2022年第10期14卷 219-234页

作者： Chen Qiu Kun Qian Jun Yu Mingzi Sun Shoufu Cao Jinqiang Gao Rongxing Yu Lingzhe Fang Youwei Yao xiaoqing Lu Tao Li Bolong Huang Shihe Yang Guangdong Key Lab of Nano-Micro Material research School of Chemical Biology and BiotechnologyPeking University Shenzhen Graduate SchoolShenzhen 518055People’s Republic of China Department of Chemistry and Biochemistry Northern Illinois UniversityDeKalbIL 60115USA Department of Applied Biology and Chemical Technology The Hong Kong Polytechnic UniversityHung HomKowloonHong Kong SARPeople’s Republic of China School of Materials science and Engineering China University of PetroleumQingdaoShandong 266580People’s Republic of China Shenzhen International Graduate School Tsinghua UniversityShenzhenPeople’s Republic of China x-ray science division and joint center for energy storage research Argonne National LaboratoryLemontIL 60439USA Institute of Biomedical Engineering Shenzhen Bay LaboratoryShenzhen 518107People’s Republic of China

For electrochemical CO_(2) reduction to HCOOH,an ongoing challenge is to design energy efficient electrocatalysts that can deliver a high HCOOH current density(JHCOOH)at a low overpotential.Indium oxide is good HCOOH production catalyst but with low con-ductivity.In this work,we report a unique corn design of In_(2)O_(3-x)@C nanocatalyst,wherein In_(2)O_(3-x)nanocube as the fine grains dispersed uniformly on the carbon nanorod cob,resulting in the enhanced conductivity.Excellent performance is achieved with 84%Faradaic efficiency(FE)and 11 mA cm^(−2)JHCOOH at a low potential of−0.4 V versus RHE.At the current density of 100 mA cm^(−2),the applied potential remained stable for more than 120 h with the FE above 90%.Density functional theory calculations reveal that the abundant oxygen vacancy in In_(2)O_(3-x) has exposed more In^(3+) sites with activated electroactivity,which facilitates the formation of HCOO*intermediate.Operando x-ray absorp-tion spectroscopy also confirms In^(3+) as the active site and the key intermediate of HCOO*during the process of CO_(2) reduction to HCOOH.

关键词： CO_(2)reduction Indium oxide Formate Corn design Active sites