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Nano Research 2023年第5期16卷 8012-8017页

作者： Xinran Li Yipei Li Changli Wang Huaiguo Xue Huan Pang Qiang Xu School of Chemistry and Chemical Engineering Yangzhou UniversityYangzhou 225009China Shenzhen Key Laboratory of Micro/Nano-Porous Functional Materials(SKLPM) SUSTech-Kyoto University Advanced Energy Materials Joint Innovation Laboratory(SKAEM-JIL)Key University Laboratory of Highly Efficient Utilization of Solar Energy and Sustainable Development of GuangdongDepartment of ChemistryDepartment of Materials Science and Engineering and SUSTech Academy for Advanced Interdisciplinary StudiesSouthern University of Science and Technology(SUSTech)Shenzhen 518055China

Cu-based materials are seldom reported as oxygen evolution reaction(OER)electrocatalysts due to their inherent electron orbital configuration,which makes them difficult to adsorb oxygen-intermediates during OER.Reasonably engineering the hierarchical architectures and the electronic structures can improve the performance of Cu-based OER catalysts,such as constructing multilevel morphology,inducing the porous materials,improving the Cu valence,building heterostructures,doping heteroatoms,etc.In this work,copper-1,3,5-benzenetricarboxylate(HKUST-1)octahedra in-situ grow on the Cu nanorod(NR)-supported N-doped carbon microplates,meanwhile an active layer of Cu(OH)_(2)forms on the surface of the original conductive Cu NRs.The octahedral HKUST-1,serving as a spacer between the microplates,greatly improves the porosity and increases the available active sites,facilitating the mass transport and electron transfer,thus resulting in greatly enhanced OER performance.

关键词： core–shell nanorod Cu@Cu(OH)_(2) metal–organic framework oxygen evolution reaction

Acid-stable antimonate based catalysts for the electrocatalytic oxygen evolution reaction

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Nano Research 2023年第4期16卷 4691-4697页

作者： Xiaoping Gao Huang Zhou Zhe Wang Gang Zhou Jin Wang Yuen Wu College of Materials Science and Engineering Shenzhen UniversityShenzhen 518071China School of Chemistry and Materials Science University of Science and Technology of ChinaHefei 230026China Preservation Technology Advanced Research CenterHefei Hualing Co.LtdHefei 230000China School of Science Hubei University of TechnologyWuhan 430068China

Acid-stable and highly active catalysts for the electrocatalytic oxygen evolution reaction(OER)are paramount to the advancement of electrochemical technologies for clean energy conversion and utilization.In this work,based on the density functional theory(DFT)calculations,we systematically investigated the MSb_(2)O_(6)(M=Fe,Co,and Ni)and transition metal(TM)doped MSb_(2)O_(6)(TM-MSb_(2)O_(6),TM=Mn,Fe,Co,Ni,Cu,Zn,Ru,Rh,Pd,Ir,and Pt)as potential antimonate-based electrocatalysts for the OER.The stability and OER activity of these considered electrocatalysts were systematically studied under acidic conditions.It was found that Rh-NiSb_(2)O_(6),Pt-CoSb_(2)O_(6),Rh-FeSbO4,and Co-NiSb_(2)O_(6)can serve as efficient and stable OER electrocatalysts,and their OER catalytic activities are better than that of the current state-of-the-art OER catalyst(IrO2).Our findings highlight a family of promising antimonate-based OER electrocatalysts for future experimental verification.

关键词： oxygen evolution reaction antimonates acid-stable oxides electrocatalysis density functional theory

Interfacial engineering of transition-metal sulfides heterostructures with built-in electric-field effects for enhanced oxygen evolution reaction

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Chinese Journal of Chemical Engineering 2022年第1期35卷 320-328页

作者： Shan Ni Hongnan Qu Huifang Xing Zihao Xu Xiangyang Zhu Menglei Yuan Meng Rong Li Wang Jiemiao Yu Yanqing Li Liangrong Yang Huizhou Liu CAS Key Laboratory of Green Process and Engineering State Key Laboratory of Biochemical EngineeringInstitute of Process EngineeringChinese Academy of SciencesBeijing 100190China School of Chemical Engineering University of Chinese Academy of SciencesBeijing 100049China Qingdao Institute of Bioenergy and Bioprocess Technology Chinese Academy of SciencesQingdao 266061China

Developing highly efficient,durable,and non-noble electrocatalysts for the sluggish anodic oxygen evolution reaction(OER)is the pivotal for meeting the practical demand in water splitting.However,the current transition-metal electrocatalysts still suffer from low activity and durability on account of poor interfacial reaction kinetics.In this work,a facile solid-state synthesis strategy is developed to construct transition-metal sulfides heterostructures(denoted as MS_(2)/NiS_(2),M=Mo or W)for boosting OER electrocatalysis.As a result,MoS2/NiS2 and WS2/NiS2 show lower overpotentials of 300 mV and 320 mV to achieve the current density of 10 mA·cm^(-2),and smaller Tafel slopes of 60 mV.dec^(-1) and 83 mV.dec^(-1)in 1 mol·L^(-1) KOH,respectively,in comparison with the single MoS2,WS2,NiS2,as well as even the benchmark RuO2.The experiments reveal that the designed heterostructures have strong electronic interactions and spontaneously develop a built-in electric field at the heterointerface with uneven charge distribution based on the difference of band structures,which promote interfacial charge transfer,improve absorptivity of OH-,and modulate the energy level more comparable to the OER.Thus,the designed transition-metal sulfides heterostructures exhibit a remarkably high electrocatalytic activity for OER.This study provides a simple strategy to manipulate the heterostructure interface via an energy level engineering method for OER and can be extended to fabricate other heterostructures for various energy-related applications.

关键词： oxygen evolution reaction Transition-metal sulfides heterostructures Heterointerface Built-in electric field

Interface construction of NiCo LDH/NiCoS based on the 2D ultrathin nanosheet towards oxygen evolution reaction

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Nano Research 2022年第6期15卷 4986-4995页

作者： Jiahui Li Lili Wang Haojia He Yiquan Chen Zirui Gao Na Ma Bing Wang Linlin Zheng Rulin Li Yujia Wei Junqing Xu Yao Xu Bowen Cheng Zhen Yin Ding Ma State Key Laboratory of Separation Membranes and Membrane Processes School of ChemistryTiangong UniversityTianjin 300387China School of Chemical Engineering and Technology Tiangong UniversityTianjin 300387China Beijing National Laboratory for Molecular Sciences College of Chemistry and Molecular Engineering and College of Engineeringand BIC-ESATPeking UniversityBeijing 100871China College of Chemical Engineering and Materials Science Tianjin University of Science and TechnologyTianjin 300457China China Tianchen Engineering Corporation Tianjin 300400China

Carbon-free hydrogen as a promising clean energy source can be produced with electrocatalysts via water electrolysis.oxygen evolution reaction(OER)as anodic reaction determines the overall efficiency of water electrolysis due to sluggish OER kinetics.Thus,it’s much desirable to explore the efficient and earth-abundant transition-metal-based OER electrocatalysts with high current density and superior stability for industrial alkaline electrolyzers.Herein,we demonstrate a significant enhancement of OER kinetics with the hybrid electrocatalyst arrays in alkaline via judiciously combining earth-abundant and ultrathin NiCo-based layered double hydroxide(NiCo LDH)nanosheets with nickel cobalt sulfides(NiCoS)with a facile metal-organic framework(MOF)-template-involved surface sulfidation process.The obtained NiCo LDH/NiCoS hybrid arrays exhibits an extremely low OER overpotential of 308 mV at 100 mA·cm^(−2),378 mV at 200 mA·cm^(−2)and 472 mV at 400 mA·cm^(−2)in 1 M KOH solution,respectively.A much low Tafel slope of 48 mV·dec^(−1)can be achieved.Meanwhile,with the current density from 50 to 250 mA·cm^(−2),the NiCo-LDH/NiCoS hybrid arrays can run for 25 h without any degradation.Our results demonstrate that the construction of hybrid arrays with abundant interfaces of NiCo LDH/NiCoS can facilitate OER kinetics via possible modulation of binding energy of O-containing intermediates in alkaline media.The present work would pave the way for the development of lowcost and efficient OER catalysts and industrial application of water alkaline electrolyzers.

关键词： oxygen evolution reaction hybrid structure ultrathin nanosheet layered double hydroxide surface sulfidation interface of NiCo LDH/NiCoS

The surface of metal boride tinted by oxygen evolution reaction for enhanced water electrolysis

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Journal of Energy Chemistry 2022年第9期31卷 509-515,I0014页

作者： Xu Zou Wei Zhang Xinyan Zhou Kexin Song Xin Ge Weitao Zheng Key Laboratory of Automobile Materials MOE School of Materials Science&Engineeringand Jilin Provincial International Cooperation Key Laboratory of High-Efficiency Clean Energy MaterialsElectron Microscopy Centerand International Center of Future ScienceJilin UniversityChangchun 130012JilinChina

oxygen evolution reaction(OER)is a bottleneck half-reaction in many important energy conversion processes(e.g.,water splitting),and one of the key issues lies to develop high-efficiency,cost-effective OER electrocatalysts.Rather than those popular extrinsic modulations of any catalysts with gradually degraded performance,we aim at the utilization of the intermediates offered from the undergoing OER as long-standing electrocatalysts.Herein,by inverted design,we extracted the bimetallic borides(FeCoB_(2))-derived intermediates metal borates in the OER,unlocking their potential as a selffunctionalized highly active catalytic phase in-situ formed on the metal boride surface for continuing OER operation.Mechanistically,the surface metal atoms are oxidized to oxyhydroxides,and the surface metalloids(B)are further transformed to the corresponding oxoanions to form metal borates.Such OER self-produced electrocatalyst exhibits a small overpotential of 295 mV at 10 mA/cm2 and its high catalytic activity lasts even after 200 h.Compared with FeCoB_(2),the catalytic activity of this electrochemically activated FeCoB_(2) is~7 times higher.The in-situ formed metal borate is dominatingly responsible for the obtained high catalytic activity.Such unique OER-produced self-functionalization surfaces of metal borates afford to greatly reduce the energy barrier of the continuing OER,thereby accelerating the reaction process.

关键词： Inverted design Self-functional surfaces Metal borate Water splitting oxygen evolution reaction

Super-exchange effect induced by early 3d metal doping on NiFe_(2)O_(4)(001)surface for oxygen evolution reaction

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Journal of Energy Chemistry 2023年第3期78卷 21-29,I0002页

作者： Shuhao Wang Xinyan Liu Xiang Chen Kamran Dastafkan Zhong-Heng Fu Xin Tan Qiang Zhang Chuan Zhao School of Chemistry The University of New South WalesSydneyNSW 2052Australia Beijing Key Laboratory of Green Chemical reaction Engineering and Technology Department of Chemical EngineeringTsinghua UniversityBeijing 100084China Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of ChinaChengdu 611731SichuanChina Integrated Materials Design Laboratory Department of Applied MathematicsResearch School of PhysicsThe Australian National UniversityCanberraACT 2601Australia

Understanding the intrinsic activity of oxygen evolution reaction(OER) is crucial for catalyst design.To date,different metal-doping strategies have been developed to achieve this,but the involving mechanisms remain unclear.Here,the electronic structure of the transition metal-doped NiFe_(2)O_(4)(001) surface is scrutinized for OER intrinsic activity using density functional theory calculations.Five 3d-orbital filling metals(Ti,V,Cr,Mn,and Co) are introduced as dopants onto A-and B-layers of the NiFe_(2)O_(4)(001) surface,and variation of oxidation states over Fe sites is observed on B-layer.Analyzing the magnetic moment and charge transfer of surface cation sites reveals that the variation of Fe oxidation states originates from the super-exchange effect and is influenced by the t2g-electron configuration of 3d metal dopants.This trend governs the generation of highly-active Fe3+sites on the B-layer,the adsorption strength of OER intermediates,i.e.,*O and*OH,and therefore the intrinsic activity.The finding of super-exchange mechanism induced by 3d early metal doping offers insights into electronic structure tailoring strategies for improving the intrinsic activity of OER electrocatalysts.

关键词： oxygen evolution reaction NiFe spinel Oxidation states Super-exchange mechanism Density functional theory

Organophosphine ligand derived sandwich-structural electrocatalyst for oxygen evolution reaction

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Journal of Energy Chemistry 2022年第7期31卷 74-83,I0003页

作者： Zejun Sun Wenjuan Xu Liutao Guo Qiang Han Jianyi Gao Jiaping Wang Yanru Feng Chengrui Li Qionglin Liang Hong-bin Sun Yang Yang Department of Chemistry Northeastern UniversityShenyang 110819LiaoningChina Key Laboratory of Bioorganic Phosphorus Chemistry&Chemical Biology(Ministry of Education) Department of ChemistryCenter for Synthetic and Systems BiologyTsinghua UniversityBeijing 100084China Astronaut Centre of China Beijing 100094China Nano Science Technology Center Department of Materials Science and EngineeringDepartment of ChemistryRenewable Energy and Chemical Transformation Cluster University of Central FloridaOrlandoFL 32826United States

The synchronous construction of metal phosphate and phosphorus-doped carbon structures is of great significance to innovate the design,synthesis,and application of catalysts,as these phosphoruscontaining composite materials have shown a remarkable contribution to electrocatalysts.However,their preparation procedure generally involves using large amounts of excess phosphorus sources for phosphorization,which inevitably release poisonous PH_(3) or dangerous phosphorus vapor.Here,a strategy for in-situ formation of FePO_(4) embedded in P-doped carbon 2D nano film(FePO_(4)/PdC)is developed using a highly integrated precursor,which is a small molecular organophosphine ligand,1,1’bis(diphenylphosphine)ferrocene(DPPF).The multi-source precursor DPPF that contains Fe,P,and C is molecular-vapor-deposited on the nickel foam(NF)supported ZIF-67 nanosheets to obtain the composite catalyst,namely DPPF-500/ZIF-67/NF.FePO_(4)/PdC encapsulated the ZIF-67 derived Co/N-doped carbon matrix(Co NC)to form a sandwich structure FePO_(4)/PdC@CoNC.The constructed catalyst shows good performance for OER,requiring an overpotential of only 297 m V to deliver 600 m A/cm^(2) with a Tafel slope of 42.7 m V dec^(-1).DFT calculations demonstrate that the synergistic effects between the metal active center and P-doped carbon film reduce the energy barriers and improve electron transport.This method of constructing P-containing catalysts overcomes the demand for additional P sources to realize eco-friendly fabrication and yields a unique structure with good catalytic activity.

关键词： Organophosphorus ligand Synchronous Synthesis FePO_(4) P-doped Carbon 2D nano film oxygen evolution reaction

Rational construction of high-active CO_(3)O_(4) electrocatalysts for oxygen evolution reaction

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Nano Research 2023年第1期16卷 624-633页

作者： Tianyun Zhang Shichao Zhao Chuanming Zhu Jing Shi Chao Su Jiawen Yang Meng Wang Jun Li Junhui Li Pingle Liu Conghui Wang College of Chemical Engineering Xiangtan UniversityXiangtan 411105China State Key Laboratory of Coal Conversion Institute of Coal ChemistryChinese Academy of SciencesTaiyuan 030001China Analytical Instrumentation center Institute of Coal ChemistryChinese Academy of SciencesTaiyuan 030001China

Rational construction of high-efficiency electrocatalysts for oxygen evolution reaction(OER)is critical for renewable-energy technologies,but it is highly challenging to rationally regulate their surface structures to improve the OER performance.Herein,we proposed a“model-etching”strategy to investigate chemical etching of CO_(3)O_(4).The cubic CO_(3)O_(4)nanocrystals enclosed by well-defined facets are synthesized as model crystals,whose uniform surface structures allow us to study the etching mechanism at atomic level.Etching kinetics study together with DFT calculations discloses that{111}facets,the highly active facets for OER,serve as etch-stop facets in the etching reaction and H_(2)SO_(4)molecules play a special role in creating surface Co2^(+),the active center of OER.These results direct us to rationally optimize the surface structures of CO_(3)O_(4) to develop highly active OER electrocatalysts.The favorable performance of overpotential(η)and the Tafel slope decrease even to 268 mV@10 mA·cm−2 and 74 mV·dec−1,respectively.In general,our study shows that chemical etching of model crystals could help us rationally construct high-efficiency electrocatalysts.

关键词： cobalt oxide chemical etching high active facets oxygen evolution reaction surface structure

Recent progress on bimetallic NiCo and CoFe based electrocatalysts for alkaline oxygen evolution reaction: A review

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Journal of Energy Chemistry 2022年第4期31卷 101-137页

作者： Gebrehiwet Abrham Gebreslase Maria Victoria Martínez-Huerta Maria Jesus Lázaro Instituto de Carboquímica CSIC.Miguel LuesmaCastán 450018ZaragozaSpain Instituto de Catálisis y Petroleoquímica CSIC.Marie Curie 228049MadridSpain

The deployment of hydrogen as an energy carrier is found to be a vital alternative fuel for the future. It is expected that water electrolysis, powered by renewable energy sources, be able to scale-up hydrogen production. However, the reaction kinetic of oxygen evolution reaction(OER) is a sluggish process, which predominantly limits the efficiency of water electrolysis. This review recapitulates the recent progress and efforts made in the design and development of two selected earth-abundant bimetallic electrocatalysts(Ni Co and Co Fe) for alkaline OER. Each bimetal electrocatalyst is thoroughly outlined and discussed in five sub-sections, including bimetal(oxy) hydroxides, Layered double hydroxides(LDHs) structures,oxides, composites, alloy and nanostructured electrocatalysts, and assembled with heteroatoms.Furthermore, a brief introduction to an in situ/operando characterization techniques and advantages for monitoring the structure of the electrocatalysts is provided. Finally, a summary outlining the challenges and conceivable approaches to advance OER performance is highlighted and discussed.

关键词： Water electrolysis oxygen evolution reaction Bimetallic electrocatalyst Nickel Cobalt and iron

Heterointerface of all-alkynyl-protected Au_(28) nanoclusters anchored on NiFe-LDHs boosts oxygen evolution reaction:a case to unravel ligand effect

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Rare Metals 2023年第12期42卷 4029-4038页

作者： Quan-Li Shen Long-Yun Shen Le-Yi Chen Lu-Bing Qin Yong-Gang Liu Nicholas M.Bedford Francesco Ciucci Zheng-Hua Tang School of Environment and Energy Guangzhou Higher Education Mega CentreNew Energy Research InstituteSouth China University of TechnologyGuangzhou 510006China Division of Emerging Interdisciplinary Areas The Hong Kong University of Science and TechnologyHong Kong 999077China Department of Mechanical and Aerospace Engineering The Hong Kong University of Science and TechnologyHong Kong 999077China School of Chemical Engineering University of New South Wales SydneySydneyNSW2052Australia HKUST Shenzhen-Hong Kong Collaborative Innovation Research Institute Shenzhen 518048China Energy Institute The Hong Kong University of Science and TechnologyHong Kong 999077China

Ultrasmall Au nanoclusters have been proven to effectively enhance the catalytic performance of NiFe layered double hydroxides(NiFe-LDHs)toward oxygen evolution reaction(OER),yet the surface ligand effect of the Au nanoclusters still remains elusive.Herein,a systematic study is reported to examine the OER performance of NiFe-LDHs supported atom-precise all alkynyl-protected[Au_(28)(~tBuC≡C)17]~-nanoclusters(Au_(28)-Alkynyl in short)and thiolate-protected Au_(28)(TBBT)_(20)(TBBT=4-tert-butylbenzene thiol)counterp arts(Au_(28)-Thiolate in short).The Au_(28)-Alkynyl cluster has characteristic absorbance feature,and its composition is verified by mass spectrometry.It possesses a drastically different structure from the reported mixed ligand protected Au_(28)nanoclusters.Interestingly,the NiFe-LDHs loaded with Au_(28)-Alkynyl exhibited a superior OER performance than the sample loaded with Au28-Thiolate under the same conditions,evidenced by a smaller overpotential of 205 mV at the current density of 10 mA·cm^(-2)and a lower Tafel slope value of 41.0 mV·dec^(-1)in 1 mol·L^(-1)KOH.Such excellent performance is attributed to the interfaces created between the NiFe-LDHs and the Au nanoclusters,as density functional theory calculations reveal that more significant charge transfer occurs in Au_(28)-Alkynyl/NiFeLDHs catalyst,and more importantly,the energy barrier of the potential-determining step in the OER process for Au28-Alkynyl/NiFe-LDHs is much lower than that of Au28-Thiolate/NiFe-LDHs hence favors the electrocatalytic reaction.

关键词： NiFe layered double hydroxides Au_(28)nanoclusters Alkynyl ligand oxygen evolution reaction Density functional theory calculations