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Nitrogen incorporated oxygen vacancy enriched MnCo_(2)O_(x)/BiVO_(4) photoanodes for efficient and stable photoelectrochemical water splitting

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Nano Research 2024年第3期17卷 1140-1150页

作者： Liangcheng Xu Yingjuan Zhang Boyan Liu Xin Wang Gangqiang Zhu Lianzhou Wang Songcan Wang Wei Huang Frontiers Science Center for Flexible Electronics Xi’an Institute of Flexible Electronics(IFE)Northwestern Polytechnical University127 West Youyi RoadXi’an 710072China School of Physics and Information Technology Shaanxi Normal UniversityXi’an 710062China Nanomaterials Centre Australian Institute for Bioengineering and Nanotechnology and School of Chemical EngineeringThe University of QueenslandBrisbaneQueensland 4072Australia Research&Development Institute of Northwestern Polytechnical University in Shenzhen Sanhang Science&Technology BuildingNo.45thGaoxin South 9th RoadNanshan DistrictShenzhen 518063China

Oxygen vacancies in oxygen evolution cocatalysts(OECs)can significantly improve the photoelectrochemical(PEC)water splitting performance of photoanodes.However,OECs with abundant oxygen vacancies have a poor stability when exposing to the highly-oxidizing photogenerated holes.Herein,we partly fill oxygen vacancies in a MnCo_(2)O_(x) OEC with N atoms by a combined electrodeposition and sol-gel method,which dramatically improves both photocurrent density and stability of a BiVO_(4) photoanode.The optimized N filled oxygen vacancy-rich MnCo_(2)O_(x)/BiVO_(4) photoanode(3 at.%of N)exhibits an outstanding photocurrent density of 6.5 mA·cm^(-2) at 1.23 VRHE under AM 1.5 G illumination(100 mW·cm^(-2)),and an excellent stability of over 150 h.Systematic characterizations and theoretical calculations demonstrate that N atoms stabilize the defect structure and modulate the surface electron distribution,which significantly enhances the stability and further increases the photocurrent density.Meanwhile,other heteroatoms such as carbon,phosphorus,and sulfur are confirmed to have similar effects on improving PEC water splitting performance of photoanodes.

关键词： water splitting oxygen evolution bismuth vanadate(BiVO_(4)) filling oxygen vacancies cocatalysts

Recent progress of cobalt-based electrocatalysts for water splitting: Electron modulation, surface reconstitution, and applications

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Nano Research 2024年第4期17卷 2234-2269页

作者： Zhijian Liang Di Shen Lei Wang Honggang Fu Key Laboratory of Functional Inorganic Material Chemistry Ministry of Education of the People’s Republic of ChinaHeilongjiang UniversityHarbin 150080China

Electrocatalytic water splitting is an essential and effective means to produce green hydrogen energy structures,so it is necessary to develop non-precious metal catalysts to replace precious metals.Cobalt-based catalysts present effective alternatives due to the diverse valence states,adjustable electronic structures,and plentiful components.In this review,the catalytic mechanisms of hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)for electrocatalytic water splitting are described.Then,the synthesis strategies of various cobalt-based catalysts are systematically summarized,followed by the relationships between the structure and performance clarified.Subsequently,the effects of d-band center and spin regulation for cobalt-based catalysts are also discussed.Furthermore,the dynamic electronic and structural devolution of cobalt-based catalysts are elucidated by combining a series of in-situ characterizations.Finally,we highlight the challenges and future developed directions of cobalt-based catalysts for electrocatalytic water splitting.

关键词： cobalt-based electrocatalysts water splitting electron modulation surface reconfiguration

Electrostatically connected nanoarchitected electrocatalytic films for boosted water splitting

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Nano Research 2024年第3期17卷 1114-1122页

作者： Chao-Peng Wang Hao Sun Gang Bian Jia-Xi Wang Xixi Pang Guoqi Wang Jian Zhu Xian-He Bu School of Materials Science and Engineering National Institute for Advanced MaterialsNankai UniversityTianjin 300350China Tianjin Key Laboratory of Metal and Molecule-Based Material Chemistry Nankai UniversityTianjin 300350China Tianjin Key Laboratory for Rare Earth Materials and Applications Nankai UniversityTianjin 300350China

Active sites of two-dimensional(2D)electrocatalysts are often partially blocked owing to their inevitable stacking and hydrophobic polymeric binders in macroscale electrodes,therefore impeding their applications in efficient electrolyzers.Here,using layered double hydroxide(LDH)nanosheets as a model 2D electrocatalyst,we demonstrate that their performance toward water splitting can be boosted when they are electrostatically assembled into an organized structure pillared by hydrophilic polyelectrolytes or nanoparticles in a layer-by-layer(LbL)fashion.In particular,their mass activity on a planar electrode can be as large as 2.267 mA·μg^(-1) toward oxygen evolution reaction(OER),when NiFe-LDH nanosheets are electrostatically connected by poly(sodium 4-styrenesulfonate)(PSS),while drop-casted NiFe-LDH nanosheets only have a mass activity of 0.116 mA·μg^(-1).In addition,these homogeneous NiFe-LDH nanofilms can be easily deposited on three-dimensional(3D)surfaces with high areas,such as carbon cloths,to serve as practical electrodes with overpotentials of 328 mV at a current density of 100 mA·cm^(-2),and stability for 40 h.Furthermore,Pt nanoparticles can be LbL assembled with NiFe-LDH as bifunctional electrodes for synergistically boosted oxygen and hydrogen evolution reactions(HER),leading to successful overall water splitting powered by a 1.5 V battery.This study heralds the spatial control of 2D nanomaterials in nanoscale precision as an efficient strategy for the design of advanced electrocatalysts.

关键词： layer-by-layer(LbL)assembly layered double hydroxides(LDH) two-dimensional(2D)electrocatalysts oxygen evolution reaction(OER) water splitting

Molecular-level proton acceptor boosts oxygen evolution catalysis to enable efficient industrial-scale water splitting

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Green Energy & Environment 2024年第2期9卷 344-355页

作者： Yaobin Wang Qian Lu Xinlei Ge Feng Li Le Chen Zhihui Zhang Zhengping Fu Yalin Lu Yang Song Yunfei Bu Jiangsu Collaborative Innovation Center of Atmospheric Environment and Equipment Technology(CICAEET) Jiangsu Key Laboratory of Atmospheric Environment Monitoring and Pollution Control(AEMPC)UNIST-NUIST Energy and Environment Jointed Lab(UNNU)School of Environmental Science and TechnologyNanjing University of Information Science and Technology(NUIST)219 NingliuNanjing210044China Laboratory of Advanced Materials Shanghai Key Laboratory of Molecular Catalysis and Innovative MaterialsFudan University220 HandanShanghai200433China Jiangsu Key Laboratory of Advanced Materials and Technology School of Petrochemical EngineeringChangzhou University1 GehuChangzhou213164China Anhui Laboratory of Advanced Photon Science and Technology University of Science and Technology of China(USTC)96 JinzhaiHefeiAnhui 230026China School of Chemistry and Chemical Engineering Nanjing University of Science and Technology200 Xiaolingwei210094China

Industrial water splitting has long been suppressed by the sluggish kinetics of the oxygen evolution reaction(OER),which requires a catalyst to be efficient.Herein,we propose a molecular-level proton acceptor strategy to produce an efficient OER catalyst that can boost industrial-scale water splitting.Molecular-level phosphate(-PO_(4))group is introduced to modify the surface of PrBa_(0.5)Ca_(0.5)Co_(2)O_(5)+δ(PBCC).The achieved catalyst(PO_(4)-PBCC)exhibits significantly enhanced catalytic performance in alkaline media.Based on the X-ray absorption spectroscopy results and density functional theory(DFT)calculations,the PO_(4)on the surface,which is regarded as the Lewis base,is the key factor to overcome the kinetic limitation of the proton transfer process during the OER.The use of the catalyst in a membrane electrode assembly(MEA)is further evaluated for industrial-scale water splitting,and it only needs a low voltage of 1.66 V to achieve a large current density of 1 A cm^(-2).This work provides a new molecular-level strategy to develop highly efficient OER electrocatalysts for industrial applications.

关键词： Oxygen evolution reaction Nanofiber water splitting Proton acceptor Perovskite

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Atomically dispersed Ni electrocatalyst for superior urea-assisted water splitting

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Journal of Energy Chemistry 2024年第3期90卷 1-6,I0002页

作者： Fang Luo Shuyuan Pan Yuhua Xie Chen Li Yingjie Yu Zehui Yang College of Materials Science and Engineering State Key Laboratory of New Textile Materials&Advanced Processing TechnologyWuhan Textile UniversityWuhan 430200China Hubei Hydrogen Energy Technology Innovation Center Faculty of Materials Science and ChemistryChina University of GeosciencesWuhan 430074HubeiChina

Urea oxidation reaction(UOR) has been selected as substitution for oxygen evolution reaction ascribing to its low thermodynamic voltage as well as utilization of nickel as electrocatalyst.Herein,we report the formation of nickel single atoms(Ni-SAs) as exceptional bifunctional electrocatalyst toward UOR and hydrogen evolution reaction(HER) in urea-assisted water splitting.In UOR catalysis,Ni-SAs perform a superior catalytic performance than Ni-NP/NC and Pt/C ascribing to the formation of HOO-Ni-N_(4) structure evidenced by in-situ Raman spectroscopy,corresponding to a boosted mass activity by 175-fold at 1.4 V vs.RHE than Ni-NP/NC.Furthermore,Ni-SAs requires only 450 mV overpotential to obtain HER current density of 500 mA cm^(-2).136 mA cm^(-2) is achieved in urea-assisted water splitting at1.7 V for Ni-SAs,boosted by 5.7 times than Pt/C-IrO_(2) driven water splitting.

关键词： Urea oxidation reaction Hydrogen evolution reaction Nickel single atoms water splitting

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Insights on advanced substrates for controllable fabrication of photoanodes toward efficient and stable photoelectrochemical water splitting

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Carbon Energy 2024年第4期6卷 164-221页

作者： Huilin Hou Gang Shao Yang Wang Wai‐Yeung Wong Weiyou Yang Institute of Micro/Nano Materials and Devices Ningbo University of TechnologyNingboChina School of Materials Science and Engineering Zhengzhou UniversityZhengzhouChina Department of Applied Biology and Chemical Technology and Research Institute for Smart Energy The Hong Kong Polytechnic UniversityHong KongChina

Conversion of solar energy into H2 by photoelectrochemical(PEC)water splitting is recognized as an ideal way to address the growing energy crisis and environmental issues.In a typical PEC cell,the construction of photoanodes is crucial to guarantee the high efficiency and stability of PEC reactions,which fundamentally rely on rationally designed semiconductors(as the active materials)and substrates(as the current collectors).In this review work,we start with a brief introduction of the roles of substrates in the PEC process.Then,we provide a systematic overview of representative strategies for the controlled fabrication of photoanodes on rationally designed substrates,including conductive glass,metal,sapphire,silicon,silicon carbide,and flexible substrates.Finally,some prospects concerning the challenges and research directions in this area are proposed.

关键词： hydrogen photoanode photoelectrochemical substrates water splitting

Towards a new avenue for rapid synthesis of electrocatalytic electrodes via laser-induced hydrothermal reaction for water splitting

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International Journal of Extreme Manufacturing 2024年第1期6卷 340-351页

作者： Yang Sha Menghui Zhu Kun Huang Yang Zhang Francis Moissinac Zhizhou Zhang Dongxu Cheng Paul Mativenga Zhu Liu Department of Materials School of Natural SciencesThe University of ManchesterOxford RoadManchester M139PLUnited Kingdom Laser Processing Research Centre Department of MechanicalAerospace and Civil EngineeringSchool of EngineeringThe University of ManchesterOxford RoadManchester M139PLUnited Kingdom National Graphene Institute The University of ManchesterOxford RoadManchester M139PLUnited Kingdom Department of Chemical Engineering and Analytical Science School of EngineeringThe University of ManchesterOxford RoadManchester M139PLUnited Kingdom Research Centre for Laser Extreme Manufacturing Ningbo Institute of Materials Engineering and TechnologyChinese Academy of SciencesNingboPeople’s Republic of China

Electrochemical production of hydrogen from water requires the development ofelectrocatalysts that are active,stable,and low-cost for water splitting.To address these challenges,researchers are increasingly exploring binder-free electrocatalytic integratedelectrodes (IEs) as an alternative to conventional powder-based electrode preparation methods,for the former is highly desirable to improve the catalytic activity and long-term stability for large-scale applications of electrocatalysts.Herein,we demonstrate a laser-inducedhydrothermal reaction (LIHR) technique to grow NiMoO4nanosheets on nickel foam,which is then calcined under H2/Ar mixed gases to prepare the IE IE-NiMo-LR.This electrode exhibits superior hydrogen evolution reaction performance,requiring overpotentials of 59,116 and143 mV to achieve current densities of 100,500 and 1000 mA·cm-2.During the 350 h chronopotentiometry test at current densities of 100 and 500 m A·cm-2,the overpotentialremains essentially unchanged.In addition,NiFe-layered double hydroxide grown on Ni foam is also fabricated with the same LIHR method and coupled with IE-NiMo-IR to achieve water splitting.This combination exhibits excellent durability under industrial current density.The energy consumption and production efficiency of the LIHR method are systematicallycompared with the conventional hydrothermal method.The LIHR method significantly improves the production rate by over 19 times,while consuming only 27.78%of the total energy required by conventional hydrothermal methods to achieve the same production.

关键词： electrocatalytic electrode laser-induced hydrothermal reaction NiFe layered double hydroxides hydrogen evolution reaction water splitting energy consumption production rate

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Heterointerface engineering of assembled CoP_(2) on N-modified carbon as efficient trifunctional electrocatalysts for Zn-Air batteries and overall water splitting

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Nano Research 2024年第5期17卷 3801-3809页

作者： Yan Chen Zhenrui Yang Juan Wang Yun Yang Xuedong He Yang Wang Jiadong Chen Yaqing Guo Xin Wang Shun Wang Huile Jin Wenzhou Key Lab of Advanced Energy Storage and Conversion Zhejiang Province Key Lab of Leather EngineeringCollege of Chemistry and Materials EngineeringWenzhou UniversityWenzhou 325035China Zhejiang Engineering Research Center for Electrochemical Energy Materials and Devices Institute of New Materials and Industrial TechnologiesWenzhou UniversityWenzhou 325035China School of Chemical and Biomedical Engineering Nanyang Technological UniversitySingapore 637459Singapore

Enhancing catalytic activity through modulating the interaction between N-doped carbon and metal phosphides clusters is an effective approach.Herein,the electronic structure modulation of CoP_(2) supported N-modified carbon(CoP_(2)/NC)has been designed and prepared as efficient electrocatalysts for oxygen reduction reaction(ORR),oxygen evolution reaction(OER),and hydrogen evolution reaction(HER).Notably,CoP_(2)/NC-1 catalyst exhibits impressive performance in alkaline media,with an ORR half-wave potential of 0.84 V,as well as OER and HER overpotentials of 290 and 129 mV(at 10 mA·cm^(−2)),respectively.In addition,CoP_(2)/NC-1 produces a power density as high as 172.9 mW·cm^(−2),and excellent reversibility of 100 h at 20 mA·cm^(−2) in home-made Zn-air batteries.The experimental results demonstrate that the synergistic interactions between N modified carbon substrate and CoP_(2) material significantly enhance the kinetics of ORR,OER,and HER.Density functional theory(DFT)calculations reveal the strong electrons redistribution of CoP_(2) induced by high-density N atoms at the interface,thus optimizing the key intermediates and significantly lower the energy barrier of reactions.These electronic adjustments of CoP_(2) greatly enhance its kinetics of ORR/OER/HER,leading to faster reactions.This study provides profound insights into the specific modification of CoP_(2) by N-doped carbon,enabling the construction of efficient catalysts.

关键词： two-dimensional(2D)carbon metal-organic framework cobalt phosphide zinc air battery water splitting

MnS–MnO heterogeneous nanocube@N, S-doped carbon as a highly efficient bifunctional water splitting electrocatalyst

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Rare Metals 2024年第5期43卷 1977-1988页

作者： Xue-Qian Wang Xiang-Ying Ma Wang-Zhi Wu Hui-Bing He Nan-Nan Wang Ren-Ji Zheng Shao-Jian Ma Yan-Qiu Zhu Pei-Kang Shen Jin-Liang Zhu School of Resources Environment and Materials State Key Laboratory of Featured Metal Materials and Life-Cycle Safety for Composite Structures College of Chemistry and Chemical Engineering Guangxi University School of Chemistry and Chemical Engineering Guangxi Minzu University School of Minerals Processing and Bioengineering Central South University

A stable,efficient,and economical bifunctional electrolytic catalyst would be incredibly beneficial for the development of hydrogen production by electrocatalytic water splitting.In this study,we synthesized a novel MnS–MnO heterogeneous nanocube@N,S-doped carbon （MnS–MnO@NSC）.MnS–MnO nanocubes possess rich heterogeneous interfaces and plentiful catalytic active sites to promote electrochemical reactions,while the N,S-doped carbon shell possesses excellent conductivity and catalytic properties and protects the nanocubes.MnS–MnO@NSC exhibited excellent electrochemical properties as an effective bifunctional electrocatalyst for the hydrogen evolution reaction （HER） and oxygen evolution reaction（OER） in KOH solution.In the HER,the overpotential was as low as 124 mV at a current density of 10 mA·cm-2while in the OER,it was only 340 mV at 100 mA·cm-2under the same conditions.In addition,a MnS–MnO@NSC||MnS–MnO@NSC electrolyzer exhibited almost comparable activity and higher steadiness than those exhibited by the state-of-the-art Pt/C||RuO2/C system for full water splitting in KOH solution.

关键词： Manganese sulfide Manganese oxide Doped carbon Heterogeneous nanocube water splitting