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Design Principles and Mechanistic Understandings of Non-Noble-Metal bifunctional electrocatalysts for Zinc-Air Batteries

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Nano-Micro Letters 2024年第9期16卷 13-48页

作者： Yunnan Gao Ling Liu Yi Jiang Dexin Yu Xiaomei Zheng Jiayi Wang Jingwei Liu Dan Luo Yongguang Zhang Zhenjia Shi Xin Wang Ya‑Ping Deng Zhongwei Chen Power Battery and Systems Research Center State Key Laboratory of CatalysisDalian Institute of Chemical PhysicsDalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023People’s Republic of China Department of Chemical Engineering University of WaterlooWaterlooON N2L 3G1Canada Institute of Carbon Neutrality Zhejiang Wanli UniversityNingbo 315100People’s Republic of China College of Materials and Chemistry China Jiliang UniversityHangzhou 310018People’s Republic of China

Zinc-air batteries(ZABs)are promising energy storage systems because of high theoretical energy density,safety,low cost,and abundance of ***,the slow multi-step reaction of oxygen and heavy reliance on noble-metal catalysts hinder the practical applications of ***,feasible and advanced non-noble-metal elec-trocatalysts for air cathodes need to be identified to promote the oxygen catalytic *** this review,we initially introduced the advancement of ZABs in the past two decades and provided an overview of key developments in this ***,we discussed the work-ing mechanism and the design of bifunctional electrocatalysts from the perspective of morphology design,crystal structure tuning,interface strategy,and atomic *** also included theoretical studies,machine learning,and advanced characterization technologies to provide a comprehensive understanding of the structure-performance relationship of electrocatalysts and the reaction pathways of the oxygen redox ***,we discussed the challenges and prospects related to designing advanced non-noble-metal bifunctional electrocatalysts for ZABs.

关键词： Zinc-air batteries bifunctional electrocatalysts Design principles Mechanistic understandings

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Synergistic Ru/RuO_(2) heterojunctions stabilized by carbon coating as efficient and stable bifunctional electrocatalysts for acidic overall water splitting

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Nano Research 2024年第8期17卷 6931-6939页

作者： Man Wu Yuying Fan Yang Huang Dongxu Wang Ying Xie Aiping Wu Chungui Tian Key Laboratory of Functional Inorganic Material Chemistry Ministry of Education of the People’s Republic of ChinaHeilongjiang UniversityHarbin 150080China

The development of highly active and stable acidic water oxidation electrocatalysts is of great significant for promoting the industrial application of proton exchange membrane ***-based catalysts have broad application prospects in acidic water oxidation,but their limitations in stability and activity hinder their further ***,a nitrogen-doped carbon(NC)coated porous Ru/RuO_(2) heterojunctional hollow sphere(Ru/RuO_(2)/NC)is designed as high-active and stable bifunctional electrocatalyst for acidic oxygen evolution reaction(OER)and hydrogen evolution reaction(HER).In synthesis,the key is to use mesoporous polydopamine spheres as a template for forming hollow spheres,a source of NC coating and a reducing agent for forming Ru/RuO_(2) *** Ru/RuO_(2) heterojunction adjusts the electronic structure of Ru active sites,optimizing the adsorption of intermediate ***,the NC coating and the interaction between NC and Ru/RuO_(2) effectively prevent Ru from over-oxidation and *** porous hollow structure provides more exposed active sites and promotes mass ***,Ru/RuO_(2)/NC exhibits outstanding OER and HER performance with low overpotentials of 211 and 32 mV at 10 mA·cm^(−2),respectively,and shows excellent *** acid water splitting electrolyzer,based on the bifunctional Ru/RuO_(2)/NC,requires low cell voltages of 1.46 and 1.76 V at 10 and 100 mA·cm^(−2),respectively,with good stability for over 100 h operation,surpassing Pt/C||RuO_(2) and most of the reported catalysts.

关键词： hollow heterojunction bifunctional electrocatalysts oxygen evolution hydrogen evolution acidic water splitting

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Self-supported NiFe-LDH nanosheets on NiMo-based nanorods as high-performance bifunctional electrocatalysts for overall water splitting at industrial-level current densities

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Nano Research 2024年第5期17卷 3769-3776页

作者： Yan Zhang Biao Feng MingLei Yan Zhen Shen Yiqun Chen Jingyi Tian Fengfei Xu Guanghai Chen Xizhang Wang Lijun Yang Qiang Wu Zheng Hu Key Laboratory of Mesoscopic Chemistry of Ministry of Education(MOE)and Jiangsu Provincial Lab for Nanotechnology School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China College of Water Conservancy and Hydropower Engineering Sichuan Agricultural UniversityYa’an 625014China

Efficient,durable and economic electrocatalysts are crucial for commercializing water electrolysis ***,we report an advanced bifunctional electrocatalyst for alkaline water splitting by growing NiFe-layered double hydroxide(NiFe-LDH)nanosheet arrays on the conductive NiMo-based nanorods deposited on Ni foam to form a three-dimensional(3D)architecture,which exhibits exceptional performances for both hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).In overall water splitting,only the low operation voltages of 1.45/1.61 V are required to reach the current density of 10/500 mA·cm^(-2),and the continuous water splitting at an industrial-level current density of 500 mA·cm^(-2) shows a negligible degradation(1.8%)of the cell voltage over 1000 *** outstanding performance is ascribed to the synergism of the HER-active NiMo-based nanorods and the OER-active NiFe-LDH nanosheet arrays of the hybridized 3D ***,the dense NiFe-LDH nanosheet arrays enhance the local pH on cathode by retarding OH-diffusion and enlarge the electrochemically active surface area on anode,while the conductive NiMo-based nanorods on Ni foam much decrease the charge-transfer resistances of both *** study provides an efficient strategy to explore advanced bifunctional electrocatalysts for overall water splitting by rationally hybridizing HER-and OER-active components.

关键词： alkaline water splitting bifunctional electrocatalysts layered double hydroxides high durability industrial current densities

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Constructing P-CoMoO_(4)@NiCoP heterostructure nanoarrays on Ni foam as efficient bifunctional electrocatalysts for overall water splitting

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纳米材料科学:英文版 2023年第3期5卷 278-286页

作者： Ning You Shuai Cao Mengqiu Huang Xiaoming Fan Kun Shi Haijian Huang Zhangxian Chen Zeheng Yang Weixin Zhang School of Chemistry and Chemical Engineering Hefei University of Technology230009HefeiAnhuiPR China Anhui Province Key Laboratory of Advanced Catalytic Materials and Reaction Engineering 230009HefeiAnhuiPR China

Improving catalytic activity and durabilty through the structural and compositional development of bifunctional electrocatalysts with low cost,high activity and stability is a challenging issue in electrochemical water ***,we report the fabrication of heterostructured P-CoMoO_(4)@NiCoP on a Ni foam substrate through interface engineering,by adjusting its composition and *** from the tailored electronic structure and exposed active sites,the heterostructured P-CoMoO_(4)@NiCoP/NF arrays can be coordinated to boost the overall water *** addition,the superhydrophilic and superaerophobic properties of P-CoMoO_(4)@NiCoP/NF make it conducive to water dissociation and bubble separation in the electrocatalytic *** heterostructured PCoMoO_(4)@NiCoP/NF exhibits excellent bifunctional electrocatalysis activity with a low overpotential of 66 mV at 10 mA cm^(-2) for HER and 252 mV at 100 mA cm^(-2) for *** 1.62 V potential is required to deliver 20 mA cm^(-2) in a two-electrode electrolysis system,providing a decent overall water splitting *** rational construction of the heterostructure makes it possible to regulate the electronic structures and active sites of the electrocatalysts to promote their catalytic activity.

关键词： Heterostructure P-CoMoO_(4)@NiCoP bifunctional electrocatalysts Overall water splitting

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bifunctional electrocatalysts for rechargeable Zn-air batteries

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Chinese Journal of Catalysis 2019年第9期40卷 1298-1310页

作者： Yibo Guo Ya-Nan Chen Huijuan Cui Zhen Zhou School of Materials Science and Engineering Institute of New Energy Material ChemistryKey Laboratory of Advanced Energy Materials Chemistry (Ministry of Education)Renewable Energy Conversion and Storage Center (ReCast)Nankai UniversityTianjin 300350China

Zn-air batteries have attracted extensive attention for their unique features including high energy density,safety,low cost and environmental ***,due to their poor chargeability and low efficiency,the practical application remains a *** main obstacles are the intrinsic slow reaction kinetics on air cathodes,including oxygen reduction reaction during the discharging process and oxygen evolution reaction during the recharging *** for efficient bifunctional oxygen electrocatalysts is key to solve these *** this review,the configuration and fundamental oxygen electrochemical reactions on air cathodes are briefly introduced for Zn-air batteries ***,the latest bifunctional oxygen electrocatalysts are summarized in ***,the perspectives are provided for the future investigations on bifunctional oxygen electrocatalysts.

关键词： bifunctional electrocatalysts Oxygen-reduction reaction Oxygen-evolution reaction Zn-air batteries Hybrid materials

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Optimizing band structure of CoP nanoparticles via rich-defect carbon shell toward bifunctional electrocatalysts for overall water splitting

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Carbon Energy 2023年第3期5卷 112-125页

作者： Juncheng Wu Zhe‐Fan Wang Taotao Guan Guoli Zhang Juan Zhang Jie Han Shengqin Guan Ning Wang Jianlong Wang Kaixi Li CAS Key Laboratory of Carbon Materials Institute of Coal ChemistryChinese Academy of SciencesTaiyuanShanxiPR China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijingPR China Institute Energy Innovation College of Materials Science and EngineeringTaiyuan University of TechnologyTaiyuanShanxiPR China

Transition-metal phosphides(TMPs)with high catalytic activity are widely used in the design of electrodes for water ***,a major challenge is how to achieve the trade-off between activity and stability of ***,a novel method for synthesizing CoP nanoparticles encapsu-lated in a rich-defect carbon shell(CoP/DCS)is developed through the self-assembly of modified polycyclic aromatic *** graft and removal of high-activity C-N bonds of aromatic molecules render the controllable design of crystallite defects of carbon *** density functional theory calculation indicates that the carbon defects with unpaired electrons could effectively tailor the band structure of *** from the improved activity and corrosion resistance,the CoP/DCS delivers outstanding difunctional hydrogen evolution reaction(88 mV)and oxygen evolution reaction(251 mV)performances at 10 mA cm^(−2)current ***,the coupled water electrolyzer with CoP/DCS as both the cathode and anode presents ultralow cell voltages of 1.49 V to achieve 10 mA cm^(−2)with long-time *** strategy to improve TMPs electrocatalyst with rich-DCS and heterogeneous structure will inspire the design of other transition metal compound electrocatalysts for water splitting.

关键词： band structure bifunctional electrocatalysts CoP nanoparticles overall water splitting rich‐defect carbon

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Micro-nanostructural designs of bifunctional electrocatalysts for metal-air batteries

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Chinese Journal of Catalysis 2020年第3期41卷 390-403页

作者： Fang Shi Xuefeng Zhu Weishen Yang State Key Laboratory of Catalysis Dalian Institute of Chemical Physics the Chinese AcademyDalian 116023LiaoningChina University of Chinese Academy of Sciences Beijing 100049China

Water-based rechargeable metal-air batteries play an important role in the storage and conversion of renewable electric ***,the sluggish kinetics of the oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)have limited the practical application of rechargeable metal-air *** of reviews were focused on single functional electrocatalysts while few on bifunctional *** is indispensable but challenging to design a bifunctional electrocatalyst that is active and stable to the two ***,attempts to develop high active bifunctional electrocatalysts for both ORR and OER increase *** work is focused on the micro-nano design of advanced structures to improve the performance of bifunctional ***-metal materials,carbon materials and composite materials,and the methods developed to prepare micro-nano structures,such as electrochemical methods,chemical vapor deposition,hydrothermal methods and template methods are reported in ***,many strategies,such as adjustments of electronic structures,oxygen defects,metal-oxygen bonds,interfacial strain,nano composites,heteroatom doping etc.,have been used extensively to design bifunctional *** well understand the achievements in the recent literatures,this review focuses on the micro-nano structural design of materials,and the related methods and strategies are classed into two groups for the improvement of intrinsic and apparent *** fine adjustment of nano structures and an in-depth understanding of the reaction mechanism are also discussed briefly.

关键词： Oxygen reduction reaction Oxygen evolution reaction Rechargeable metal-air batteries bifunctional electrocatalysts Micro-nano structure

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CoxP@NiCo-LDH heteronanosheet arrays as efficient bifunctional electrocatalysts for co-generation of value-added formate and hydrogen with less-energy consumption

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Journal of Energy Chemistry 2020年第11期29卷 314-323页

作者： Mei Li Xiaohui Deng Yue Liang Kun Xiang Dan Wu Bin Zhao Haipeng Yang Jing-Li Luo Xian-Zhu Fu College of Materials Science and Engineering Shenzhen UniversityShenzhen 518055GuangdongChina Department of Chemical and Materials Engineering University of AlbertaEdmonton T6G 1H9AlbertaCanada

The inefficiency of water splitting is mainly due to the sluggish anodic water oxidation reaction. Replacing water oxidation with thermodynamically more favorable selective methanol oxidation reaction and developing robust bifunctional electrocatalysts are of great significance. Herein, a hierarchical heteronanostructure with Ni–Co layered double hydroxide(LDH) ultrathin nanosheets coated on cobalt phosphide nanosheets arrays(CoxP@NiCo-LDH) are fabricated and used for co-electrolysis of methanol/water to co-produce value-added formate and hydrogen with saving energy. Benefiting from the fast charge transfer introduced by phosphide nanoarrays, the synergy in nanosheets catalysts with hetero-interface,CoxP@NiCo-LDH/Ni foam(NF) exhibits superior electrocatalytic performance(10 mA cm-2@ 1.24 V and-0.10 V for methanol selective oxidation and hydrogen evolution reaction, respectively). Furthermore,CoxP@NiCo-LDH/NF-based symmetric two-electrode electrolyzer drives a current density of 10 m A cm-2 with a low cell voltage of only 1.43 V and the Faradaic efficiency towards the generation of formate and H2 are close to 100% in the tested range of current density(from 40 to 200 m A cm-2). This work highlights the positive effect of hetero-interaction in the design of more efficient eletrocatalysts and might guide the way towards facile upgrading of alcohols and energy-saving electrolytic H2 co-generation.

关键词： Cobalt phosphide bifunctional electrocatalysts Selective methanol oxidation H2 evolution reaction Co-electrolysis

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Biomass-derived nitrogen self-doped porous activation carbon as an effective bifunctional electrocatalysts

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Chinese Chemical Letters 2021年第1期32卷 92-98页

作者： Yuanqing Sun Yiming Ouyang Jiaqing Luo Huihui Cao Xiang Li Jingwen Ma Jian Liu Yuanhao Wang Lin Lu State Key Laboratory of Heavy Oil and Beijing Key Lab of Oil&Gas Optical Detection Technology College of ScienceChina University of PetroleumBeijing 102249China Hoffmann Institute of Advanced Materials Shenzhen PolytechnicShenzhen 518055China Renewable Energy Research Group(RERG) Department of Building Services EngineeringThe Hong Kong Polytechnic UniversityHong KongChina

The strategy of adopting cheap precursors or abundant resources,which can be obtained directly from nature,is a simple and excellent method of introducing accessible research into environmentally friendly ***,this is also an urgent requirement for the sustainable development of green ***,we introduce a simplistic and expandable method to prepare metal-free biomassderived nitrogen self-doped porous activation carbon(N-PAC) with large specific surface area(S_(BET)=1300.58 m^(2)/g).Moreover,the manufactural electrocatalysts exhibit prominent oxygen reduction reaction(ORR) performance in all PH *** compared with the commercial Pt/C catalyst,the N-PAC/800 with a positive onset potential at 10 mA/cm^(2)(0.93 V),half-wave potential(0.87 V),and limiting current(6.34 mA/cm^(2)) bring to light excellent catalytic stability,selectivity,and much-enhanced methanol ***,the prepared electrocatalysts possess considerable hydrogen evolution reaction(HER) performance with a less onset potential of 0.218 V(acidic medium) and0.271 V(alkaline medium) respectively,which can show similar catalytic activity across the whole pH *** bifunctional electrocatalyst,with excellent electrocatalytic properties,resource-rich,low cost,and environmental-friendly,hold a promising application in energy conversion and reserve.

关键词： Biomass-derived High specific surface area bifunctional electrocatalysts Metal-free Nitrogen-doped carbon

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Engineering iron-group bimetallic nanotubes as efficient bifunctional oxygen electrocatalysts for flexible Zn–air batteries

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eScience 2022年第5期2卷 546-556页

作者： Yanli Niu Shuaiqi Gong Xuan Liu Chen Xu Mingze Xu Shi-Gang Sun Zuofeng Chen Shanghai Key Laboratory of Chemical Assessment and Sustainability School of Chemical Science and EngineeringTongji UniversityShanghai200092China State Key Lab of Physical Chemistry of Solid Surface College of Chemistry and Chemical EngineeringXiamen UniversityXiamen361005China

Air cathode performance is essential for rechargeable zinc–air batteries(ZABs).In this study,we develop a self-templated synthesis technique for fabricating bimetallic alloys(FeNi_(3)),bimetallic nitrides(FeNi_(3)N)and heterostructured FeNi_(3)/FeNi_(3)N hollow *** to its structural and compositional advantages,FeNi_(3)/FeNi_(3)N exhibits remarkable bifunctional oxygen electrocatalytic performance with an extremely small potential gap of 0.68V between the oxygen evolution reaction(OER)and oxygen reduction reaction(ORR).Theoretical calculations reveal reduced Gibbs free energy for the rate-limiting O–O bond formation during OER due to the self-adaptive surface reconfiguration,which induces a synergistic effect between Fe(Ni)OOH developed in situ on the surface and the inner FeNi_(3)/FeNi_(3)*** fabricated using the FeNi_(3)/FeNi_(3)N catalyst shows high power density,small charge/discharge voltage gap and excellent cycling *** addition to its excellent battery performance,the corresponding quasi-solid-state ZAB shows robust flexibility and *** synthesis method is extended to prepare a CoFe/CoFeN oxygen electrocatalyst,demonstrating its applicability to other iron-group elements.

关键词： bifunctional electrocatalysts Oxygen electrocatalysis Bimetallic nitrides Hollow nanotube structure Zn-air batteries

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