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single-atom electrocatalyst and gel polymer electrolyte boost the energy density and life of aluminum-sulfur batteries

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Journal of Materials Science & Technology 2023年第21期152卷 86-93页

作者： Zheng Huang Wei Wang Mingyin Kou Haiping Lei Yiwa Luo Shuqiang Jiao State Key Laboratory of Advanced Metallurgy University of Science and Technology BeijingBeijing 100083China

Aluminum-sulfur(Al-S)batteries are regarded as a desirable candidate for large-scale energy storage be-cause of their high energy density and abundant natural resources of electrode materials.To address the critical issues of low discharge voltage and rapid capacity decay in Al-S batteries,here an electrocatalyst-assisted gel-polymer electrolyte(GPE)-based Al-S battery is fabricated using platinum nanoparticles deco-rated platinum/nitrogen co-doped graphene(PtNG)as sulfur host for positive electrode and metal-organic frameworks(MOF)filled GPE(MOF@GPE)as solid electrolyte.Pt-based active sites derived from Pt nan-oclusters’surface and atomically dispersed Pt-N_(2) chemical bonds in PtNG can catalyze the decomposition of sulfur and polysulfides in the electrochemical process,greatly accelerating the sulfur redox kinetics.Furthermore,the MOF fillers in MOF@GPE electrolyte significantly inhibit the shuttle effect of polysul-fides,efficiently improving the utilization of sulfur.Consequently,the established Al-S battery delivers a specific capacity of 1009 mAh g^(−1) with a discharge plateau of∼0.95 V,along with a capacity retention of 65% after 300 cycles,revealing ultrahigh energy density and long cycle life.Such a strategy of combin-ing electrocatalyst and MOF-based gel electrolyte affords a fresh plateau for promoting the rechargeable ability of Al-S batteries,advancing remarkable routes for achieving efficient and stable energy storage devices.

关键词： Aluminum-sulfur batteries Gel polymer electrolyte single atom electrocatalyst Shuttle effect Reaction kinetics

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Engineering the morphology and electronic structure of atomic cobalt-nitrogen-carbon catalyst with highly accessible active sites for enhanced oxygen reduction

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Journal of Energy Chemistry 2022年第10期31卷 469-477,I0012页

作者： Zhijun Li Leipeng Leng Siqi Ji Mingyang Zhang Hongxue Liu Jincheng Gao Jiangwei Zhang J.Hugh Horton Qian Xu Junfa Zhu Joint International Research Laboratory of Advanced Chemical Catalytic Materials&Surface Science College of Chemistry and Chemical EngineeringNortheast Petroleum UniversityDaqing 163318HeilongjiangChina Dalian National Laboratory for Clean Energy&State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina Department of Chemistry Queen0s UniversityKingstonOntario K7L 3N6Canada National Synchrotron Radiation Laboratory University of Science and Technology of ChinaHefei 230029AnhuiChina

The stabilization of non-precious metals as isolated active sites with high loading density over nitrogendoped carbon materials is essential for realizing the industrial application of single atom catalysts.However,achieving high loading of single cobalt active sites with greatly enhanced oxygen reduction reaction(ORR)activity and stability remains challenging.Here,an efficient approach was described to create a single atom cobalt electrocatalyst(Co SAs/NC)which possesses enhanced mesoporosity and specific surface area that greatly favor the mass transportation and exposure of accessible active sites.The electronic structure of the catalyst by the strong metal-support interaction has been elucidated through experimental characterizations and theoretical calculations.Due to dramatically enhanced mass transport and electron transfer endowed by morphology and electronic structure engineering,Co SAs/NC exhibits remarkable ORR performance with excellent activity(onset and half-wave potentials of 1.04 V(RHE)and 0.90 V(RHE),Tafel slope of 69.8 mV dec^(-1)and J_(k) of 18.8 mA cm^(-2)at 0.85 V)and stability(7 mV activity decay after 10,000 cycles).In additio n,the catalyst demonstrates great promise as an alternative to traditional Pt/C catalyst in zinc-air batteries while maintaining high performance in terms of high specific capacity of(796.1 mAh/g_(Zn)),power density(175.4 mW/cm^(2)),and long-term cycling stability(140 h).This study presents a facile approach to design SACs with highly accessible active sites for electrochemical transformations.

关键词： single atom electrocatalyst Non-precious metal Coordination environment Oxygen reduction reaction Catalytic activity Zn-air battery

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Enhancing electrical conductivity of single-atom doped Co_(3)O_(4) nanosheet arrays at grain boundary by phosphor doping strategy for efficient water splitting

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Nano Research 2022年第10期15卷 9511-9519页

作者： Yaohang Gu Xuanyu Wang Ateer Bao Liang Dong Xiaoyan Zhang Haijun Pan Wenquan Cui Xiwei Qi School of Materials Science and Engineering Northeastern UniversityShenyang 110189China College of Metallurgy and Energy North China of Science and TechnologyTangshan 063210China School of Resources and Materials Northeastern University at QinhuangdaoQinhuangdao 066004China Key Laboratory of Dielectric and Electrolyte Functional Material Hebei Province Northeastern University at QinhuangdaoQinhuangdao 066004China College of Chemical Engineering Hebei Provincial Key Laboratory of Environmental Photocatalytic and Electrocatalytic MaterialsNorth China University of Science and TechnologyTangshan 063210China

High electrical conductivity guarantees a rapid electron transfer and thus plays an important role in electrocatalysis.In particular,for the single atom catalysts(SACs),to facilitate interaction between the single atom and supports,precisely engineering the conductivity represents a promising strategy to design SACs with high electrochemical efficiency.Here we show rhodium(Rh)SAC anchored on Co_(3)O_(4) nanosheets arrays on nickel foam(NF),which is modified by a facile phosphorus(P-doped Rh SACCo_(3)O_(4)/NF),possessing an appropriate electronic structure and high conductivity for electrocatalytic reaction.With the introduction of P atom in the lattice,the electrocatalyst demonstrates outstanding alkaline oxygen evolution reaction(OER)activity with 50 mA·cm^(−2) under overpotential of 268 mV,6 times higher than that of Ir/C/NF.More interestingly,the P-doped Rh SAC-Co_(3)O_(4)/NF can get 50 mA·cm^(−2) at only 1.77 V for overall water splitting.Both electrical conductivity studies and density functional theory(DFT)calculations reveal that the high conductivity at grain boundary improves the charge transfer efficiency of the Rh catalytic center.Furthermore,other noble-metal(Ir,Pd,and Ru)doped Co_(3)O_(4) nanosheets arrays are prepared to exhibit the general efficacy of the phosphorus doping strategy.

关键词： overall water splitting electrical conductivity single atom electrocatalyst phosphor doping strategy

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