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An insight into the enhanced mechanism of Ru–MoO_(2)interfacial chemical bonding for hydrogen evolution reaction in alkaline media

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Nano Research 2023年第2期16卷 2230-2235页

作者： Ying Yuan Wei Han Chenchen Zhang Qi Sun Yingxin Hao Jiamin Zhao Jinsheng Zhao Xiujuan Zhong Ningqiang Zhang School of Chemistry and chemical Engineering Liaocheng UniversityLiaocheng 252059China National Energy R&D Center for Petroleum Refining Technology Research Institute of Petroleum ProcessingChina Petroleum&Chemical Corporation(SINOPEC)Beijing 100083China Institute for Catalysis Hokkaido UniversityN-21W-10SapporoHokkaido 001-0021Japan

An effective strategy was proposed to control the formation of the interfacial bonding between Ru and molybdenum oxide support to stabilize the Ru atoms with the aim to enhance the hydrogen evolution reaction(HER)activity of the resultant catalysts in alkaline medium.The different interfacial chemical bonds,including Ru–O,Ru–O–Mo,and mixed Ru–Mo/Ru–O–Mo,were prepared using an induced activation strategy by controlling the composition of reducing agents in the calcination process.And the regulation mechanism of the interfacial chemical bonds in molybdenum oxide supported Ru catalysts for optimizing HER activity was investigated by density functional theory(DFT)and experimental studies.We found that a controlled interfacial chemical Ru–O–Mo bonding in Ru-MoO_(2)/C manifests a 12-fold activity increase in catalyzing the hydrogen evolution reaction relative to the conventional metal/metal oxide catalyst(Ru-O-MoO_(2)/C).In a bifunctional effect,the interfacial chemical Ru-O-Mo sites promoted the dissociation of water and the production of hydrogen intermediates that were then adsorbed on the nearby Ru surfaces and recombined into molecular hydrogen.As compared,the nearby Ru surfaces in Ru–Mo bonding have weak adsorption capacity for the generation of these hydrogen intermediates,resulting in a 5-fold increase HER activity for Ru-Mo-MoO_(2)/C catalyst compared with Ru-O-MoO_(2)/C.

关键词： interfacial chemical bonds alkaline media hydrogen evolution reaction Ru–O–Mo

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Rational design of interfacial bonds within dual carbon-protected manganese oxide towards durable aqueous zinc ion battery

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Science China Chemistry 2023年第5期66卷 1406-1416页

作者： Xiuli Guo Chunguang Li Xiyang Wang Zhenhua Li Hui Zeng Pan Hou Minggang Xie Yuxin Li Zhan Shi Shouhua Feng State Key Laboratory of Inorganic Synthesis and Preparative Chemistry College of ChemistryJilin UniversityChangchun 130012China Department of Mechanical and Mechatronics Engineering Waterloo Institute for NanotechnologyMaterials Interface FoundryUniversity of WaterlooWaterlooOntario N2L 3G1Canada

Manganese-based cathode materials are promising candidates for aqueous zinc ion batteries(AZIBs)by reason of their low cost and high energy density.However,their practical applicability is hampered by the intrinsic defects of poor electrical conductivity,sluggish reaction kinetics,and severe structural deterioration.Herein,we constructed a hierarchically porous structure composed of carbon-encapsulated Mn O nanoparticles(MOC)and three-dimensional(3D)nitrogen-doped graphene aerogel(NGA)(denoted as MOC@NGA).The hybrid was synthesized by a facile in-situ coprecipitation and annealing of manganesebased metal-organic framework(Mn-MOF74)and NGA composite(Mn-MOF74@NGA).Specifically,the carbon shells inherited from organic ligand of Mn-MOF74 could restrain the volume changes of Mn O,and the porous NGA prevented the agglomeration of MOC nanoparticles and enriched the types of interfacial chemical bonds.Profiting from the synergistic effect of rich interface chemical bonds and dual-carbon protection,the MOC@NGA hybrids exhibit fast interfacial electron/charge transfer and transport,and outstanding structural stability.Therefore,MOC@NGA cathode delivers an excellent rate performance(270 and 99.8 m Ah g^(-1)at 0.1 and 2.0 A g^(-1))and maintains an excellent specific capacity of 151.6 m Ah g^(-1)after 2,000cycles at 1.0 A g^(-1).Moreover,the fabricated MOC@NGA-based quasi-solid-state battery not only achieves outstanding flexibility but also displays impressive cycling stability,demonstrating a promising potential for portable and flexible equipment.This work provides a feasible strategy for the fabrication of the bridging structure of manganese-based oxides and porous carbon matrix for high-specific capacity and durable AZIBs cathodes.

关键词： manganese oxide interfacial chemical bonds carbon modification aqueous zinc ion batteries

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