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Multi-functional layered double hydroxides supported by nanoporous gold toward overall hydrazine splitting

Frontiers of Chemical Science and Engineering 2024年第1期18卷 61-69页

作者： Yongji Qin Huijie Cao Qian Liu Shaoqing Yang Xincai Feng Hao Wang Meiling Lian Dongxing Zhang Hua Wang Jun Luo Xijun Liu ShenSi Lab Shenzhen Institute for Advanced StudyUniversity of Electronic Science and Technology of ChinaShenzhen 518110China Institute for New Energy Materials and Low-Carbon Technologies School of Materials Science and EngineeringTianjin University of TechnologyTianjin 300384China State Key Laboratory of Featured Metal Materials and Life-cycle Safety for Composite Structures Guangxi Key Laboratory of Processing for Non-ferrous Metals and Featured MaterialsSchool of ResourcesEnvironment and MaterialsGuangxi UniversityNanning 530004China Institute for Advanced Study Chengdu UniversityChengdu 610106China China National Coal Group Corporation Beijing 100120China Tianjin Engineering Research Center of Civil Aviation Energy Environment and Green Development School of Transportation Science and EngineeringCivil Aviation University of ChinaTianjin 300300China

Layered double hydroxides have demonstrated great potential for the oxygen evolution reaction,which is a crucial half-reaction of overall water splitting.However,it remains challenging to apply layered double hydroxides in other electrochemical reactions with high efficiency and stability.Herein,we report two-dimensional multifunctional layered double hydroxides derived from metalorganic framework sheet precursors supported by nanoporous gold with high porosity,which exhibit appealing performances toward oxygen/hydrogen evolution reactions,hydrazine oxidation reaction,and overall hydrazine splitting.The as-prepared catalyst only requires an overpotential of 233 mV to reach 10 mA·cm^(-2) toward oxygen evolution reaction.The overall hydrazine splitting cell only needs a cell voltage of 0.984 V to deliver 10 mA·cm^(-2),which is far more superior than that of the overall water splitting system(1.849 V).The appealing performances of the catalyst can be contributed to the synergistic effect between the metal components of the layered double hydroxides and the supporting effect of the nanoporous gold substrate,which could endow the sample with high surface area and excellent conductivity,resulting in superior activity and stability.

关键词： layered double hydroxide oxygen evolution reaction hydrazine oxidation reaction overall hydrazine splitting hydrogen production

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Resisting metal aggregation in pyrolysis of MOFs towards highdensity metal nanocatalysts for efficient hydrazine assisted hydrogen production

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Nano Research 2023年第5期16卷 6067-6075页

作者： Jieting Ding Danyu Guo Anqian Hu Xianfeng Yang Kui Shen Liyu Chen Yingwei Li School of Chemistry and Chemical Engineering South China University of TechnologyGuangzhou 510640China Analytical and Testing Centre South China University of TechnologyGuangzhou 510640China South China University of Technology-Zhuhai Institute of Modern Industrial Innovation Zhuhai 519175China

The preparation of supported high-density metal nanoparticles(NPs)is of great importance to boost the performance in heterogeneous catalysis.Thermal transformation of metal-organic frameworks(MOFs)has been demonstrated as a promising route for the synthesis of supported metal NPs with high metal loadings,but it is challenge to achieve uniform metal dispersion.Here we report a strategy of“spatial isolation and dopant anchoring”to resist metal aggregation in the pyrolysis of MOFs through converting a bulk MOF into dual-heteroatom-containing flower-like MOF sheets(B/N-MOF-S).This approach can spatially isolate metal ions and increase the number of anchoring sites,thus efficiently building physical and/or chemical barriers to cooperatively prevent metal NPs from aggregation in the high-temperature transformation process.After thermolysis at 1,000℃,the B/N-MOFS affords B,N co-doped carbon-supported Co NPs(Co/BNC)with uniform dispersion and a high Co loading of 37.3 wt.%,while untreated bulk MOFs yield much larger sizes and uneven distribution of Co NPs.The as-obtained Co/BNC exhibits excellent electrocatalytic activities in both hydrogen evolution and hydrazine oxidation reactions,only a voltage of 0.617 V at a high current density of 100 mA·cm^(−2)is required when applied to a two-electrode overall hydrazine splitting electrolyzer.

关键词： electrocatalysis metal-organic frameworks metal nanoparticles overall hydrazine splitting thermal transformation

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