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Heterostructuring 2D Co_(2)P nanosheets with 0D CoP via a saltassisted strategy for boosting hydrogen evolution from ammonia borane hydrolysis

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Nano Research 2023年第5期16卷 6260-6269页

作者： Chao Wan Xiaoling Liu Jiapei Wang Fengqiu Chen Dang-Guo Cheng Zhejiang Provincial Key Laboratory of Advanced Chemical Engineering Manufacture Technology College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310027China Institute of Zhejiang University-Quzhou Quzhou 324000China School of Chemistry and Chemical Engineering Anhui University of TechnologyMa’anshan 243002China

ammonia borane(NH3BH3,AB)holds promise for chemical storage of hydrogen.However,designing superb and low-cost photocatalyst to drive hydrogen evolution from AB under visible light irradiation is highly desirable but remains a major challenge for promoting the practical utilization of AB.Herein,we demonstrated a heterostructure photocatalyst consisting of zerodimensional(0D)CoP nanoparticles immobilized on two-dimensional(2D)Co_(2)P nanosheets(CoP/Co_(2)Ps)as a high-performance and low-cost catalyst for hydrogen evolution from AB hydrolysis,in which 0D/2D heterostructure was synthesized using the saltinduced phase transformation strategy.Interestingly,the optimized CoP/Co_(2)Ps exhibit a robust H_(2) evolution rate of 32.1 L∙min^(−1)∙g_(Co)^(−1),corresponding to a turnover frequency(TOF)value of 64.1 min^(−1),being among the highest TOF for non-noblemetal catalysts ever reported,even outperforming some precious metal catalysts.This work not only opens a new avenue to accelerate hydrogen evolution from AB by regulating the electronic structures of heterointerfaces,but also provides a novel strategy for the construction of precious-metal-free materials for hydrogen-related energy catalysis in the future.

关键词： hydrogen storage ammonia borane hydrolysis heterostructure CoP/Co_(2)P nanosheets(CoP/Co_(2)Ps) hydrogen evolution

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Oxygen modified CoP2 supported palladium nanoparticles as highly efficient catalyst for hydrolysis of ammonia borane

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Nano Research 2022年第4期15卷 3034-3041页

作者： Leijie Zhang Jian Ye Yi Tu Qingyu Wang Haibin Pan Lihui Wu Xusheng Zheng Junfa Zhu National Synchrotron Radiation Laboratory Department of Chemical Physics and Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education InstitutesUniversity of Science and Technology of ChinaHefei 230029China School of Science Anhui Agricultural UniversityHefei 230036China

ammonia borane(AB)is regarded as a promising chemical hydrogen-storage material due to its high hydrogen content,nontoxicity,and long-term stability under ambient temperature.However,constructing advanced catalysts to further promote the hydrogen production still remains a challenge for the hydrolysis of AB.Herein,we report a novel oxygen modified CoP_(2)(O-CoP_(2))material with dispersed palladium nanoparticles(Pd NPs)as a highly efficient and sustainable catalyst for AB hydrolysis.The modification of oxygen could optimize the catalytic synergy effect between CoP_(2)and Pd NPs,achieving enhanced catalytic activity with a turnover frequency(TOF)number of 532 min^(-1)and an activation energy(E_(a))value of 16.79 kJ·mol^(-1).Meanwhile,reaction kinetic experiments prove that the activation of water is the rate-determining step(RDS).The water activation mechanism is revealed by quasi in-situ X-ray photoelectron spectroscopy(XPS)and in-situ X-ray absorption fine structure(XAFS)measurements.The activation of water leads to the production of-H and-OH groups,which are further adsorbed on the oxygen atoms in P-O bond and Pd atoms,respectively.In addition,density functional theory(DFT)calculations indicate that the introduced oxygen facilitates the adsorption and activation of water molecules.This novel modulation strategy successfully sheds new light on the development of advanced catalysts for hydrolysis of AB and beyond.

关键词： Pd-based catalysis ammonia borane hydrolysis water activation quasi in-situ X-ray photoelectron spectroscopy density functional theory(DFT)calculations

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