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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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