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Polar O-Co-P Surface for Bimolecular Activation in Catalytic Hydrogen Generation

Energy & Environmental Materials 2023年第1期6卷 224-233页

作者： Huanhuan Zhang Ke Zhang Saima Ashraf Yanping Fan Shuyan Guan Xianli Wu Yushan Liu Baozhong Liu Baojun Li Research Center of Green Catalysis College of ChemistryZhengzhou University100 Science RoadZhengzhou 450001China College of Chemistry and Chemical Engineering Henan Polytechnic University2001 Century AvenueJiaozuo 454000China

Boron hydrides release an abundant amount of hydrogen in the presence of a suitable *** bimolecular activation kinetics is the key to designing cost-effective catalysts for borohydride *** this study,the bimolecular activation of a polar O-Co-P site demonstrated superior hydrogen-generation kinetics(turnover frequency,TOF=37 min−1,298 K)and low activation energy(41.0 kJ mol^(−1))close to that of noble-metal-based *** a combination of experiments and theoretical calculations,it was revealed that the activated dangling oxygen atom in the Co–O precursor effectively replaced via surface-phosphorization because of strong electronic interactions between the dangling oxygen and P *** substitution modulated the local coordination environment and electronegativity around the surface Co sites and formed a new polar O-Co-P active site for optimizing the activation kinetics of ammonia borane and *** strategy based on bimolecular activation may create new avenues in the field of catalysis.

关键词： bimolecular activation borohydride hydrolysis hydrogen generation noble-metal-free catalysts polar site

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Coupling atom ensemble and electron transfer in PdCu for superior catalytic kinetics in hydrogen generation

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Nano Research 2023年第7期16卷 9012-9021页

作者： Xinru Zhao Yanyan Liu Huiyu Yuan Hao Wen Huanhuan Zhang Saima Ashraf Shuyan Guan Tao Liu Sehrish Mehdi Ruofan Shen Xianji Guo Yanping Fan Baozhong Liu Baojun Li College of Chemistry and Chemical Engineering Henan Polytechnic UniversityJiaozuo 454000China College of Science Henan Agriculture UniversityZhengzhou 450002China College of Materials Science and Engineering Zhengzhou UniversityZhengzhou 450001China Research Center of Green Catalysis College of ChemistryCollege of Mechanical and Power EngineeringZhengzhou UniversityZhengzhou 450001China CAS Key Laboratory for Biomedical Effects of Nanomaterials and Nanosafety National Centre for Nanoscience and TechnologyBeijing 100190China State Collaborative Innovation Center of Coal Work Safety and Clean-efficiency Utilization Jiaozuo 454003China Department of Chemistry Tsinghua UniversityBeijing 100084China

The design of high-performance catalysts is the key to the efficient utilization of hydrogen *** this work,a PdCu nanoalloy was successfully anchored on TiO_(2)encapsulated with carbon to construct a *** kinetics of the hydrolysis of ammonia borane(turnover frequency of 279 mol·min^(-1·)mol_(Pd)^(-1))ranking the third place among Pd-based catalysts was achieved in the absence of *** experimental research and theoretical calculations reveal a lower activation energy of the B-H bond on the PdCu nanoalloy catalyst than that on pristine Pd and a lower activation energy of the O-H bond than that on pristine *** redistribution of d electron and the shift of the d-band center play a critical role in increasing the electron density of Pd and improving the catalytic performances of Pd_(0.1)Cu_(0.9)/TiO_(2)-porous carbon(Pd_(0.1)Cu_(0.9)/T-PC).This work provides novel insights into highly dual-active alloys and sheds light on the mechanism of dual-active sites in promoting borohydride hydrolysis.

关键词： PdCu nanoalloy d-band holes ensemble effect borohydride hydrolysis dual-active sites

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