Synergistic effect of Pd single atoms and clusters on the de/re-hydrogenation performance of MgH2

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外文摘要：Hydrogen storage plays a pivotal role in the hydrogen industry,yet its current status presents a bottle-neck.Diverse strategies have emerged in recent years to address this challenge.MgH2 has stood out as a promising solid-state hydrogen storage material due to its impressive gravimetric and volumetric hy-drogen density,but its practical application is hampered by elevated thermal stability and sluggish kinet-ics.In this study,we introduce a solution by synthesizing Pd metallene through a one-pot solvothermal method,revealing a distinctive highly curved lamellar structure with a thickness of around 1.6 nm.Incor-porating this Pd metallene into MgH2 results in a composite system wherein the starting dehydrogenation temperature is significantly lowered to 439 K and complete dehydrogenation occurs at 583 K,releasing 6.14 wt.％hydrogen.The activation energy of dehydrogenation for MgH2 was reduced from 170.4 kJ mol-1 to 79.85 kJ mol-1 after Pd metallene decoration.The enthalpy of dehydrogenation of the MgH2-10 wt.％Pd sample was calculated to be 73 kJ mol-1 H2-1 and decreased by 4.4 kJ mol-1 H2-1 from that of dehy-drogenation of pure MgH2(77.4 kJ mol-1 H2-1).Theoretical calculations show that the average formation energy and average adsorption energy of hydrogen vacancies can be significantly reduced in the presence of both Pd clusters and Pd single atoms on the surface of MgH2/Mg,respectively.It suggests that the synergistic effect of in situ formed Pd single atoms and clusters significantly improves the hydrogenation and dehydrogenation kinetics.The identified active sites in this study hold potential as references for forthcoming multi-sized active site catalysts,underscoring a significant advancement toward resolving hydrogen storage limitations.

外文关键词：

MgH2MetalleneSingle atomsClustersHydrogen storage

作者：

Nuo Xu、Haoran Zhou、Mingqiang Zhang、Yuchuan Ye、Kaiwen Wang、Yingtang Zhou、Yunfeng Zhu、Yao Zhang

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作者单位：

School of Materials Science and Engineering,Jiangsu Key Laboratory of Advanced Metallic Materials,Southeast University,Nanjing,211189,China

Zhejiang Key Laboratory of Petrochemical Environmental Pollution Control,National Engineering Research Center for Marine Aquaculture,Marine Science and Technology College,Zhejiang Ocean University,Zhoushan 316004,China

ICFO-Institut de Ciències Fotòniques,The Barcelona Institute of Science and Technology,Castelldefels(Barcelona)08860,Spain

Faculty of Materials and Manufacturing,Beijing University of Technology,Beijing 100124,China

College of Materials Science and Engineering,Jiangsu Collaborative Innovation Centre for Advanced Inorganic Function Composites,Nanjing Tech University,Nanjing 211816,China

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基金：

National Key R&D Program of ChinaNational Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaNatural Science Foundation of Jiangsu province,China

项目编号：

2023YFB4005402NSFC-NSAF U233011152071177BK20221473

出版年：

2024

DOI：

10.1016/j.jmst.2024.01.009

材料科学技术(英文版)

中国金属学会中国材料研究学会中国科学院金属研究所

材料科学技术(英文版)

CSTPCD

影响因子：0.657

ISSN：1005-0302

年,卷(期)：2024.191(24)