• 文献标题:   Bonding states of hydrogen for supported Ti clusters on pristine and defective graphene
  • 文献类型:   Article
  • 作  者:   MA LJ, HAN T, HAO ZC, WANG JF, JIA JF, WU HS
  • 作者关键词:   hydrogen adsorption, graphene supported ti cluster, metalsupport interaction, bonding state of hydrogen, hydrogen spillover
  • 出版物名称:   INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
  • ISSN:   0360-3199 EI 1879-3487
  • 通讯作者地址:  
  • 被引频次:   0
  • DOI:   10.1016/j.ijhydene.2022.12.351 EA APR 2023
  • 出版年:   2023

▎ 摘  要

To determine whether graphene-supported Ti clusters can synergistically store hydrogen through Kubas and spillover effect, we systematically investigate the growth pattern of Tin (n = 1-10) clusters on pristine and defective graphene and analyze multiple types of bonding states of hydrogen in detail. For pristine graphene, the most stable Tin (n = 1-10) clusters are the quasi-planar structure except for supported Ti4 and Ti5. The Ti dissociation energies and the binding energy of Tin clusters gradually increase with increasing n, which indicates that larger Tin clusters tend to form. Efficient spillover will occur on single-site Ti Catalysts at low hydrogen concentration due to the lower hydrogen spillover energy barrier (3.05 eV), while the energy barrier of hydrogen migration from Tin (n = 2-7) clusters to graphene on the cluster is 5.34-6.82 eV. The Ti: H ratio is a maximum of 1:8 for the singlesite Ti catalyst, while decreases with the Tin cluster increases. Therefore, the pristine graphene-supported Ti nanoclusters are more suitable as substrates for hydrogen adsorbent rather than spillover. The introduced defects make Tin clusters have threedimensional conical configurations from n = 4. Ti3 and Ti6 are the most stable clusters. Moreover, the migration energy barriers of H atoms on them decrease from 6.54 eV to 6.82 eV-4.32 eV and 3.42 eV, respectively. Our results explain recent experimental phenomena [Appl Phys Lett 2015; 106: 083,901. ACS Energy Lett 2022; 7 (7): 2297-2303] in depth at the molecular level. (c) 2022 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.