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Pt Catalysts Supported on H2 and O2 Plasma-Treated Al2O3 for Hydrogenation and Dehydrogenation of the Liquid Organic Hydrogen Carrier Pair Dibenzyltoluene and Perhydrodibenzyltoluene
ACS Catalysis ( IF 12.9 ) Pub Date : 2020-08-24 , DOI: 10.1021/acscatal.0c03091
Libin Shi 1, 2 , Yiming Zhou 1 , Suitao Qi 1 , Kevin J. Smith 2 , Xiao Tan 1 , Jiawei Yan 1 , Chunhai Yi 1
Affiliation  

Dibenzyltoluene (DBT) is a promising liquid organic hydrogen carrier (LOHC) with theoretical 6.2 wt % hydrogen storage capacity which can be coupled with a renewable energy power generation system. In this work, the surface hydroxyl groups and surface oxygen vacancies (SOVs) on alumina were modified by a convenient and environmentally friendly plasma treatment method. Different Pt/Al2O3 catalysts were prepared via impregnation of the treated alumina, and the effects of different surface hydroxyl groups and SOVs on their reactivity for the reversible hydrogenation and dehydrogenation of DBT were investigated. The results show that SOVs increased after H2 plasma treatment, whereas the surface hydroxyl groups increased and SOVs decreased after O2 plasma treatment. Both the surface hydroxyl group and SOV can improve Pt metal dispersion. The more interesting observation is that the hydroxyl groups promote hydrogen spillover and the proportion of Pt(0), which not only benefit the catalyst hydrogenation and dehydrogenation activity but also reduce side reactions and increase long-term cycle performance. However, increased SOVs increased the fraction of low coordinated Pt which reduces the long-term cycle performance of the catalyst. As a result, increasing surface hydroxyl groups and appropriately reducing SOVs on Pt/Al2O3 are propitious for improving both reactivity and long-term cycle performance when using DBT as a LOHC.

中文翻译:

H 2和O 2等离子处理的Al 2 O 3上负载的Pt催化剂,用于液态有机氢载体对二苄基甲苯和全氢二苄基甲苯的加氢和脱氢

二苄基甲苯(DBT)是一种有前途的液态有机氢载体(LOHC),理论储氢量为6.2 wt%,可与可再生能源发电系统结合使用。在这项工作中,氧化铝上的表面羟基和表面氧空位(SOV)通过一种方便且环保的等离子体处理方法进行了改性。通过浸渍处理过的氧化铝制备了不同的Pt / Al 2 O 3催化剂,研究了不同的表面羟基和SOV对DBT可逆加氢和脱氢反应活性的影响。结果表明,H 2等离子体处理后SOV增加,而O 2处理后表面羟基增加而SOV减少等离子处理。表面羟基和SOV均可改善Pt金属的分散性。更有趣的观察是,羟基促进了氢的溢出和Pt(0)的比例,这不仅有利于催化剂的氢化和脱氢活性,而且还减少了副反应并提高了长期循环性能。但是,增加的SOV增加了低配位Pt的比例,从而降低了催化剂的长期循环性能。结果,当使用DBT作为LOHC时,增加表面羟基和适当降低Pt / Al 2 O 3上的SOV有利于改善反应性和长期循环性能。
更新日期:2020-09-20
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