On the nature of Pt-carbon interactions for enhanced hydrogen generation
On the nature of Pt-carbon interactions for enhanced hydrogen generation
复制标题
关于增强氢生成的 Pt-碳相互作用的性质
DOI：
10.1016/j.jcat.2020.06.028
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发表时间：
2020-09-01
影响因子：
7.3
通讯作者：
Duan, Xuezhi
中科院分区：
文献类型：
--
作者：
Chen, Wenyao;Chen, Shuangming;Duan, Xuezhi
Understanding the metal-support interactions in heterogeneous catalysis is critical yet complicated to tailor-design the catalysts with desirable properties. Exemplified with Pt-catalyzed ammonia borane (AB) hydrolysis, a dramatic increase of 20 folds in the catalytic activity is achieved by engineering the Pt-carbon interactions via adopting four different carbon materials (AC, CNT, f-CNF and p-CNF) as the catalyst supports. Multiple characterization techniques reveal that the Pt-carbon electronic interactions, including electron transfer and interfacial bonding, are deemed to be mainly responsible for the remarkable enhancement in the hydrogen generation rate. The molar ratio of electron-withdrawing group to electron-donating group (n(EWG)/n(EDG)) is further identified as a descriptor of catalyst in terms of Pt binding energy, which exhibits an almost linear relationship with the catalytic activity. Moreover, a comparison of Pt catalyst pre-treatments, i.e., H-2 and AB reduction as well as Ar calcination, suggests that the Pt-O-C linkages within the Pt-carbon interactions are highly stable yet inferior to this reaction. As a result, combining the merits of the highest Pt binding energy as well as the minimum Pt-O-C linkages, the Pt/p-CNF delivers the highest catalytic activity. The insights presented here could shed new lights on the nature of Pt-carbon interactions, which could be extended to the design and manipulation of other metal-carbon catalysts. (C) 2020 Elsevier Inc. All rights reserved.
