催化作用
化学
氨硼烷
氢
煅烧
电子转移
金属
碳纤维
化学工程
制氢
光化学
有机化学
复合数
材料科学
工程类
复合材料
作者
Wenyao Chen,Shuangming Chen,Gang Qian,Song Li,De Chen,Xin Zhou,Xuezhi Duan
标识
DOI:10.1016/j.jcat.2020.06.028
摘要
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 (nEWG/nEDG) 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., H2 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.
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