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On the nature of Pt-carbon interactions for enhanced hydrogen generation
Journal of Catalysis ( IF 7.3 ) Pub Date : 2020-07-02 , DOI: 10.1016/j.jcat.2020.06.028
Wenyao Chen , Shuangming Chen , Gang Qian , Li Song , De Chen , Xinggui Zhou , Xuezhi Duan

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.



中文翻译:

关于Pt碳相互作用增强氢生成的性质

了解多相催化中的金属-载体相互作用是至关重要的,但要定制设计具有所需性能的催化剂则很复杂。以Pt催化的氨硼烷(AB)水解为例,通过采用四种不同的碳材料(AC,CNT,f-CNF和p-CNF)来设计Pt-碳相互作用,从而使催化活性急剧提高了20倍。作为催化剂的载体。多种表征技术表明,Pt-碳电子相互作用(包括电子转移和界面键合)被认为是氢生成速率显着提高的主要原因。吸电子基团与给电子基团的摩尔比(n EWG / n EDG根据Pt结合能,其被进一步鉴定为催化剂的描述子,其与催化活性表现出几乎线性的关系。此外,对Pt催化剂预处理(即H 2和AB还原以及Ar煅烧)的比较表明,Pt-碳相互作用内的Pt-OC键非常稳定,但不如该反应。结果,Pt / p-CNF结合了最高的Pt结合能和最小的Pt-OC键的优点,提供了最高的催化活性。此处介绍的见解可以为Pt-碳相互作用的性质提供新的思路,可以扩展到其他金属-碳催化剂的设计和操作。

更新日期:2020-07-15
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