Gao Zhe, Wang Guofu, Lei Tingyu, Lv Zhengxing, Xiong Mi, Wang Liancheng, Xing Shuangfeng, Ma Jingyuan, Jiang Zheng, Qin Yong
State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan, 030001, China.
Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences, Beijing, 100049, China.
Nat Commun. 2022 Jan 10;13(1):118. doi: 10.1038/s41467-021-27785-5.
The contribution of the reverse spillover effect to hydrogen generation reactions is still controversial. Herein, the promotion functions for reverse spillover in the ammonia borane hydrolysis reaction are proven by constructing a spatially separated NiO/AlO/Pt bicomponent catalyst via atomic layer deposition and performing in situ quick X-ray absorption near-edge structure (XANES) characterization. For the NiO/AlO/Pt catalyst, NiO and Pt nanoparticles are attached to the outer and inner surfaces of AlO nanotubes, respectively. In situ XANES results reveal that for ammonia borane hydrolysis, the H species generated at NiO sites spill across the support to the Pt sites reversely. The reverse spillover effects account for enhanced H generation rates for NiO/AlO/Pt. For the CoO/AlO/Pt and NiO/TiO/Pt catalysts, reverse spillover effects are also confirmed. We believe that an in-depth understanding of the reverse effects will be helpful to clarify the catalytic mechanisms and provide a guide for designing highly efficient catalysts for hydrogen generation reactions.
逆溢流效应在产氢反应中的贡献仍存在争议。在此，通过原子层沉积构建空间分离的NiO/AlO/Pt双组分催化剂并进行原位快速X射线吸收近边结构（XANES）表征，证实了逆溢流在氨硼烷水解反应中的促进作用。对于NiO/AlO/Pt催化剂，NiO和Pt纳米颗粒分别附着在AlO纳米管的外表面和内表面。原位XANES结果表明，对于氨硼烷水解，在NiO位点产生的H物种反向跨越载体扩散到Pt位点。逆溢流效应导致NiO/AlO/Pt的产氢速率提高。对于CoO/AlO/Pt和NiO/TiO/Pt催化剂，也证实了逆溢流效应。我们认为，深入了解这些逆向效应将有助于阐明催化机理，并为设计高效的产氢反应催化剂提供指导。
