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易于构建的 Ru-CoO 莫特-肖特基催化剂,可有效促进氨硼烷脱氢生成氢气。

Facile construction of robust Ru-CoO Mott-Schottky catalyst enabling efficient dehydrogenation of ammonia borane for hydrogen generation.

机构信息

College of Materials Science and Engineering, Chongqing Jiaotong University, Chongqing 400074, China.

College of Materials Science and Engineering, Chongqing Jiaotong University, Chongqing 400074, China.

出版信息

J Colloid Interface Sci. 2023 Sep 15;646:25-33. doi: 10.1016/j.jcis.2023.04.181. Epub 2023 May 6.

Abstract

Developing efficient catalysts for the dehydrogenation of ammonia borane (AB) is important for the safe storage and controlled release of hydrogen, but it is a challenging task. In this study, we designed a robust Ru-CoO catalyst using the Mott-Schottky effect to induce favorable charge rearrangement. The self-created electron-rich CoO and electron-deficient Ru sites at heterointerfaces are indispensable for the activation of the B-H bond in NHBH and the OH bond in HO, respectively. The synergistic electronic interaction between the electron-rich CoO and electron-deficient Ru sites at the heterointerfaces resulted in an optimal Ru-CoO heterostructure that exhibited outstanding catalytic activity for the hydrolysis of AB in the presence of NaOH. The heterostructure had an extremely high hydrogen generation rate (HGR) of 12238 mL min g and an expected high turnover frequency (TOF) of 755 mol mol min at 298 K. The activation energy needed for the hydrolysis was low (36.65 kJ mol). This study opens up a new avenue for the rational design of high-performance catalysts for AB dehydrogenation based on the Mott-Schottky effect.

摘要

开发用于氨硼烷 (AB) 脱氢的高效催化剂对于安全储存和控制氢气释放非常重要,但这是一项具有挑战性的任务。在这项研究中,我们设计了一种使用 Mott-Schottky 效应诱导有利电荷重排的坚固 Ru-CoO 催化剂。在异质界面处自生成的富电子 CoO 和缺电子 Ru 位点对于 NHBH 中的 B-H 键和 HO 中的 OH 键的活化是必不可少的。富电子 CoO 和异质界面处的缺电子 Ru 位点之间的协同电子相互作用导致形成了具有优异催化活性的最佳 Ru-CoO 异质结构,该结构在存在 NaOH 的情况下对 AB 的水解表现出出色的催化活性。该异质结构具有极高的产氢率(HGR)为 12238 mL min g,在 298 K 时预计高的周转频率(TOF)为 755 mol mol min。水解所需的活化能较低(36.65 kJ mol)。这项研究为基于 Mott-Schottky 效应的 AB 脱氢高性能催化剂的合理设计开辟了新途径。

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