Heterogeneous Hydrogenation with Hydrogen Spillover Enabled by Nitrogen Vacancies on Boron Nitride‐Supported Pd Nanoparticles. (18th January 2023)

• Record Type: Journal Article
• Authors: Zhang, Yazhou; Zhan, Shaoqi; Liu, Kunlong; Qiao, Mengfei; Liu, Ning; Qin, Ruixuan; Xiao, Liangping; You, Pengyao; Jing, Wentong; Zheng, Nanfeng
• Is Part Of: Angewandte Chemie. Volume 135:Number 9(2023)
• Page Start: n/a
• Page End: n/a
• Publication Date: 2023-01-18
• Subjects: Boron Nitride -- Carbonyl Hydrogenation -- Hydrogen Spillover -- Nitrogen Vacancy -- Selective Hydrogenation; Chemistry -- Periodicals; 540
• DOI: 10.1002/ange.202217191
• Languages: English
• ISSNs: 0044-8249

Abstract

Abstract: Heterogeneous hydrogenation with hydrogen spillover has been demonstrated as an effective route to achieve high selectivity towards target products. More effort should be paid to understand the complicated correlation between the nature of supports and hydrogenation involving hydrogen spillover. Herein, we report the development of the hydrogenation system of hexagonal boron nitride (h‐BN)‐supported Pd nanoparticles for the hydrogenation of aldehydes/ketones to alcohols with hydrogen spillover. Nitrogen vacancies in h‐BN determine the feasibility of hydrogen spillover from Pd to h‐BN. The hydrogenation of aldehydes/ketones with hydrogen spillover from Pd proceeds on nitrogen vacancies on h‐BN. The weak adsorption of alcohols to h‐BN inhibits the deep hydrogenation of aldehydes/ketones, thus leading to high catalytic selectivity to alcohols. Moreover, the hydrogen spillover‐based hydrogenation mechanism makes the catalyst system exhibit a high tolerance to CO poisoning. Abstract : h‐BN containing abundant nitrogen vacancies is demonstrated as an effective support for Pd nanocatalysts to develop the capability for the hydrogenation of aldehydes/ketones to alcohols with hydrogen spillover. While nitrogen vacancies play a crucial role in the spillover of H atoms from Pd onto h‐BN, high selectivity to alcohols by hydrogen spillover is ascribed to the weak adsorption of alcohols to the hydrogenation sites (nitrogen vacancies).