Nature Communications ( IF 14.7 ) Pub Date : 2022-10-14 , DOI: 10.1038/s41467-022-33757-0 Hong-Chao Li 1, 2 , Qiang Wan 3 , Congcong Du 1, 2 , Jiafei Zhao 1, 2 , Fumin Li 1, 2 , Ying Zhang 1, 2 , Yanping Zheng 1 , Mingshu Chen 1 , Kelvin H L Zhang 1, 2 , Jianyu Huang 4 , Gang Fu 1, 2 , Sen Lin 3 , Xiaoqing Huang 1, 2 , Haifeng Xiong 1, 2
Hydrogen peroxide (H2O2) has the wide range of applications in industry and living life. However, the development of the efficient heterogeneous catalyst in the direct H2O2 synthesis (DHS) from H2 and O2 remains a formidable challenge because of the low H2O2 producibility. Herein, we develop a two-step approach to prepare PdSn nanowire catalysts, which comprises Pd oxide layered on PdSn nanowires (PdL/PdSn-NW). The PdL/PdSn-NW displays superior reactivity in the DHS at zero Celcius, presenting the H2O2 producibility of 528 mol kgcat−1·h−1 and H2O2 selectivity of >95%. A layer of Pd oxide on the PdSn nanowire generates bi-coordinated Pd, leading to the different adsorption behaviors of O2, H2 and H2O2 on the PdL/PdSn-NW. Furthermore, the weak adsorption of H2O2 on the PdL/PdSn-NW contributes to the low activation energy and high H2O2 producibility. This surface engineering approach, depositing metal layer on metal nanowires, provides a new insight in the rational designing of efficient catalyst for DHS.
中文翻译:
PdSn 纳米线上的层状 Pd 氧化物用于促进 H2O2 的直接合成
过氧化氢(H 2 O 2)在工业和生活中有着广泛的应用。然而,由于H 2 O 2 的低产率,在由H 2 和O 2 直接合成H 2 O 2 (DHS)中开发高效的多相催化剂仍然是一个巨大的挑战。在此,我们开发了一种两步法来制备 PdSn 纳米线催化剂,该催化剂包括在 PdSn 纳米线上的 Pd 氧化物(Pd L /PdSn-NW)。Pd L /PdSn-NW 在 DHS 中在零摄氏度下表现出优异的反应性,呈现出528 mol kg的 H 2 O 2产率cat -1 ·h -1和H 2 O 2选择性>95%。PdSn纳米线上的一层Pd氧化物产生双配位Pd,导致O 2、H 2和H 2 O 2在Pd L /PdSn-NW上的不同吸附行为。此外,H 2 O 2在 Pd L /PdSn-NW 上的弱吸附有助于低活化能和高 H 2 O 2产率。这种表面工程方法,在金属纳米线上沉积金属层,为合理设计用于 DHS 的高效催化剂提供了新的见解。