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Activation of oxygen on oxygenated boron nitride: the proof of quasi-MvK mechanism on a nonmetal catalyst
Hao Yang, Yushu Xie, Libin Zeng, Wandong Xing, Rui Xiong*, Yidong Hou, Jimmy C. Yu, Can Yang*
https://doi.org/10.1016/j.cjsc.2026.101041
Oxygen activation; Quasi-MvK mechanism; Non-metallic BON; H2S-ODH
ABSTRACT
Oxygen activation is a critical step in heterogeneous aerobic oxidation processes. Although conventional metal-based catalysts are effective for oxygen activation, they are often vulnerable to sulfur poisoning, which limits their practical applications. A sensible solution is to develop a stable non-metallic catalyst with a sufficient number of active sites for oxygen activation. Herein, we report the synthesis of an oxygenated boron nitride (BON) ceramic featuring a high concentration of oxygen species incorporated into its framework. The resulting metal-free BON catalyst exhibits excellent performance in the selective oxidative dehydrogenation of hydrogen sulfide (H2S-ODH). The reaction mechanisms, particular the roles of proton transfer and oxygen activation on BON, was systematically investigated, and a quasi-Mars-Van Krevelen (quasi-MvK) mechanism is proposed. The results reveal that the lattice oxygen species (O-O species) in BON possess an excellent affinity for protons and readily accepts hydrogen from H2S, generating oxygen vacancies on the BON surface. These vacancies subsequently facilitate the activation of oxygen molecules. As a result, the BON catalyst achieves high H2S conversion, excellent sulfur selectivity (above 90%), and outstanding long-term stability over 200 h of continuous operation. This proton-transfer-assisted oxygen activation strategy provides new insights into the design of efficient metal-free catalysts for aerobic oxidation reactions.
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CN 35–1112/TQ, ISSN 0254–5861, Online ISSN: 2949-768X Copyright @ 2022 Chinese Journal of Structural Chemistry-www.Chinese Journal of Structural Chemistry.net. All Rights Reserved 闽ICP备2022002645号-1