催化作用
单线态氧
化学
选择性
氮化硼
吸附
光化学
分解
氧气
硼
无机化学
有机化学
作者
Jianzheng Zhen,Jiahao Sun,Xiangwei Xu,Zenglong Wu,Wenkai Song,Ying Yu,Septimus H. Liang,Lingshan Miao,Jiazhen Cao,Weiyang Lv,Changsheng Song,Yingming Yao,Mingyang Xing
标识
DOI:10.1002/anie.202402669
摘要
Singlet oxygen (1O2) is an essential reactive species responsible for selective oxidation of organic matter, especially in Fenton‐like processes. However, due to the great limitations in synthesizing catalysts with well‐defined active sites, the controllable production and practical application of 1O2 remain challenging. Herein, guided by theoretical simulations, a series of boron nitride‐based single‐atom catalysts (BvBN/M, M = Co, Fe, Cu, Ni and Mn) were synthesized to regulate 1O2 generation by activating peroxymonosulfate (PMS). All the fabricated BvBN/M catalysts with explicit M‐N3 sites promoted the self‐decomposition of the two PMS molecules to generate 1O2 with high selectivity, where BvBN/Co possessed moderate adsorption energy and d‐band center exhibited superior catalytic activity. As an outcome, the BvBN/Co‐PMS system coupled with membrane filtration technology could continuously transform aromatic alcohols to aldehydes with nearly 100% selectivity and conversion rate under mild conditions, suggesting the potential of this novel catalytic system for green organic synthesis.
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