Atom(片上系统)
调制(音乐)
化学
电子结构
结晶学
材料科学
计算化学
物理
计算机科学
嵌入式系统
声学
作者
Yuhan Long,Zhenhua Cao,Wei-Ran Wu,Wenhao Liu,Peizhen Yang,Xuesong Zhan,Rongzhi Chen,Dongfang Liu,Wenli Huang
标识
DOI:10.1016/j.apcatb.2023.123643
摘要
The important role of optimizing the coordination environment of single-atom catalysts (SACs) for selective production of singlet oxygen (1O2) in Fenton-like reactions is revealed. Herein, we introduce electron-depletion boron atoms to manipulate the coordination number and atom types of Fe site simultaneously and construct a six-coordination Fe-N2B4 catalyst for peroxymonosulfte (PMS) activation. Particularly, it achieves 98.68% 1O2 generation selectivity superior to unregulated Fe-N4 catalyst (64.57%), exhibiting an exceptional bisphenol A (BPA) degradation performance with a reaction rate constant of 0.249 min−1. Experimental and theoretical results unveil that the tailored electronic structure of Fe not only enhances the adsorption selectivity of terminal oxygen atoms in PMS and alters the reaction pathway preference, but also facilitates the electron donation from PMS and lowers the energy barrier for 1O2 generation. This work provides a universal strategy for rational and precise modulation of SACs for specific reactive species conversion in environment remediation.
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