催化作用
化学
协调数
Atom(片上系统)
配位复合体
催化效率
纳米技术
化学工程
离子
材料科学
有机化学
金属
计算机科学
嵌入式系统
工程类
作者
Zelin Wu,Bingkun Huang,Sheng Wang,Chuan-Shu He,Yang Liu,Ye Du,Wen Liu,Zhaokun Xiong,Bo Lai
标识
DOI:10.1021/acs.est.3c04343
摘要
Precisely identifying the atomic structures in single-atom sites and establishing authentic structure-activity relationships for single-atom catalyst (SAC) coordination are significant challenges. Here, theoretical calculations first predicted the underlying catalytic activity of Fe-NxC4-x sites with diverse first-shell coordination environments. Substituting N with C to coordinate with the central Fe atom induces an inferior Fenton-like catalytic efficiency. Then, Fe-SACs carrying three configurations (Fe-N2C2, Fe-N3C1, and Fe-N4) fabricate facilely and demonstrate that optimized coordination environments of Fe-NxC4-x significantly promote the Fenton-like catalytic activity. Specifically, the reaction rate constant increases from 0.064 to 0.318 min-1 as the coordination number of Fe-N increases from 2 to 4, slightly influencing the nonradical reaction mechanism dominated by 1O2. In-depth theoretical calculations unveil that the modulated coordination environments of Fe-SACs from Fe-N2C2 to Fe-N4 optimize the d-band electronic structures and regulate the binding strength of peroxymonosulfate on Fe-NxC4-x sites, resulting in a reduced energy barrier and enhanced Fenton-like catalytic activity. The catalytic stability and the actual hospital sewage treatment capacity also showed strong coordination dependency. This strategy of local coordination engineering offers a vivid example of modulating SACs with well-regulated coordination environments, ultimately maximizing their catalytic efficiency.
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