@article {doi:10.1021/acs.est.3c04343,
	title = {Facilely Tuning the First-Shell Coordination Microenvironment in Iron Single-Atom for Fenton-like Chemistry toward Highly Efficient Wastewater Purification},
	journal = {Environmental Science \&amp; Technology},
	volume = {57},
	number = {37},
	year = {2023},
	note = {PMID: 37658810},
	pages = {14046-14057},
	abstract = {Precisely identifying the atomic structures in single-atom sites and establishing authentic structure{\textendash}activity relationships for single-atom catalyst (SAC) coordination are significant challenges. Here, theoretical calculations first predicted the underlying catalytic activity of Fe{\textendash}NxC4{\textendash}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{\textendash}N2C2, Fe{\textendash}N3C1, and Fe{\textendash}N4) fabricate facilely and demonstrate that optimized coordination environments of Fe{\textendash}NxC4{\textendash}x significantly promote the Fenton-like catalytic activity. Specifically, the reaction rate constant increases from 0.064 to 0.318 min{\textendash}1 as the coordination number of Fe{\textendash}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{\textendash}N2C2 to Fe{\textendash}N4 optimize the d-band electronic structures and regulate the binding strength of peroxymonosulfate on Fe{\textendash}NxC4{\textendash}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.},
	doi = {10.1021/acs.est.3c04343},
	url = {https://doi.org/10.1021/acs.est.3c04343},
	author = {Zelin Wu and Bingkun Huang and Xinhao Wang and He, Chuan-Shu and Yang Liu and Du, Ye and Liu, Wen and Zhaokun Xiong and Bo Lai}
}
