<?xml version="1.0" encoding="UTF-8"?><xml><records><record><source-app name="Biblio" version="7.x">Drupal-Biblio</source-app><ref-type>17</ref-type><contributors><authors><author><style face="normal" font="default" size="100%">Zelin Wu</style></author><author><style face="normal" font="default" size="100%">Bingkun Huang</style></author><author><style face="normal" font="default" size="100%">Xinhao Wang</style></author><author><style face="normal" font="default" size="100%">He, Chuan-Shu</style></author><author><style face="normal" font="default" size="100%">Yang Liu</style></author><author><style face="normal" font="default" size="100%">Du, Ye</style></author><author><style face="normal" font="default" size="100%">Liu, Wen</style></author><author><style face="normal" font="default" size="100%">Zhaokun Xiong</style></author><author><style face="normal" font="default" size="100%">Bo Lai</style></author></authors></contributors><titles><title><style face="normal" font="default" size="100%">Facilely Tuning the First-Shell Coordination Microenvironment in Iron Single-Atom for Fenton-like Chemistry toward Highly Efficient Wastewater Purification</style></title><secondary-title><style face="normal" font="default" size="100%">Environmental Science &amp;amp; Technology</style></secondary-title></titles><dates><year><style  face="normal" font="default" size="100%">2023</style></year></dates><urls><web-urls><url><style face="normal" font="default" size="100%">https://doi.org/10.1021/acs.est.3c04343</style></url></web-urls></urls><number><style face="normal" font="default" size="100%">37</style></number><volume><style face="normal" font="default" size="100%">57</style></volume><pages><style face="normal" font="default" size="100%">14046-14057</style></pages><language><style face="normal" font="default" size="100%">eng</style></language><abstract><style face="normal" font="default" size="100%">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.</style></abstract><notes><style face="normal" font="default" size="100%">PMID: 37658810</style></notes></record></records></xml>