文献类型：期刊文献

英文题名：Interlayer Structure Manipulation of Iron Oxychloride by Potassium Cation Intercalation to Steer H2O2 Activation Pathway

作者：Wang, Jinling[1,2];Hou, Kai-Peng[3];Wen, Yuzhen[1,4];Liu, Honglai[2];Wang, Hualin[1];Chakarawet, Khetpakorn[3,5];Gong, Ming[6,7];Yang, Xuejing[1,2]

机构：[1]East China Univ Sci & Technol, Natl Engn Lab Ind Wastewater Treatment, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[3]Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA;[4]Shanghai Vico Precis Mold & Plast Co Ltd, Shanghai 200231, Peoples R China;[5]Univ Calif Davis, Dept Chem, Davis, CA 95695 USA;[6]Fudan Univ, Dept Chem, Shanghai 200438, Peoples R China;[7]Fudan Univ, Shanghai Key Lab Mol Catalysis & Innovat Mat, Shanghai 200438, Peoples R China

年份：2022

卷号：144

期号：10

起止页码：4294

外文期刊名：JOURNAL OF THE AMERICAN CHEMICAL SOCIETY

收录：;EI(收录号：20220711632997);WOS:【SCI-EXPANDED(收录号:WOS:000776234200002)】；

基金：The authors are grateful for the support from the National Key Projects for Fundamental Research and Development of China (2019YFC1906700) and the National Natural Science Foundation of China (21876049, 91834301). We thank Prof. Christopher J. Chang (University of California, Berkeley) for the use of Mossbauer spectrometer, Prof. Mian Guo (Wuhan University) and Dr. Benjamin Snyder (University of California, Berkeley) for the helpful comments during the preparation of this paper, and Shiyanjia Lab (www.shiyanjia.com) for the support of XPS test.

语种：英文

外文关键词：Scaffolds - Potassium hydroxide - Catalytic oxidation - Energy utilization - Positive ions - Catalysis - Organic pollutants - Reaction kinetics

摘要：Structural regulation of the active centers is often pivotal in controlling the catalytic functions, especially in iron-based oxidation systems. Here, we discovered a significantly altered catalytic oxidation pathway via a simple cation intercalation into a layered iron oxychloride (FeOCl) scaffold. Upon intercalation of FeOCl with potassium iodide (KI), a new stable phase of K+-intercalated FeOCl (K-FeOCl) was formed with slided layers, distorted coordination, and formed high-spin Fe(II) species compared to the pristine FeOCl precursor. This structural manipulation steers the catalytic H2O2 activation from a traditional Fenton-like pathway on FeOCl to a nonradical ferryl (Fe(IV)=O) pathway. Consequently, the K-FeOCl catalyst can efficiently remove various organic pollutants with almost 2 orders of magnitude faster reaction kinetics than other Fe-based materials via an oxidative coupling or polymerization pathway. A reaction-filtration coupled process based on K-FeOCl was finally demonstrated and could potentially reduce the energy consumption by almost 50%, holding great promise in sustainable pollutant removal technologies.