聚合
污染物
中心(范畴论)
金属
材料科学
化学
纳米技术
化学工程
结晶学
聚合物
有机化学
冶金
工程类
作者
Hongzhi Liu,Xin Shu,Mao-Suan Huang,Bingbing Wu,Jie-Jie Chen,Xi‐Sheng Wang,LI Hui-lin,Han‐Qing Yu
标识
DOI:10.1038/s41467-024-46739-1
摘要
Abstract Polymerization-driven removal of pollutants in advanced oxidation processes (AOPs) offers a sustainable way for the simultaneous achievement of contamination abatement and resource recovery, supporting a low-carbon water purification approach. However, regulating such a process remains a great challenge due to the insufficient microscopic understanding of electronic structure-dependent reaction mechanisms. Herein, this work probes the origin of catalytic pollutant polymerization using a series of transition metal (Cu, Ni, Co, and Fe) single-atom catalysts and identifies the d -band center of active site as the key driver for polymerization transfer of pollutants. The high-valent metal-oxo species, produced via peroxymonosulfate activation, are found to trigger the pollutant removal via polymerization transfer. Phenoxyl radicals, identified by the innovative spin-trapping and quenching approaches, act as the key intermediate in the polymerization reactions. More importantly, the oxidation capacity of high-valent metal-oxo species can be facilely tuned by regulating their binding strength for peroxymonosulfate through d -band center modulation. A 100% polymerization transfer ratio is achieved by lowering the d -band center. This work presents a paradigm to dynamically modulate the electronic structure of high-valent metal-oxo species and optimize pollutant removal from wastewater via polymerization.
科研通智能强力驱动
Strongly Powered by AbleSci AI