反键分子轨道
活性氧
催化作用
析氧
氧气
材料科学
纳米技术
化学工程
分子内力
化学
光化学
原子轨道
立体化学
有机化学
电子
电极
生物化学
物理
物理化学
量子力学
工程类
电化学
作者
Dongya Li,Shiyu Zuo,Jinquan Wan,Yan Wang,Zeyu Guan,Zhicheng Yan,Fan Yang
标识
DOI:10.1016/j.apcatb.2023.122507
摘要
Reactive oxygen species (ROS) play important roles in environmental, chemical and biological fields, but the controlled release and migration of ROS remain a major challenge. Here, a highly efficient catalyst (Cu-MIL-101(Fe)) by modifying the electronic structure was designed. The orbital hybridization achieves a deep optimization of the d-band (d band center shifted from −1.01 eV to −1.32 eV), which reduces bonding and antibonding orbitals energy levels, thus promoting release of SO4·-. More importantly, the interfacial micro-electric field (IMEF) formed by the intramolecular charge offset mediates the directional migration of SO4·- from Fe sites to Cu sites. These properties endow the catalyst with high-efficiency SO4·- generation, rapid release, directional migration and utilization, with a 4.3-fold increase in effective oxidant utilization over Fe2+ (from 17.12% to 73.54%). This study highlights a catalytic strategy for efficient ROS generation, release, migration and utilization for a wide range of potential applications including environmental remediation.
科研通智能强力驱动
Strongly Powered by AbleSci AI