化学
合作性
氧化还原
反应性(心理学)
配体(生物化学)
非无辜配体
光化学
催化作用
单线态氧
组合化学
氧气
无机化学
有机化学
受体
医学
替代医学
病理
生物化学
作者
Sung Gyu Kim,Dong‐Young Kim,Joo Yeon Oh,Yeong Jun Son,Sangmin Jeong,Joonghan Kim,Seung Jun Hwang
摘要
The reduction of dioxygen to water is crucial in biology and energy technologies, but it is challenging due to the inertness of triplet oxygen and complex mechanisms. Nature leverages high-spin transition metal complexes for this, whereas main-group compounds with their singlet state and limited redox capabilities exhibit subdued reactivity. We present a novel phosphorus complex capable of four-electron dioxygen reduction, facilitated by unique phosphorus-ligand redox cooperativity. Spectroscopic and computational investigations attribute this cooperative reactivity to the unique electronic structure arising from the geometry of the phosphorus complex bestowed by the ligand. Mechanistic study via spectroscopic and kinetic experiments revealed the involvement of elusive phosphorus intermediates resembling those in metalloenzymes. Our result highlights the multielectron reactivity of phosphorus compound emerging from a carefully designed ligand platform with redox cooperativity. We anticipate that the work described expands the strategies in developing main-group catalytic reactions, especially in small molecule fixations demanding multielectron redox processes.
科研通智能强力驱动
Strongly Powered by AbleSci AI