石墨烯
密度泛函理论
催化作用
化学物理
吸附
材料科学
Atom(片上系统)
活动站点
吸收光谱法
氧气
基质(水族馆)
结晶学
纳米技术
化学
计算化学
物理化学
物理
光学
计算机科学
嵌入式系统
地质学
海洋学
有机化学
生物化学
作者
Guang Han,Xue Zhang,Wei Liu,Qinghua Zhang,Zhiqiang Wang,Jun Cheng,Takeshi Yao,Lin Gu,Chunyu Du,Yunzhi Gao,Geping Yin
标识
DOI:10.1038/s41467-021-26747-1
摘要
Single-atom catalysts are becoming increasingly significant to numerous energy conversion reactions. However, their rational design and construction remain quite challenging due to the poorly understood structure-function relationship. Here we demonstrate the dynamic behavior of CuN2C2 site during operando oxygen reduction reaction, revealing a substrate-strain tuned geometry distortion of active sites and its correlation with the activity. Our best CuN2C2 site, on carbon nanotube with 8 nm diameter, delivers a sixfold activity promotion relative to graphene. Density functional theory and X-ray absorption spectroscopy reveal that reasonable substrate strain allows the optimized distortion, where Cu bonds strongly with the oxygen species while maintaining intimate coordination with C/N atoms. The optimized distortion facilitates the electron transfer from Cu to the adsorbed O, greatly boosting the oxygen reduction activity. This work uncovers the structure-function relationship of single-atom catalysts in terms of carbon substrate, and provides guidance to their future design and activity promotion.
科研通智能强力驱动
Strongly Powered by AbleSci AI