光催化
人工光合作用
材料科学
可见光谱
二氧化碳电化学还原
光化学
等离子体子
纳米颗粒
甲酸
催化作用
拉曼光谱
一氧化碳
吸附
纳米技术
等离子纳米粒子
化学工程
化学
光电子学
光学
物理化学
物理
工程类
生物化学
色谱法
作者
Gayatri Kumari,Xueqiang Zhang,Dinumol Devasia,Heo Jae-young,Prashant K. Jain
出处
期刊:ACS Nano
[American Chemical Society]
日期:2018-08-08
卷期号:12 (8): 8330-8340
被引量:145
标识
DOI:10.1021/acsnano.8b03617
摘要
Photocatalytic reduction of carbon dioxide (CO2) by visible light has the potential to mimic plant photosynthesis and facilitate the renewable production of storable fuels. Accomplishing desirable efficiency and selectivity in artificial photosynthesis requires an understanding of light-driven pathways on photocatalyst surfaces. Here, we probe with single-nanoparticle spatial resolution the dynamics of a plasmonic silver (Ag) photocatalyst under conditions of visible light-driven CO2 reduction. In situ surface-enhanced Raman spectroscopy captures discrete adsorbates and products formed dynamically on single photocatalytic nanoparticles, most prominent among which is a surface-adsorbed hydrocarboxyl (HOCO*) intermediate critical to further reduction of CO2 to carbon monoxide (CO) and formic acid (HCOOH). Density functional theory simulations of the captured adsorbates reveal the mechanism by which plasmonic excitation activates physisorbed CO2 leading to the formation of HOCO*, indicating close interplay between photoexcited states and adsorbate/metal interactions.
科研通智能强力驱动
Strongly Powered by AbleSci AI