卟啉
动力学
纳米片
光化学
氧化还原
材料科学
可见光谱
催化作用
化学动力学
化学工程
化学
纳米技术
光电子学
有机化学
工程类
物理
冶金
量子力学
作者
Qian Chen,Yue Zhang,En‐Ming You,Qiaorong Jiang,Xianjie Chen,Yu Wang,Zhijia Song,Kuan Chang,Zhaoxiong Xie,Qin Kuang
出处
期刊:Small
[Wiley]
日期:2022-11-06
卷期号:18 (51)
被引量:8
标识
DOI:10.1002/smll.202204924
摘要
Water oxidation is one of the most challenging steps in CO2 photoreduction, but its influence on CO2 photoreduction is still poorly understood. Herein, the concept of accelerating the water oxidation kinetics to promote the CO2 photoreduction is realized by incorporating supramolecular porphyrin nanosheets (NS) into the C3 N4 catalyst. As a prototype, porphyrin-C3 N4 based van der Waals heterojunctions with efficient charge separation are elaborately designed, in which the porphyrin and C3 N4 NS serve as the water oxidation booster and CO2 reduction center, respectively. Theoretical calculations and relevant experiments demonstrate that the added porphyrin NS reverses the rate-limiting step in the water oxidation while reducing its energy barrier, thus resulting in faster reaction kinetics. Therefore, the optimal sample shows excellent performance in visible-light-driven CO2 reduction with a maximum CO evolution rate of 16.8 µmol g-1 h-1 , which is 6.8 times that of the C3 N4 NS and reaches the current state of the art for C3 N4 -based materials in CO2 photoreduction. Overall, this work throws light that accelerating water oxidation kinetics can effectively improve the CO2 photoreduction efficiency.
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