乙基修饰的氮化碳增强光催化CO2转化

Ethyl-activated carbon nitride for efficient photocatalytic CO2 conversion

陈冻冻 ¹王中辽 ¹傅俊伟 ²张金锋 ¹代凯¹

扫码查看

作者信息

1. Key Laboratory of Green and Precise Synthetic Chemistry and Applications,Ministry of Education,Anhui Province Key Laboratory of Pollutant Sensitive Materials and Environmental Remediation,Huaibei Normal University,Huaibei 235000,China
2. School of Physics,Central South University,Changsha 410083,China
折叠

摘要

光催化剂的表面官能团对光生载体的转移和反应的活性位点起着关键作用,对光催化转化过程影响很大.因此,合理准确地调控表面基团可以极大地优化光催化性能.本文通过引入给电子能力强的乙基,对氮化碳(g-C3N4)未聚合的NH2基团进行优化.通过X射线光电子能谱证实了乙基包埋的成功.时间分辨光谱和密度泛函理论(DFT)计算证实了光生载流子沿有利方向变化.最后,Gibbs自由能表明,乙基改性的氮化碳具有显著降低的CO2转化为*COOH的能垒.其CO2到CO的转化率为47.08 μmol g-1 h-1.本研究为通过优化表面官能团来提高光催化剂性能的研究提供了可靠参考.

Abstract

Surface functional groups of photocatalysts play a key role in the transfer of photogenerated carriers and the active site of the reaction,which severely influence the pho-tocatalytic conversion process.Therefore,reasonable and ac-curate regulation of surface groups can greatly optimize photocatalytic performance.Herein,we performed optimiza-tion on the unpolymerized NH2 group of carbon nitride(g-C3N4)by introducing an ethyl group with a strong electron-donating ability to obtain the E-CN photocatalysts.X-ray photoelectron spectroscopy confirmed the successful embed-ding of the ethyl group.Time-resolved spectroscopy and density function theory calculations verified that the photo-generated carrier changes in a favorable direction.Finally,the Gibbs free energy showed that E-CN significantly decreases the energy barrier of CO2 conversion to*COOH.The results revealed that the conversion rate of CO2 to CO is 47.08 μmol g-1 h-1.This work offers a reliable reference to improve the performance of photocatalysts by optimizing their surface functional groups.

关键词

photocatalytic CO2 reduction/ethyl group/carbon nitride/charge separation

Key words

photocatalytic CO2 reduction/ethyl group/carbon nitride/charge separation

引用本文复制引用

基金项目

National Key R&D Program of China(2022YFE0126500)

National Natural Science Foundation of China(22278169)

National Natural Science Foundation of China(22150610467)

National Natural Science Foundation of China(52372253)

National Natural Science Foundation of China(51973078)

Excellent Scientific Research and Innovation Team of the Education Department of Anhui Province(2022AH010028)

Major projects of Education Department of Anhui Province(2022AH040068)

Key Foundation of Educational Commission of Anhui Province(2022AH050396)

Key Foundation of Educational Commission of Anhui Province(2022AH050376)

Anhui Provincial Quality Engineering Project(2022sx13)

Innovation Fund for Postgraduates of Huaibei Normal University(CX2023038)

Surplus Funds to Expand Research Projects of Huaibei Normal University(2023ZK045)

Open Project from the Key Laboratory of Green and Precise Synthetic Chemistry and Applications(2020KF07)

出版年

2024

中国科学:材料科学(英文)

CSTPCD

ISSN：

参考文献量68

段落导航