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-C_(3)N_(4))未聚合的NH_(2)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CO_(2)转化为*COOH的能垒.其CO_(2)到CO的转化率为47.08μmolg^(-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.
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 photocatalytic conversion process.Therefore,reasonable and accurate regulation of surface groups can greatly optimize photocatalytic performance.Herein,we performed optimization on the unpolymerized NH_(2)group of carbon nitride(g-C3N4)by introducing an ethyl group with a strong electrondonating ability to obtain the E-CN photocatalysts.X-ray photoelectron spectroscopy confirmed the successful embedding of the ethyl group.Time-resolved spectroscopy and density function theory calculations verified that the photogenerated carrier changes in a favorable direction.Finally,the Gibbs free energy showed that E-CN significantly decreases the energy barrier of CO_(2)conversion to*COOH.The results revealed that the conversion rate of CO_(2)to CO is 47.08μmol g^(−1)h^(−1).This work offers a reliable reference to improve the performance of photocatalysts by optimizing their surface functional groups.
作者
陈冻冻
王中辽
傅俊伟
张金锋
代凯
Dongdong Chen;Zhongliao Wang;Junwei Fu;Jinfeng Zhang;Kai Dai(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;School of Physics,Central South University,Changsha 410083,China)
基金
supported by the National Key R&D Program of China(2022YFE0126500)
the National Natural Science Foundation of China(22278169,22150610467,52372253,51973078)
the Excellent Scientific Research and Innovation Team of the Education Department of Anhui Province(2022AH010028)
the Major projects of Education Department of Anhui Province(2022AH040068)
the Key Foundation of Educational Commission of Anhui Province(2022AH050396,2022AH050376)
Anhui Provincial Quality Engineering Project(2022sx13)
the Innovation Fund for Postgraduates of Huaibei Normal University(CX2023038)
Surplus Funds to Expand Research Projects of Huaibei Normal University(2023ZK045)
the Open Project from the Key Laboratory of Green and Precise Synthetic Chemistry and Applications(2020KF07)。
