TY - JOUR
T1 - Modulating the Molecular Structure of Graphitic Carbon Nitride for Identifying the Impact of the Piezoelectric Effect on Photocatalytic H2O2 Production
AU - Wang, Penglei
AU - Fan, Shiying
AU - Li, Xinyong
AU - Duan, Jun
AU - Zhang, Dongke
N1 - Funding Information:
This work was financially supported by the National Natural Science Foundation of China (no. 22076018), the “Xing Liao Talents Program” Project (XLYC1902051), the Program of Introducing Talents of Discipline to Universities (B13012), the Fundamental Research Funds for the Central Universities (DUT19LAB10), the Key Laboratory of Industrial Ecology and Environmental Engineering, China Ministry of Education, the State Key Laboratory of Catalysis in DICP (N-20-06), and the Hong Kong Scholars Program (XJ2022006). Additionally, the authors acknowledge the assistance of the DUT Instrumental Analysis Center.
Publisher Copyright:
© 2023 American Chemical Society.
PY - 2023/7/21
Y1 - 2023/7/21
N2 - The use of the piezoelectric effect for regulating the separation and transportation of charge carriers in the artificial photosynthesis of H2O2 has been established as a promising approach. However, an in-depth and comprehensive understanding of the piezoelectric effect on photocatalysis is still far from satisfactory. Herein, we have accurately modulated the molecular structure of graphitic carbon nitride (CN) to investigate the effect of piezoelectricity on photocatalytic H2O2 production over CN. Our results show that the role of the piezoelectric effect in photocatalytic H2O2 production over CN strongly depends on the molecular structure of CN. Specifically, for CN, CN modified by phosphorus (CN-P), oxygen-functionalized CN (CN-OF), and cyano-group-grafted CN (CN-CA), the photocatalytic activity of CN, CN-P, and CN-OF is enhanced by approximately 1.40, 1.46, and 1.51 times due to the piezoelectric effect, respectively, while the photocatalytic activity of CN-CA is decreased by 6.0 times. To clarify and understand the key factors affecting piezo-photocatalysis activity, we employed density functional theory, photo-electrochemical measurements, and piezoresponse force microscopy measurements to explore active sites, piezoelectric polarization, and charge separation over molecular-functionalized CN. Our results reveal that the impact of the piezoelectric effect on photocatalytic H2O2 production over CN results from the comprehensive influence of multiple factors. This work not only demonstrates that the molecular structure of CN determines whether the piezoelectric effect improves photocatalytic H2O2 production over CN but also unveils the mechanism of the piezoelectric effect on photocatalytic H2O2 production over CN.
AB - The use of the piezoelectric effect for regulating the separation and transportation of charge carriers in the artificial photosynthesis of H2O2 has been established as a promising approach. However, an in-depth and comprehensive understanding of the piezoelectric effect on photocatalysis is still far from satisfactory. Herein, we have accurately modulated the molecular structure of graphitic carbon nitride (CN) to investigate the effect of piezoelectricity on photocatalytic H2O2 production over CN. Our results show that the role of the piezoelectric effect in photocatalytic H2O2 production over CN strongly depends on the molecular structure of CN. Specifically, for CN, CN modified by phosphorus (CN-P), oxygen-functionalized CN (CN-OF), and cyano-group-grafted CN (CN-CA), the photocatalytic activity of CN, CN-P, and CN-OF is enhanced by approximately 1.40, 1.46, and 1.51 times due to the piezoelectric effect, respectively, while the photocatalytic activity of CN-CA is decreased by 6.0 times. To clarify and understand the key factors affecting piezo-photocatalysis activity, we employed density functional theory, photo-electrochemical measurements, and piezoresponse force microscopy measurements to explore active sites, piezoelectric polarization, and charge separation over molecular-functionalized CN. Our results reveal that the impact of the piezoelectric effect on photocatalytic H2O2 production over CN results from the comprehensive influence of multiple factors. This work not only demonstrates that the molecular structure of CN determines whether the piezoelectric effect improves photocatalytic H2O2 production over CN but also unveils the mechanism of the piezoelectric effect on photocatalytic H2O2 production over CN.
KW - HO
KW - molecular engineering
KW - photocatalysis
KW - piezoelectric effect
UR - http://www.scopus.com/inward/record.url?scp=85164926530&partnerID=8YFLogxK
U2 - 10.1021/acscatal.3c02565
DO - 10.1021/acscatal.3c02565
M3 - Article
AN - SCOPUS:85164926530
SN - 2155-5435
VL - 13
SP - 9515
EP - 9523
JO - ACS Catalysis
JF - ACS Catalysis
IS - 14
ER -