Perylenetetracarboxylic acid nanosheets with internal electric fields and anisotropic charge migration for photocatalytic hydrogen evolution

• Published in: Nature communications Vol. 13; no. 1; p. 2067
• Main Authors: Guo, Yan, Zhou, Qixin, Nan, Jun, Shi, Wenxin, Cui, Fuyi, Zhu, Yongfa
• Format: Journal Article
• Language: English
• Published: London Nature Publishing Group UK 19.04.2022; Nature Publishing Group; Nature Portfolio
• Subjects: 140/125; 140/131; 140/146; 140/58; 147/135; 147/143; 147/3; 639/301/299/890; 639/4077/909; 639/638/77/885; 639/925/357; Acids; Carrier recombination; Conjugation; Current carriers; Electric fields; Electronics industry; Evolution; Humanities and Social Sciences; Hydrogen; Hydrogen evolution reactions; Inorganic materials; Molecular structure; multidisciplinary; Nanosheets; Organic semiconductors; Photocatalysis; Photocatalysts; Recombination; Reduction; Science; Science (multidisciplinary)
• ISSN: 2041-1723; 2041-1723
• DOI: 10.1038/s41467-022-29826-z

Highly efficient hydrogen evolution reactions carried out via photocatalysis using solar light remain a formidable challenge. Herein, perylenetetracarboxylic acid nanosheets with a monolayer thickness of ~1.5 nm were synthesized and shown to be active hydrogen evolution photocatalysts with production rates of 118.9 mmol g −1 h −1 . The carboxyl groups increased the intensity of the internal electric fields of perylenetetracarboxylic acid from the perylene center to the carboxyl border by 10.3 times to promote charge-carrier separation. The photogenerated electrons and holes migrated to the edge and plane, respectively, to weaken charge-carrier recombination. Moreover, the perylenetetracarboxylic acid reduction potential increases from −0.47 V to −1.13 V due to the decreased molecular conjugation and enhances the reduction ability. In addition, the carboxyl groups created hydrophilic sites. This work provides a strategy to engineer the molecular structures of future efficient photocatalysts. While organic semiconductors provide a highly tailorable set of systems for solar-to-fuel conversion, such materials often show worse activities than inorganic materials. Here, authors prepare perylene-based nanosheets that demonstrate excellent performances for photocatalytic H 2 evolution.