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

Yan Guo; Qixin Zhou; Jun Nan; Wenxin Shi; Fuyi Cui; Yongfa Zhu

doi:10.1038/s41467-022-29826-z

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

Nat Commun. 2022 Apr 19;13(1):2067. doi: 10.1038/s41467-022-29826-z.

Authors

Yan Guo^{1

2}, Qixin Zhou², Jun Nan¹, Wenxin Shi³, Fuyi Cui³, Yongfa Zhu⁴

Affiliations

¹ School of Environment, Harbin Institute of Technology, 150090, Harbin, China.
² Department of Chemistry, Tsinghua University, 100084, Beijing, China.
³ College of Environment and Ecology, Chongqing University, 400044, Chongqing, China.
⁴ Department of Chemistry, Tsinghua University, 100084, Beijing, China. Zhuyf@tsinghua.edu.cn.

Abstract

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.