Enhanced localized dipole of Pt-Au single-site catalyst for solar water splitting

Xingyu Liu; Zhifei Hao; Haitao Wang; Tuo Wang; Zhurui Shen; Hao Zhang; Sihui Zhan; Jinlong Gong

doi:10.1073/pnas.2119723119

Enhanced localized dipole of Pt-Au single-site catalyst for solar water splitting

Proc Natl Acad Sci U S A. 2022 Feb 22;119(8):e2119723119. doi: 10.1073/pnas.2119723119.

Authors

Xingyu Liu¹, Zhifei Hao¹, Haitao Wang¹, Tuo Wang², Zhurui Shen^{3

4}, Hao Zhang⁴, Sihui Zhan³, Jinlong Gong^{5

6}

Affiliations

¹ Ministry of Education Key Laboratory of Pollution Processes and Environmental Criteria Tianjin Key Laboratory of Environmental Remediation and Pollution Control, College of Environmental Science and Engineering, Nankai University, Tianjin 300350, China.
² Key Laboratory for Green Chemical Technology of Ministry of Education, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China.
³ Ministry of Education Key Laboratory of Pollution Processes and Environmental Criteria Tianjin Key Laboratory of Environmental Remediation and Pollution Control, College of Environmental Science and Engineering, Nankai University, Tianjin 300350, China; shenzhurui@nankai.edu.cn sihuizhan@nankai.edu.cn jlgong@tju.edu.cn.
⁴ School of Materials Science and Engineering, Nankai University, Tianjin 300350, China.
⁵ Key Laboratory for Green Chemical Technology of Ministry of Education, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China; shenzhurui@nankai.edu.cn sihuizhan@nankai.edu.cn jlgong@tju.edu.cn.
⁶ Joint School of National University of Singapore and Tianjin University, International Campus of Tianjin University, Binhai New City, Fuzhou 350207, China.

Abstract

Solar water splitting is regarded as holding great potential for clean fuels production. However, the efficiency of charge separation/transfer of photocatalysts is still too low for industrial application. This paper describes the synthesis of a Pt-Au binary single-site loaded g-C₃N₄ nanosheet photocatalyst inspired by the concept of the dipole. The existent larger charge imbalance greatly enhanced the localized molecular dipoles over adjacent Pt-Au sites in contrast to the unary counterparts. The superposition of molecular dipoles then further strengthened the internal electric field and thus promoted the charge transportation dynamics. In the modeling photocatalytic hydrogen evolution, the optimal Pt-Au binary site photocatalysts (0.25% loading) showed 4.9- and 2.3-fold enhancement of performance compared with their Pt and Au single-site counterparts, respectively. In addition, the reaction barrier over the Pt-Au binary sites was lowered, promoting the hydrogen evolution process. This work offers a valuable strategy for improving photocatalytic charge transportation dynamics by constructing polynary single sites.

Keywords: binary single sites; internal electric field; localized dipole; solar water splitting.