Constructing built-in electric field via ruthenium/cerium dioxide Mott-Schottky heterojunction for highly efficient electrocatalytic hydrogen production

Xinyu Chen; Diwei Shi; Min Bi; Jiexi Song; Yanqing Qin; Shiyu Du; Bianjing Sun; Chuntao Chen; Dongping Sun

doi:10.1016/j.jcis.2023.07.203

Constructing built-in electric field via ruthenium/cerium dioxide Mott-Schottky heterojunction for highly efficient electrocatalytic hydrogen production

J Colloid Interface Sci. 2023 Dec 15;652(Pt A):653-662. doi: 10.1016/j.jcis.2023.07.203. Epub 2023 Jul 31.

Authors

Xinyu Chen¹, Diwei Shi², Min Bi¹, Jiexi Song³, Yanqing Qin³, Shiyu Du⁴, Bianjing Sun⁵, Chuntao Chen⁶, Dongping Sun⁷

Affiliations

¹ School of Chemistry and Chemical Engineering, Nanjing University of Science and Technology, 200 Xiao Ling Wei Street, Nanjing 210094, China.
² School of Naval Architecture and Maritime, Zhejiang Ocean University, Zhoushan 316022, China.
³ School of Physical Science and Technology, Northwestern Polytechnical University, Xian 710072, China.
⁴ Engineering Laboratory of Nuclear Energy Materials, Ningbo Institute of Industrial Technology, Chinese Academy Sciences, Ningbo 315201, China.
⁵ School of Chemistry and Chemical Engineering, Nanjing University of Science and Technology, 200 Xiao Ling Wei Street, Nanjing 210094, China. Electronic address: bjsun1992@163.com.
⁶ School of Chemistry and Chemical Engineering, Nanjing University of Science and Technology, 200 Xiao Ling Wei Street, Nanjing 210094, China. Electronic address: chchunt@njust.edu.cn.
⁷ School of Chemistry and Chemical Engineering, Nanjing University of Science and Technology, 200 Xiao Ling Wei Street, Nanjing 210094, China. Electronic address: sundpe301@163.com.

PMID: 37543477
DOI: 10.1016/j.jcis.2023.07.203

Abstract

Ensuring the consumption rate of noble metals while guaranteeing satisfactory hydrogen evolution reaction (HER) performance at different pH values is imperative to the development of Ru-based catalysts. Herein, we design a Mott-Schottky electrocatalyst (Ru/CeO₂) with a built-in electric field (BEF) based on density functional theory (DFT). The Ru/CeO₂ achieves the criterion current density of 10 mA cm^-2 at overpotentials of 55 mV, 80 mV, and 120 mV in alkaline, acidic and neutral media, respectively. Both theoretical calculations and experimental analysis confirm that the improved HER activity in the Ru/CeO₂ catalyst could be due to the successful construction of BEF at the interface between the prepared Ru clusters and CeO₂. Under the action of BEF, the electron-deficient Ru atoms can optimize the adsorption energy of H* and H₂O and thus promote HER kinetics. Furthermore, the Ru/CeO₂ catalyst delivers a power density of approximately 94.5 mW cm^-2 in alkaline-acidic Zn-H₂O cell applications while maintaining good H₂ production stability. In this work, we optimize the electrocatalytic performance of the Ru/CeO₂ catalyst through examination of the interfacial BEF electrical charge, which combines hydrogen production with power generation and provides a promising method for sustainable energy conversion.

Keywords: Built-in electric field; DFT; Hydrogen production; Ru/CeO(2); Zn-H(2)O cell.