Well-Dispersed Ruthenium in Mesoporous Crystal TiO2 as an Advanced Electrocatalyst for Hydrogen Evolution Reaction

Shuying Nong; Wujie Dong; Junwen Yin; Bowei Dong; Yue Lu; Xiaotao Yuan; Xin Wang; Kejun Bu; Mingyang Chen; Shangda Jiang; Li-Min Liu; Manling Sui; Fuqiang Huang

doi:10.1021/jacs.7b13736

Well-Dispersed Ruthenium in Mesoporous Crystal TiO₂ as an Advanced Electrocatalyst for Hydrogen Evolution Reaction

J Am Chem Soc. 2018 May 2;140(17):5719-5727. doi: 10.1021/jacs.7b13736. Epub 2018 Apr 17.

Authors

Shuying Nong¹, Wujie Dong¹, Junwen Yin², Bowei Dong¹, Yue Lu³, Xiaotao Yuan¹, Xin Wang¹, Kejun Bu⁴, Mingyang Chen², Shangda Jiang¹, Li-Min Liu^{2

5}, Manling Sui³, Fuqiang Huang^{1

4}

Affiliations

¹ State Key Laboratory of Rare Earth Materials Chemistry and Applications, College of Chemistry and Molecular Engineering , Peking University , Beijing 100871 , PR China.
² Beijing Computational Science Research Center , Beijing 100084 , PR China.
³ Institute of Microstructure and Properties of Advanced Materials , Beijing University of Technology , Beijing 100124 , PR China.
⁴ State Key Laboratory of High Performance Ceramics and Superfine Microstructures, Shanghai Institute of Ceramics , Chinese Academy of Sciences , Shanghai 200050 , PR China.
⁵ School of Physics , Beihang University , Beijing 100191 , PR China.

PMID: 29644854
DOI: 10.1021/jacs.7b13736

Abstract

TiO₂ mesoporous crystal has been prepared by one-step corroding process via an oriented attachment (OA) mechanism with SrTiO₃ as precursor. High resolution transmission electron microscopy (HRTEM) and nitrogen adsorption-desorption isotherms confirm its mesoporous crystal structure. Well-dispersed ruthenium (Ru) in the mesoporous nanocrystal TiO₂ can be attained by the same process using Ru-doped precursor SrTi_{1- x}Ru _xO₃. Ru is doped into lattice of TiO₂, which is identified by HRTEM and super energy dispersive spectrometer (super-EDS) elemental mapping. X-ray photoelectron spectroscopy (XPS) and electron paramagnetic resonance spectroscopy (EPR) suggest the pentavalent Ru but not tetravalent, while partial Ti in TiO₂ accept an electron from Ru and become Ti³⁺, which is observed for the first time. This Ru-doped TiO₂ performs high activity for electrocatalytic hydrogen evolution reaction (HER) in alkaline solution. First-principles calculations simulate the HER process and prove TiO₂:Ru with Ru⁵⁺ and Ti³⁺ holds high HER activity with appropriate hydrogen-adsorption Gibbs free energies (Δ G_H).

Publication types

Research Support, Non-U.S. Gov't