Well-Dispersed Ruthenium in Mesoporous Crystal TiO 2 as an Advanced Electrocatalyst for Hydrogen Evolution Reaction

作者：Shuying Nong, Wujie Dong, Junwen Yin, Bowei Dong, Yue Lu, Xiaotao Yuan, Xin Wang, Kejun Bu, Mingyang Chen, Shang‐Da Jiang, Limin Liu, Manling Sui, Fuqiang Huang · 发表于：Journal of the American Chemical Society · 年份：2018 · DOI：10.1021/jacs.7b13736 · 被引用次数：314 · 研究领域：Electrocatalysts for Energy Conversion、Advanced Photocatalysis Techniques、Advanced battery technologies research

TiO 2 mesoporous crystal has been prepared by one-step corroding process via an oriented attachment (OA) mechanism with SrTiO 3 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 TiO 2 can be attained by the same process using Ru-doped precursor SrTi 1– x Ru x O 3 . Ru is doped into lattice of TiO 2, 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 TiO 2 accept an electron from Ru and become Ti 3+, which is observed for the first time. This Ru-doped TiO 2 performs high activity for electrocatalytic hydrogen evolution reaction (HER) in alkaline solution. First-principles calculations simulate the HER process and prove TiO 2:Ru with Ru 5+ and Ti 3+ holds high HER activity with appropriate hydrogen-adsorption Gibbs free energies (Δ G H ).