Well-dispersed Ruthenium in Mesoporous Crystal TiO2 as an Advanced Electrocatalyst for Hydrogen Evolution Reaction,Journal of the American Chemical Society

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Well-dispersed Ruthenium in Mesoporous Crystal TiO2 as an Advanced Electrocatalyst for Hydrogen Evolution Reaction
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2018-04-12 , DOI: 10.1021/jacs.7b13736
Shuying Nong ₁ , Wujie Dong ₁ , Junwen Yin ₂ , Bowei Dong ₁ , Yue Lu ₃ , Xiaotao Yuan ₁ , Xin Wang ₁ , Kejun Bu ₄ , Mingyang Chen ₂ , Shangda Jiang ₁ , Li-Min Liu _{2,

5} , Manling Sui ₃ , Fuqiang Huang _{1,

4}

Affiliation

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 SrTi1- xRu 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 GH).

中文翻译：

在介孔晶体 TiO2 中分散良好的钌作为析氢反应的高级电催化剂

以 SrTiO3 为前驱体，通过定向附着 (OA) 机制，通过一步腐蚀工艺制备了 TiO2 介孔晶体。高分辨率透射电子显微镜 (HRTEM) 和氮吸附-解吸等温线证实了其介孔晶体结构。在介孔纳米晶 TiO2 中分散良好的钌 (Ru) 可以通过使用 Ru 掺杂的前体 SrTi1-xRu xO3 的相同工艺获得。Ru掺杂到TiO2的晶格中，通过HRTEM和超能谱仪（super-EDS）元素映射鉴定。X 射线光电子能谱 (XPS) 和电子顺磁共振谱 (EPR) 表明是五价 Ru 而不是四价，而 TiO2 中的部分 Ti 接受来自 Ru 的电子并变成 Ti3+，这是首次观察到。这种 Ru 掺杂的 TiO2 在碱性溶液中对电催化析氢反应 (HER) 具有高活性。第一性原理计算模拟了 HER 过程，并证明 TiO2:Ru 与 Ru5+ 和 Ti3+ 在适当的氢吸附吉布斯自由能 (ΔGH) 下保持高 HER 活性。

更新日期：2018-04-12

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