Fu Xiuting, Huang Xiaoxiao, Cen Yaping, Ren Xiaoyang, Yan Li, Jin Shao, Zhuang Zhongbin, Li Wanlu, Tian Shubo
International Joint Bioenergy Laboratory of Ministry of Education, State Key Laboratory of Chemical Resource Engineering, College of Chemistry, Beijing University of Chemical Technology, Beijing, 100029, China.
State Key Laboratory of Organic-Inorganic Composites, Beijing University of Chemical Technology, Beijing, 100029, China.
Small. 2024 Dec;20(51):e2406387. doi: 10.1002/smll.202406387. Epub 2024 Oct 10.
The development of efficient and durable electrocatalysts for the alkaline hydrogen oxidation/evolution reaction is crucial for anion exchange membrane fuel cells/water electrolyzers. However, designing such electrocatalysts poses a challenge due to the need for optimizing various adsorbates. Herein, highly dispersed Ru nanoparticles catalysts is reported encapsulated and supported by defective anatase phase of titanium dioxide (named as Ru NPs/def-TiO(A)) for boosting hydrogen-cycle electrocatalysis with robust anti-CO-poisoning in alkaline conditions. The Ru NPs/def-TiO(A) achieves a high-quality activity of 7.65 A mg , which is 23.2 and 9.5-fold higher than commercial Ru/C and Pt/C in alkaline HOR. Moreover, this catalyst exhibits an outstanding overpotential of 21 mV at 10 mA cm in alkaline HER. Hydrogen underpotential deposition (H) and CO stripping experiments demonstrate that Ru NPs/def-TiO(A) has the optimized H*, OH*, and CO* adsorption strength, enabling the Ru NPs/def-TiO(A) catalyst to display excellent and robust HOR/HER performance under alkaline conditions. Using density functional theory calculations, the enhanced HOR performance mechanism for the Ru NPs/def-TiO(A) catalyst originates from the TiO step face in contact with the Ru nanoparticles, indicating that the kinetics of water formation are considerably more favorable at the Ru NPs/def-TiO(A) interface.
开发用于碱性氢氧化/析氢反应的高效耐用的电催化剂对于阴离子交换膜燃料电池/水电解槽至关重要。然而，由于需要优化各种吸附质，设计这样的电催化剂面临挑战。在此，报道了一种高度分散的钌纳米颗粒催化剂，其被二氧化钛的缺陷锐钛矿相包裹并负载（命名为Ru NPs/def-TiO(A)），用于在碱性条件下促进具有强大抗一氧化碳中毒能力的氢循环电催化。Ru NPs/def-TiO(A)实现了7.65 A mg的高质量活性，在碱性氢氧化反应中分别比商业Ru/C和Pt/C高23.2倍和9.5倍。此外，该催化剂在碱性析氢反应中，在10 mA cm时表现出21 mV的出色过电位。氢欠电位沉积(H)和一氧化碳剥离实验表明，Ru NPs/def-TiO(A)具有优化的H*、OH和CO吸附强度，使Ru NPs/def-TiO(A)催化剂在碱性条件下表现出优异且稳定的氢氧化/析氢性能。使用密度泛函理论计算，Ru NPs/def-TiO(A)催化剂增强的氢氧化性能机制源于与钌纳米颗粒接触的TiO台阶面，这表明在Ru NPs/def-TiO(A)界面处水形成的动力学要有利得多。
