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源自钌耦合镍金属有机框架的氧化钌镍用于高效析氧反应。

Ruthenium-nickel oxide derived from Ru-coupled Ni metal-organic framework for effective oxygen evolution reaction.

作者信息

Xu Jiayu, Yu Lice, Dong Baoxia, Yang Fulin, Feng Ligang

机构信息

School of Chemistry and Chemical Engineering, Yangzhou University, Yangzhou 225002, Jiangsu, China.

School of Chemistry and Chemical Engineering, Yangzhou University, Yangzhou 225002, Jiangsu, China.

出版信息

J Colloid Interface Sci. 2023 Oct 19;654(Pt B):1080-1088. doi: 10.1016/j.jcis.2023.10.088.

Abstract

Developing Ru-based catalysts with both high activity and stability for the oxygen evolution reaction (OER) is very significant in the water electrolysis technique. Here, a bimetallic metal oxide catalyst (RuO-NiO) derived from Ru-coupled Ni metal-organic framework (Ni-MOF) by using terephthalic acid as the ligand was successfully synthesized through a facile ultrasonic treatment and subsequent thermal annealing approach; and the effective role of the coupled effect between RuO and NiO in stabilizing Ru was found significant in OER catalysis. A relatively small d-band center due to the electronic structure regulation and synergistic effect of the heterostructure was found to cause weakened adsorption of surface oxygen species. Theoretical calculations demonstrated that the electronic modulation between RuO and NiO can significantly accelerate the dissociation of water and modulate the chemical adsorption of oxygen intermediates on the catalyst, thereby enhancing the OER activity of the catalyst. The optimized catalyst of RuO-NiO afforded a current density of 10 mA cm at low overpotentials of 210 mV toward OER, and good catalytic stability, kinetics and efficiency were also discussed. This remarkable catalytic performance can be attributed to the unique sheet-like structure and porous morphology of the catalyst with increased exposure of active sites and the coupling effect between RuO and NiO for moderate binding strength to the intermediates. This study showed an effective approach for bimetallic oxide catalyst fabrication and their applications in energy conversion reactions.

摘要

开发具有高活性和稳定性的用于析氧反应(OER)的钌基催化剂在水电解技术中具有重要意义。在此,通过简便的超声处理和随后的热退火方法,成功合成了一种由钌耦合的镍金属有机框架(Ni-MOF)以对苯二甲酸为配体衍生而来的双金属氧化物催化剂(RuO-NiO);并且发现RuO和NiO之间的耦合效应在稳定Ru方面的有效作用在OER催化中具有重要意义。由于异质结构的电子结构调控和协同效应,发现一个相对较小的d带中心会导致表面氧物种的吸附减弱。理论计算表明,RuO和NiO之间的电子调制可以显著加速水的解离并调节氧中间体在催化剂上的化学吸附,从而提高催化剂的OER活性。优化后的RuO-NiO催化剂在210 mV的低过电位下对OER提供了10 mA cm的电流密度,并且还讨论了良好的催化稳定性、动力学和效率。这种卓越的催化性能可归因于催化剂独特的片状结构和多孔形态,活性位点暴露增加,以及RuO和NiO之间的耦合效应,使其对中间体具有适度的结合强度。本研究展示了一种制备双金属氧化物催化剂及其在能量转换反应中应用的有效方法。

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