Adjustable heterointerface-vacancy enhancement effect in RuO2@Co3O4 electrocatalysts for efficient overall water splitting

Adjustable heterointerface-vacancy enhancement effect in RuO2@Co3O4 electrocatalysts for efficient overall water splitting
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DOI:
10.1016/j.apcatb.2022.122294
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发表时间:
2022-12-13
影响因子:
22.1
通讯作者:
He, Rongxing
He, Rongxing
中科院分区:
化学1区
文献类型:
--
作者:
Jiang, Yong;Liu, Hao;He, Rongxing

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揭示氧空位和异质界面增强催化活性的本质是一个重要而具有挑战性的课题。本文首次制备了具有可调异相界面放电增强效应的高性能RuO2@Co3O4电催化剂。所制备的RuO2@Co3O4(1:6)在碱性和酸性溶液中仅分别需要152,218 mV的OER和90,33 mV的HER的过电位以实现10 mA cm- 2的电流密度。此外,组装的电解池仅需要1.46,1.65 V和1.52,1.72 V的电压,以实现10和350 mA cm-2在相同的条件下。不同的Ru和Co的比例可以调节RuO 2和Co 3 O 4之间的异质界面的数量和界面氧空位的浓度。系统的实验和理论研究结果揭示了RuO 2和Co 3 O 4之间强电子耦合的异质界面加速了反应动力学,提高了催化剂的稳定性。界面氧空位不仅直接参与分解H2O的反应,而且还调节催化剂d带中心的位置和关键中间体的吸附强度,从而提高催化剂的活性。
Revealing the nature of enhanced catalytic activity by oxygen vacancy and hetero-interface is an important and challenging task. Herein, the high-performance RuO2@Co3O4 electrocatalyst with adjustable heterointerfacevacancy enhancement effect was prepared for the first time. The as-prepared RuO2@Co3O4(1:6) only respectively requires overpotentials of 152, 218 mV for OER and 90, 33 mV for HER in alkaline and acidic solutions to achieve a current density of 10 mA cm- 2. Moreover, the assembled electrolytic cell just need a voltages of 1.46, 1.65 V and 1.52, 1.72 V to achieve 10 and 350 mA cm-2 under the same conditions. The different ratios of Ru and Co can regulate the number of hetero-interfaces between RuO2 and Co3O4 and the concentration of interfacial oxygen vacancies. The systematically experimental and theoretical results unveil that the hetero-interface with strong electron coupling between RuO2 and Co3O4 accelerates the reaction kinetic and improves the stability of the catalyst. The interfacial oxygen vacancy not only directly participates in the reaction of dissociating H2O, but also adjusts the position of the d-band center of the catalyst and the adsorption strength of key intermediates, thus enhancing the activity of the catalysts.