Sixuan She, Hsiao-Chien Chen, Changsheng Chen, Yanping Zhu, Gao Chen, Yufei Song, Yiping Xiao, Zezhou Lin, Di Zu, Luwei Peng, Hao Li, Ye Zhu, Yuen Hong Tsang, Haitao Huang
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引用次数: 0
摘要
高效耐用的析氧反应电催化剂是质子交换膜水电解的关键。虽然掺杂的RuO2催化剂表现出良好的活性和稳定性,但掺杂物的存在限制了暴露活性位点的数量,使Ru的回收变得复杂。在这里,我们提出了一种具有周期性结构的点阵羟基的单金属RuO2 (d-RuO2)作为高性能的OER电催化剂。所制备的d-RuO2催化剂在10 mA cm-2下具有150 mV的低过电位和500 h的长期工作稳定性,优于目前报道的许多Ru/ ir基氧化物。使用d-RuO2的PEMWE装置在200 mA cm-2下可维持运行348小时。原位表征表明,晶格羟基的加入增加了Ru - Ru的距离,有利于Ru氧化态的翻转,促进OER过程中稳定的共边[RuO6]八面体的形成,从而加速O-O键的形成,抑制Ru位点的过度氧化。此外,催化剂的小粒径减小了三相接触线,促进了气泡的释放。该研究将为各种电化学反应催化剂的设计和优化提供新的思路。
Regulating Ru–Ru Distance in RuO2 Catalyst by Lattice Hydroxyl for Efficient Water Oxidation
Highly active and durable electrocatalysts for the oxygen evolution reaction (OER) are crucial for proton exchange membrane water electrolysis (PEMWE). While doped RuO2 catalysts demonstrate good activity and stability, the presence of dopants limits the number of exposed active sites and complicates Ru recovery. Here, we present a monometallic RuO2 (d-RuO2) with lattice hydroxyl in the periodic structure as a high-performance OER electrocatalyst. The obtained d-RuO2 catalyst exhibits a low overpotential of 150 mV and long-term operational stability of 500 h at 10 mA cm–2, outperforming many Ru/Ir-based oxides ever reported. A PEMWE device using d-RuO2 sustains operation for 348 h at 200 mA cm–2. In-situ characterization reveals that the incorporation of lattice hydroxyl increases the Ru–Ru distance, which facilitates the turnover of the Ru oxidation state and promotes the formation of stable edge-sharing [RuO6] octahedra during the OER, thereby accelerating the formation of O–O bonds and suppressing the overoxidation of Ru sites. Additionally, the small particle size of the catalyst decreases the three-phase contact line and promotes bubble release. This study will provide insights into the design and optimization of catalysts for various electrochemical reactions.
期刊介绍:
ACS Nano, published monthly, serves as an international forum for comprehensive articles on nanoscience and nanotechnology research at the intersections of chemistry, biology, materials science, physics, and engineering. The journal fosters communication among scientists in these communities, facilitating collaboration, new research opportunities, and advancements through discoveries. ACS Nano covers synthesis, assembly, characterization, theory, and simulation of nanostructures, nanobiotechnology, nanofabrication, methods and tools for nanoscience and nanotechnology, and self- and directed-assembly. Alongside original research articles, it offers thorough reviews, perspectives on cutting-edge research, and discussions envisioning the future of nanoscience and nanotechnology.