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通过晶格羟基调节RuO催化剂中Ru-Ru距离以实现高效水氧化

Regulating Ru-Ru Distance in RuO Catalyst by Lattice Hydroxyl for Efficient Water Oxidation.

作者信息

She Sixuan, Chen Hsiao-Chien, Chen Changsheng, Zhu Yanping, Chen Gao, Song Yufei, Xiao Yiping, Lin Zezhou, Zu Di, Peng Luwei, Li Hao, Zhu Ye, Tsang Yuen Hong, Huang Haitao

机构信息

Department of Applied Physics, The Hong Kong Polytechnic University, Hung Hom, Kowloon, Hong Kong, China.

Center for Reliability Science and Technologies, Chang Gung University, Taoyuan 33302, Taiwan.

出版信息

ACS Nano. 2025 May 20;19(19):18513-18521. doi: 10.1021/acsnano.5c01937. Epub 2025 May 6.

DOI:10.1021/acsnano.5c01937
PMID:40329443
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC12096437/
Abstract

Highly active and durable electrocatalysts for the oxygen evolution reaction (OER) are crucial for proton exchange membrane water electrolysis (PEMWE). While doped RuO 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 RuO (d-RuO) with lattice hydroxyl in the periodic structure as a high-performance OER electrocatalyst. The obtained d-RuO catalyst exhibits a low overpotential of 150 mV and long-term operational stability of 500 h at 10 mA cm, outperforming many Ru/Ir-based oxides ever reported. A PEMWE device using d-RuO sustains operation for 348 h at 200 mA cm. 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 [RuO] 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.

摘要

用于析氧反应(OER)的高活性和耐用的电催化剂对于质子交换膜水电解(PEMWE)至关重要。虽然掺杂的RuO催化剂表现出良好的活性和稳定性,但掺杂剂的存在限制了暴露的活性位点数量,并使Ru的回收复杂化。在此,我们展示了一种在周期性结构中具有晶格羟基的单金属RuO(d-RuO)作为高性能OER电催化剂。所获得的d-RuO催化剂在10 mA cm下表现出150 mV的低过电位和500 h的长期运行稳定性,优于许多已报道的基于Ru/Ir的氧化物。使用d-RuO的PEMWE装置在200 mA cm下可持续运行348 h。原位表征表明,晶格羟基的掺入增加了Ru-Ru距离,这有利于Ru氧化态的转变,并促进在OER过程中形成稳定的边共享[RuO]八面体,从而加速O-O键的形成并抑制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并促进气泡释放。这项研究将为各种电化学反应的催化剂设计和优化提供见解。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a168/12096437/955f72e4de18/nn5c01937_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a168/12096437/7589e1f2e12b/nn5c01937_0001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a168/12096437/d21a7fe4fe42/nn5c01937_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a168/12096437/5bc834ef9c8c/nn5c01937_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a168/12096437/955f72e4de18/nn5c01937_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a168/12096437/7589e1f2e12b/nn5c01937_0001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a168/12096437/d21a7fe4fe42/nn5c01937_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a168/12096437/5bc834ef9c8c/nn5c01937_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a168/12096437/955f72e4de18/nn5c01937_0004.jpg

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本文引用的文献

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Lanthanide-regulating Ru-O covalency optimizes acidic oxygen evolution electrocatalysis.镧系元素调控的Ru-O共价性优化了酸性析氧电催化性能。
Nat Commun. 2024 Jun 11;15(1):4974. doi: 10.1038/s41467-024-49281-2.
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Atomically dispersed hexavalent iridium oxide from MnO reduction for oxygen evolution catalysis.通过MnO还原制备的用于析氧催化的原子级分散的六价氧化铱。
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Bifunctional Electrocatalysts for Overall and Hybrid Water Splitting.用于全水分解和混合水分解的双功能电催化剂。
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Breaking the Ru-O-Ru Symmetry of a RuO Catalyst for Sustainable Acidic Water Oxidation.打破用于可持续酸性水氧化的RuO催化剂的Ru-O-Ru对称性。
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Bubble Engineering on Micro-/Nanostructured Electrodes for Water Splitting.用于水分解的微/纳米结构电极上的气泡工程
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Stable and oxidative charged Ru enhance the acidic oxygen evolution reaction activity in two-dimensional ruthenium-iridium oxide.稳定且带氧化电荷的钌增强了二维钌铱氧化物中的析氧反应活性。
Nat Commun. 2023 Sep 4;14(1):5365. doi: 10.1038/s41467-023-41036-9.
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Supported Ruthenium Single-Atom and Clustered Catalysts Outperform Benchmark Pt for Alkaline Hydrogen Evolution.负载型钌单原子和簇状催化剂在碱性析氢反应中性能优于基准铂催化剂。
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Highly active and stable OER electrocatalysts derived from SrMIrO for proton exchange membrane water electrolyzers.源自 SrMIrO 的高活性和稳定的质子交换膜水电解用 OER 电催化剂。
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