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应变和掺杂剂对打破RuO酸性析氧电催化剂活性-稳定性权衡的有效性。

Effectiveness of strain and dopants on breaking the activity-stability trade-off of RuO acidic oxygen evolution electrocatalysts.

作者信息

Liu Yang, Wang Yixuan, Li Hao, Kim Min Gyu, Duan Ziyang, Talat Kainat, Lee Jin Yong, Wu Mingbo, Lee Hyoyoung

机构信息

Shandong Provincial Key Laboratory for Science of Material Creation and Energy Conversion, Institute of Frontier Chemistry, School of Chemistry and Chemical Engineering, Shandong University, Qingdao, PR China.

Department of Chemistry, Sungkyunkwan University, Suwon, Republic of Korea.

出版信息

Nat Commun. 2025 Feb 17;16(1):1717. doi: 10.1038/s41467-025-56638-8.

Abstract

Ruthenium dioxide electrocatalysts for acidic oxygen evolution reaction suffer from mediocre activity and rather instability induced by high ruthenium-oxygen covalency. Here, the tensile strained strontium and tantalum codoped ruthenium dioxide nanocatalysts are synthesized via a molten salt-assisted quenching strategy. The tensile strained spacially elongates the ruthenium-oxygen bond and reduces covalency, thereby inhibiting the lattice oxygen participation and structural decomposition. The synergistic electronic modulations among strontium-tantalum-ruthenium groups both optimize deprotonation on oxygen sites and intermediates absorption on ruthenium sites, lowering the reaction energy barrier. Those result in a well-balanced activity-stability profile, confirmed by comprehensive experimental and theoretical analyses. Our strained electrode demonstrates an overpotential of 166 mV at 10 mA cm in 0.5 M HSO and an order of magnitude higher S-number, indicating comparable stability compared to bare catalyst. It exhibits negligible degradation rates within the long-term operation of single cell and PEM electrolyzer. This study elucidates the effectiveness of tensile strain and strategic doping in enhancing the activity and stability of ruthenium-based catalysts for acidic oxygen evolution reactions.

摘要

用于酸性析氧反应的二氧化钌电催化剂存在活性一般以及因钌-氧共价性高而导致的相当不稳定的问题。在此,通过熔盐辅助淬火策略合成了拉伸应变的锶和钽共掺杂二氧化钌纳米催化剂。拉伸应变在空间上拉长了钌-氧键并降低了共价性,从而抑制了晶格氧参与和结构分解。锶-钽-钌基团之间的协同电子调制既优化了氧位点上的去质子化又优化了钌位点上中间体的吸附,降低了反应能垒。这些导致了良好平衡的活性-稳定性分布,这通过全面的实验和理论分析得到证实。我们的应变电极在0.5 M H₂SO₄中10 mA cm⁻²时的过电位为166 mV,S值高出一个数量级,表明与裸催化剂相比稳定性相当。在单电池和质子交换膜电解槽的长期运行中,其降解率可忽略不计。这项研究阐明了拉伸应变和策略性掺杂在提高用于酸性析氧反应的钌基催化剂的活性和稳定性方面的有效性。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/49c9/11832934/5c93fb24b038/41467_2025_56638_Fig1_HTML.jpg

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