Yang Liu, Yixuan Wang, Hao Li, Min Gyu Kim, Ziyang Duan, Kainat Talat, Jin Yong Lee, Mingbo Wu, Hyoyoung Lee
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引用次数: 0
摘要
酸性析氧反应用二氧化钌电催化剂活性一般,钌氧共价高,不稳定。本文采用熔盐辅助淬火的方法合成了拉伸应变锶和钽共掺杂的二氧化钌纳米催化剂。拉伸应变在空间上拉长了钌氧键,降低了共价,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上的去质子化,又优化了钌位上的中间体吸收,降低了反应能垒。综合实验和理论分析证实,这些结果形成了平衡良好的活动-稳定性剖面。我们的应变电极在0.5 M H2SO4中显示出10 mA cm - 2时的过电位为166 mV, s数高了一个数量级,表明与裸催化剂相比稳定性相当。在单电池和PEM电解槽的长期运行中,它的降解率可以忽略不计。本研究阐明了拉伸应变和策略掺杂在增强酸性析氧反应钌基催化剂的活性和稳定性方面的有效性。
Effectiveness of strain and dopants on breaking the activity-stability trade-off of RuO2 acidic oxygen evolution electrocatalysts
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−2 in 0.5 M H2SO4 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.
期刊介绍:
Nature Communications, an open-access journal, publishes high-quality research spanning all areas of the natural sciences. Papers featured in the journal showcase significant advances relevant to specialists in each respective field. With a 2-year impact factor of 16.6 (2022) and a median time of 8 days from submission to the first editorial decision, Nature Communications is committed to rapid dissemination of research findings. As a multidisciplinary journal, it welcomes contributions from biological, health, physical, chemical, Earth, social, mathematical, applied, and engineering sciences, aiming to highlight important breakthroughs within each domain.