School of Chemistry, Beihang University, Beijing, 100191, P. R. China.
State Key Laboratory for Advanced Technologies for Comprehensive Utilization of Platinum Metals, Sino-Platinum Metals Co. Ltd., 650221, Kunming, P. R. China.
Adv Sci (Weinh). 2023 May;10(13):e2207429. doi: 10.1002/advs.202207429. Epub 2023 Feb 21.
RuO is well known as the benchmark acidic oxygen evolution reaction (OER) catalyst, but its practical application has been impeded by its limited durability. Herein, it is presented that the stability of ruthenium oxide can be significantly improved by pretrapping RuCl precursors within a cage compound possessing 72 aromatic rings, which leads to well carbon-coated RuO particles (Si-RuO @C) after calcination. The catalyst survives in 0.5 M H SO for an unprecedented period of 100 hours at 10 mA cm with minimal overpotential change during OER. In contrast, RuO prepared from similar non-tied compounds doesn't exhibit such catalytic activity, highlighting the importance of the preorganization of Ru precursors within the cage prior to calcination. In addition, the overpotential at 10 mA cm in acid solution is only 220 mV, much less than that of commercial RuO . X-ray absorption fine structure (FT-EXAFS) reveals the Si doping through unusual Ru-Si bond, and density functional theory (DFT) calculation reveals the importance of the Ru-Si bond in enhancing both the activity and stability of the catalyst.
钌氧化物是众所周知的酸性析氧反应 (OER) 基准催化剂,但由于其耐久性有限,其实际应用受到阻碍。本文提出,通过将 RuCl 前体预先捕获在具有 72 个芳环的笼状化合物内,可以显著提高氧化钌的稳定性,这导致在煅烧后形成了具有良好碳涂层的氧化钌颗粒 (Si-RuO@C)。该催化剂在 0.5 M H2SO4 中以 10 mA cm 的电流密度下稳定运行 100 小时,在 OER 过程中过电势变化极小。相比之下,由类似的非束缚化合物制备的 RuO 则没有表现出这种催化活性,这突出了在煅烧前将 Ru 前体预组织在笼内的重要性。此外,在酸性溶液中,在 10 mA cm 的过电势仅为 220 mV,远小于商用 RuO2 的过电势。X 射线吸收精细结构 (FT-EXAFS) 表明通过不寻常的 Ru-Si 键进行 Si 掺杂,密度泛函理论 (DFT) 计算表明 Ru-Si 键在提高催化剂的活性和稳定性方面的重要性。