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Nano Si-Doped Ruthenium Oxide Particles from Caged Precursors for High-Performance Acidic Oxygen Evolution
Advanced Science ( IF 14.3 ) Pub Date : 2023-02-21 , DOI: 10.1002/advs.202207429
Chunxiang Liu 1 , Yunbo Jiang 2 , Teng Wang 1, 3 , Qiaosheng Li 1 , Yuzhou Liu 1, 3, 4
Advanced Science ( IF 14.3 ) Pub Date : 2023-02-21 , DOI: 10.1002/advs.202207429
Chunxiang Liu 1 , Yunbo Jiang 2 , Teng Wang 1, 3 , Qiaosheng Li 1 , Yuzhou Liu 1, 3, 4
Affiliation
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RuO2 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 RuCl3 precursors within a cage compound possessing 72 aromatic rings, which leads to well carbon-coated RuOx particles (Si-RuOx@C) after calcination. The catalyst survives in 0.5 M H2SO4 for an unprecedented period of 100 hours at 10 mA cm−2 with minimal overpotential change during OER. In contrast, RuOx 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−2 in acid solution is only 220 mV, much less than that of commercial RuO2. 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.
中文翻译：
来自笼状前体的纳米 Si 掺杂氧化钌颗粒用于高性能酸性析氧
RuO 2是众所周知的基准酸性析氧反应 (OER) 催化剂，但其有限的耐用性阻碍了其实际应用。在此，提出通过在具有 72 个芳环的笼状化合物中预捕获 RuCl 3前体可以显着提高氧化钌的稳定性，从而在煅烧后产生良好的碳包覆 RuO x颗粒（Si-RuO x @C）。该催化剂在 0.5 MH 2 SO 4中在 10 mA cm -2下可存活 100 小时，这是前所未有的，并且在 OER 过程中过电势变化最小。相反，RuO x由类似的非束缚化合物制备的材料没有表现出这种催化活性，突出了在煅烧之前在笼内预先组织 Ru 前体的重要性。此外，在10 mA cm -2酸溶液中的过电势仅为220 mV，远低于商业RuO 2。X 射线吸收精细结构 (FT-EXAFS) 揭示了通过不寻常的 Ru-Si 键掺杂 Si，密度泛函理论 (DFT) 计算揭示了 Ru-Si 键在提高催化剂活性和稳定性方面的重要性。
更新日期：2023-02-21
中文翻译：
来自笼状前体的纳米 Si 掺杂氧化钌颗粒用于高性能酸性析氧
RuO 2是众所周知的基准酸性析氧反应 (OER) 催化剂，但其有限的耐用性阻碍了其实际应用。在此，提出通过在具有 72 个芳环的笼状化合物中预捕获 RuCl 3前体可以显着提高氧化钌的稳定性，从而在煅烧后产生良好的碳包覆 RuO x颗粒（Si-RuO x @C）。该催化剂在 0.5 MH 2 SO 4中在 10 mA cm -2下可存活 100 小时，这是前所未有的，并且在 OER 过程中过电势变化最小。相反，RuO x由类似的非束缚化合物制备的材料没有表现出这种催化活性，突出了在煅烧之前在笼内预先组织 Ru 前体的重要性。此外，在10 mA cm -2酸溶液中的过电势仅为220 mV，远低于商业RuO 2。X 射线吸收精细结构 (FT-EXAFS) 揭示了通过不寻常的 Ru-Si 键掺杂 Si，密度泛函理论 (DFT) 计算揭示了 Ru-Si 键在提高催化剂活性和稳定性方面的重要性。
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