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Amorphous-rich RuMnOx aerogel with weakened Ru–O covalency for efficient acidic water oxidation
Journal of Energy Chemistry ( IF 14.0 ) Pub Date : 2025-01-11 , DOI: 10.1016/j.jechem.2024.12.053
Tao Zhao , Yunzhen Jia , Qiang Fang , Runxin Du , Genyan Hao , Wenqing Sun , Guang Liu , Dazhong Zhong , Jinping Li , Qiang Zhao

Ruthenium dioxide (RuO2) is one of the most promising acidic oxygen evolution reaction (OER) catalysts to replace the expensive and prevalent iridium (Ir)-based materials. However, the lattice oxygen oxidation induced Ru dissolution during OER compromises the activity and stability. Amorphous materials have been identified as a viable strategy to promote the stability of RuO2 in acidic OER applications. This study reported a nanoporous amorphous-rich RuMnOx (A-RuMnOx) aerogel for efficient and stable acidic OER. Compared with highly crystalline RuMnOx, the weakened Ru–O covalency of A-RuMnOx by forming amorphous structure is favorable to inhibiting the oxidation of lattice oxygen. Meanwhile, this also optimizes the electronic structure of Ru sites from overoxidation and reduces the reaction energy barrier of the rate-determining step. As a result, A-RuMnOx aerogel exhibits an ultra-low overpotential of 145 mV at 10 mA cm−2 and durability exceeding 100 h, as well as high mass activity up to 153 mA mg−1Ru at 1.5 V vs. reversible hydrogen electrode (RHE). This work provides valuable guidance for preparing highly active and stable Ru-based catalysts for acidic OER.

中文翻译:


富含无定形的 RuMnOx 气凝胶,具有减弱的 Ru-O 共价,可实现高效的酸性水氧化



二氧化钌 (RuO2) 是最有前途的酸性析氧反应 (OER) 催化剂之一,可取代昂贵且普遍的铱 (Ir) 基材料。然而,在 OER 过程中晶格氧氧化诱导的 Ru 溶解损害了活性和稳定性。无定形材料已被确定为在酸性 OER 应用中促进 RuO2 稳定性的可行策略。本研究报道了一种纳米多孔无定形富 RuMnOx (A-RuMnOx) 气凝胶,用于高效稳定的酸性 OER。与高结晶度 RuMnOx 相比,A-RuMnOx 通过形成非晶结构而减弱的 Ru-O 共价有利于抑制晶格氧的氧化。同时,这也优化了 Ru 位点的电子结构,使其免受过氧化的影响,并减少了速率确定步骤的反应能垒。因此,与可逆氢电极 (RHE) 相比,A-RuMnOx 气凝胶在 10 mA cm-2 时表现出 145 mV 的超低过电位和超过 100 小时的耐用性,以及在 1.5 V 下高达 153 mA mg-1Ru 的高质量活度。这项工作为制备用于酸性 OER 的高活性和稳定的 Ru 基催化剂提供了有价值的指导。
更新日期:2025-01-11
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