在非碳酸盐电解质中，通过双电子水氧化产生过氧化氢的羟基自由基介导途径。
Crystal OH mediating pathway for hydrogen peroxide production via two-electron water oxidation in non-carbonate electrolytes.
作者信息
Wang Ruilin, Luo Hao, Duan Chengyu, Liu Huimin, Sun Mengdi, Zhou Quan, Ou Zheshun, Lu Yinglong, Luo Guanghui, Yu Jimmy C, Hu Zhuofeng
机构信息
School of Environmental Science and Engineering, Guangdong Provincial Key Laboratory of Environmental Pollution Control and Remediation Technology, Sun Yat-sen University, Guangzhou, 510006, China.
Department of chemistry, The Chinese University of Hong Kong, Hong Kong, China.
出版信息
Nat Commun. 2024 Dec 2;15(1):10456. doi: 10.1038/s41467-024-54593-4.
Water oxidation presents a promising avenue for hydrogen peroxide (HO) production. However, the reliance on alkaline bicarbonate electrolytes as an intermediate has limitations, such as HO decomposition and a narrow pH effectiveness range (7-9), restricting its utility across wider pH ranges. This study unveils a crystal OH mediating pathway that stabilizes SOOH* as a crucial intermediate. Basic copper carbonate (Cu(OH)CO) tablets, commonly found on cultural relics, exhibit the capability to generate HO in neutral or acidic non-bicarbonate electrolytes. By leveraging this crystal OH mediating strategy, considerable HO production in NaSO electrolytes is achievable. Notably, the HO production rate can reach 64.35 μmol h at 3.4 V vs. RHE in a 50 mL 0.5 M NaSO electrolyte. This research underscores the importance of crystal part in catalyst in catalyzing the 2e water oxidation reaction, offering valuable insights for future investigations.
水氧化是生产过氧化氢（HO）的一条有前景的途径。然而，依赖碱性碳酸氢盐电解质作为中间体存在局限性，如HO分解以及较窄的pH有效范围（7-9），限制了其在更宽pH范围内的应用。本研究揭示了一种晶体OH介导途径，该途径可稳定SOOH*作为关键中间体。在文物上常见的碱式碳酸铜（Cu(OH)CO）片剂，具有在中性或酸性非碳酸氢盐电解质中生成HO的能力。通过利用这种晶体OH介导策略，在NaSO电解质中可实现可观的HO产量。值得注意的是，在50 mL 0.5 M NaSO电解质中，相对于可逆氢电极（RHE）在3.4 V时，HO生成速率可达64.35 μmol h。本研究强调了催化剂中晶体部分在催化2e水氧化反应中的重要性，为未来的研究提供了有价值的见解。
Zotero 插件