氨基含金共价有机框架上的动态质子使H2O2的高效中性电合成成为可能
Xiaohang Yang1, Yifan Wang1, Guangming Zhan1
1State Key Laboratory of Green Papermaking and Resource Recycling, School of Environmental Science and Engineering, National Observation and Research Station of Erhai Lake Ecosystem in Yunnan, Shanghai Jiao Tong University Yunnan Dali Research Institute, Shanghai Jiao Tong University, Shanghai, 200240, China.
Angewandte Chemie (International ed. in English)
|January 16, 2026
概括
这项研究引入了一种基于子的新型共价有机框架 (Q-COF),用于在中性条件下高效的过氧化 (H2O2) 电合成. 该材料增强了质子供应,克服了可持续H2O2生产的关键限制.
科学领域:
- 电化学 电化学 电化学
- 材料科学 材料科学 材料科学
- 可持续化学 可持续化学
背景情况:
- 在中性介质中对过氧化 (H2O2) 的电合成对于可持续的应用至关重要.
- 质子供应不足是中性H2O2电合成的一个基本限制.
- 基于子的共价有机框架 (Q-COF) 为催化应用提供了潜力.
研究的目的:
- 为中性H2O2电合成开发一种高效的电催化剂.
- 为了克服中性电解质中有限的质子可用性的挑战.
- 研究Q-COF中和氨基群的协同效应,以增强质子合电子转移.
主要方法:
- 用芳香氨基基群 (TfpBQ) 设计的基于子的共价有机框架 (Q-COF) 的合成.
- 电化学表征,包括循环电压测量和时测量.
- 实验和理论分析 (例如,DFT计算) 以阐明反应机制.
- 评估H2O2产量,法拉第效率和长期稳定性.
主要成果:
- TfpBQ证明了H2O2的高效中性电合成,产量为19.3mol g-1 h-1和95.6%的法拉代效率在120mA cm-2.
- 氨基群作为动态质子继电器,显著提高了交界质子-合电子转移 (I-PCET) 动力学 (kapp = 1.97×10^4 s-1).
- 催化剂在60小时的连续运行中表现出了特殊的稳定性.
结论:
- 设计的TfpBQ Q-COF有效地解决了中性H2O2电合成中的质子供应限制.
- 和芳香氨基群之间的协同作用是提高I-PCET动力学和整体性能的关键.
- 这项工作强调了动态质子化管理在电催化剂设计中对质子缺乏环境中的反应的重要性.
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