Co─N─C单原子站点的工程不对称电子结构朝着优秀的电化学H2O2生产和生物质升级
Kun Yu1, Shiming Guan1, Wenbiao Zhang2
1Jinan University, Department of Chemistry, No. 601 Huangpu West Avenue, Guangzhou, CHINA.
Angewandte Chemie (International ed. in English)
|February 27, 2025
概括
研究人员开发了一种不对称的Co─N5单原子位点催化剂,用于高效的电化学过氧化 (H2O2) 生产. 这一突破克服了活动选择性的权衡,使可持续的生物质利用和高产的酸合成成为可能.
科学领域:
- 材料科学 材料科学 材料科学
- 电化学 电化学 电化学
- 催化剂是一种催化剂.
背景情况:
- 单原子M-N-C电催化剂的精确结构控制对于推进电化学H2O2生产和理解催化机制至关重要.
- 现有的催化剂在产生H2O2时面临着活性和选择性之间的权衡.
研究的目的:
- 构建一个不对称的Co-N5位点电催化剂,以增强两电子氧降解反应 (2e-ORR) 以获得高效的H2O2生产.
- 调查不对称电子配置对O2激活和中间吸附的影响.
主要方法:
- 合成具有不对称电子配置的Co─N5单原子位点.
- 实验和理论分析 (包括DFT计算) 来研究反应机制.
- 在流量单元中进行电化学测试,用于测量H2O2生产速度.
- 将2e− ORR与生物质衍生碳水化合物氧化进行合,用于酸合成.
主要成果:
- 与对称的Co-N4位点相比,不对称的Co-N5位点显著提高了2e-ORR.
- 断裂点对称性促进了O2激活和调节了*OOH中间吸附,破坏了线性缩放关系.
- 实现了高的H2O2生产率,为16.1 mol gcat−1 h−1.1.
- 通过合反应证明了高酸产量 (84.1%来自葡萄糖,62.0%-92.1%来自其他基质).
结论:
- 单原子位点的不对称性与高效的2e-ORR和H2O2生产密切相关.
- 开发的Co-N5催化剂为可持续的电合成和生物质利用提供了一个有希望的途径.
- 这项工作为设计各种化学转换的高性能电催化剂提供了基本的见解.
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