在膜-电极接口的CuFe合作性引发了一种Tandem 2e-+2e- 独家O2-To-H2O电还原机制
Tian Zeng1, Jiu Chen1, Zuo Hang Yu1
1Department of Chemistry, HKU-CAS Joint Laboratory on New Materials, University of Hong Kong, Hong Kong SAR, Hong Kong.
Journal of the American Chemical Society
|October 15, 2024
概括
新的双层混合膜电极具有丰富的CuFe活性位点,可以提高氧降解反应 (ORR) 的动力和选择性. 这一突破提高了能源转化效率,
科学领域:
- 电化学
- 材料科学
- 可持续能源
背景情况:
- 在氧降解反应 (ORR) 中实现高动力学和选择性对于可持续能源技术至关重要.
- 目前的非珍贵电催化剂难以同时提高ORR周转频率和H2O法拉第效率 (FE).
研究的目的:
- 开发新的混合双层膜 (HBM) 电极,使用丰富的金属控制质子合电子转移 (PCET) 以实现高效的ORR.
- 通过氧化酶启发的CuFe活性位点在三二甲基胺HBM上对ORR的性能进行研究.
主要方法:
- 混合双层膜 (HBM) 电极的制造,其中包含丰富的金属中心 (CuFe).
- 氧降解反应 (ORR) 活性和选择性的HBM电化学特征.
- 密度函数理论 (DFT) 计算以阐明反应机制.
- 使用开发的CuFeHBM构建和测试一个Zn-空气电池.
主要成果:
- 与单金属系统相比,双金属CuFe HBM的ORR活性高出1. 4倍.
- 在测试的HBM (Cu,Fe,Ni,Co) 中,达到了最高的H2O法拉代效率 (FE) ~94%.
- 加入一个基终端的质子载体使ORR电流增加了1.7倍,这与以前的疏水环境相反.
结论:
- 开发的CuFe HBM有效地控制了接口PCET,从而提高了ORR性能.
- DFT计算显示了一个协同效应,使得高性能ORR既有直接的4e-和并行的2e-+2e-路径.
- 在Zn空气电池等应用中,HBM技术显示出实用价值,为新的催化剂设计原则铺平了道路.
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