用于高内在活性电催化CO2降解的P块单原子催化剂
Zhanshuai Ma1,2, Bingqing Wang1, Xiang Yang1
1State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029, China.
一种新型的单原子催化剂 (Al-NC) 有效地将二氧化碳减少为二氧化碳,克服了活性限制. 这种土壤丰富的催化剂具有很高的选择性和效率,性能优于过渡金属催化剂.
科学领域:
- 电化学
- 催化剂
- 材料科学
背景情况:
- 在化碳上的原子分散过渡金属位点对二氧化碳转化为二氧化碳具有前景.
- 一个关键的挑战是高能量阻碍*COOH形成或*CO脱吸,限制内在活性.
- 这种缩放关系阻碍了催化剂的性能.
研究的目的:
- 开发一种能够克服二氧化碳电减缩放关系的催化剂.
- 调查一个p-块单原子催化剂 (Al-NC) 与一个Al-N4网站.
- 为了能够解开*COOH形成和*CO脱吸的动力障碍.
主要方法:
- 在现场减弱的全反射红外光谱研究反应中间体.
- 理论模拟以验证反应动力障碍.
- 在流电池和膜电极组件 (MEAs) 中进行电化学性能测试.
主要成果:
- Al-NC 催化剂对*COOH 形成和*CO 脱吸具有中等的反应动力障碍.
- 在0.65V和RHE下达到高达98.76%的 CO 法拉代效率 (FE_CO).
- 在0.99V与RHE相比,具有3.60s^-1的高内在催化转换频率,超过Ni-NC和Fe-NC.
- 在流量单元 (309 mA·cm^-2 在93.65% FE_CO) 和 MEA (605 mA 在>85% FE_CO) 配置中输送大量的部分CO电流.
- 使用低度的二氧化碳原料保持高性能 (240 mA>80%FE_CO与30%的二氧化碳).
结论:
- 酸催化剂有效地解开了二氧化碳电还原中的动力障碍.
- 与最先进的过渡金属催化剂相比,它具有更高的内在活性和选择性.
- 它的土壤丰富性和高性能使其成为CO2RR应用的有希望的替代品.
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