表面化物在Fe2P电催化剂降低CO2在低超电位:引导选择性到乙烯糖醇
Karin U D Calvinho1, Abdulaziz W Alherz2, Kyra M K Yap1
1Department of Chemistry and Chemical Biology, Rutgers, The State University of New Jersey, 123 Bevier Road, Piscataway, New Jersey 08854, United States.
Journal of the American Chemical Society
|December 9, 2021
概括
铁化物 (Fe2P) 有效地催化二氧化碳降解 (CO2RR) 成为乙烯糖醇等多碳产物. 离子化物和应用的潜在控制产品选择性,为CO2RR机制提供了新的见解.
科学领域:
- 电化学
- 催化剂
- 材料科学
背景情况:
- 降低二氧化碳到多碳产品的高效电催化剂至关重要,但面临着高过量的潜力和低选择性的挑战.
- 为了克服基于贵重金属的系统的局限性,人们寻求大量的催化剂.
研究的目的:
- 引入铁化物 (Fe2P) 作为大量存在于土壤中的电催化剂,用于将二氧化碳减少为多碳产品.
- 研究反应机制和控制产品选择性的因素,特别是化物的作用和应用潜力.
主要方法:
- 电化学二氧化碳还原反应 (CO2RR) 实验
- 大法典-DFT (GC-DFT) 的计算.
- 介质物种和表面化物结合亲缘关系的分析.
主要成果:
- 对于C2-C4产品,Fe2P在0V与RHE之间显示了53%的总CO2RR法拉代效率.
- 产品选择性转向乙烯糖醇,负偏差增加.
- GC-DFT和实验显示,最初的中间体是甲,而不是CO,而离子化物起着关键作用.
- 通过负偏差减弱化结合,影响C2选择性和演变反应 (HER) 速率.
结论:
- 离子化物形成和结合亲和力,根据应用潜力调节,决定了碳产品在CO2RR中的分布.
- 了解化物物种化提供了对过渡金属化物的CO2RR机制的关键见解.
- 作为地球上丰富的选择性二氧化碳转化催化剂,Fe2P具有前景.
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