通过金纳米集群的合体工程促进CO2到CO的电还原
Sang Myeong Han1, Minyoung Park1, Jiyoung Kim1
1Department of Chemistry, Yonsei University, Seoul, 03722, Republic of Korea.
Angewandte Chemie (International ed. in English)
|May 17, 2024
概括
研究人员使用原子精确的黄金纳米集群和带有阴离子转移连接体增强了电化学二氧化碳减排 (CO2RR). 这一战略显著促进了CO2转化为CO的转化活动,显示了高效碳利用的潜力.
科学领域:
- 电化学 电化学 电化学
- 催化剂是一种催化剂.
- 纳米材料是一种纳米材料.
背景情况:
- 电化学二氧化碳减排 (CO2RR) 是将二氧化碳转化为有价值产品的关键技术.
- 电解质中的金属离子在CO2RR活性和选择性中起着至关重要的作用.
- 精确原子金属纳米集群为CO2RR提供可调节的催化性能.
研究的目的:
- 通过将黄金纳米集群 (Au25) 功能化为带有阴离子继电联体,开发有效的CO2RR电催化剂.
- 为了研究金属离子和连接物结构对CO2RR性能的影响.
- 为了阐明在Au25纳米集群上加离子增强的CO2RR的机制.
主要方法:
- 合成了Au25纳米集群,其功能与6 - 默卡普托赫萨诺酸 (MHA) 和1-hexanethiolate (HT) 相结合.
- 对Au25 (MHA) 18和Au25 (HT) 18的CO2RR活性和选择性的电化学评估18.
- 机理学研究涉及不同的阴解质pH值,阴离子类型 (Li+,Na+,K+,Cs+) 和度.
主要成果:
- Au25(MHA) 18表现出明显高于Au25(HT) 18的CO2-CO转化活性,特别是在MHA的pH>pKa时,由于阴离子转移效应.
- 对于两个纳米集群来说,CO2RR活动遵循了Li+ < Na+ < K+ < Cs+的顺序.
- 阴离子合电子转移被确定为速度限制步骤,通过极化曲线中的Nernstian转移来证实.
结论:
- 功能化Au25纳米集群与MHA等离子中继联体是一种有效的策略,以增强CO2RR.
- 阴离子中继效应和阴离子合电子转移对于优化CO2RR性能至关重要.
- 这项工作为设计先进的电催化剂提供了洞察力,以实现高效的二氧化碳转化.
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