一个固定的Re-tricarbonyl催化剂对CO2减少的定位效应
Jeremiah C Choate1, Israel Silva1, Po Ching Hsu1
1Department of Chemistry, University of Southern California, California, Los Angeles 90089, United States.
ACS applied materials & interfaces
|September 10, 2024
概括
可再生能源储存通过将二氧化碳 (CO2) 转化为一氧化碳 (CO),使用固定化的复合体来提升. 优化对双氨酸骨干的绑定位置可以提高二氧化碳减排的选择性和稳定性.
科学领域:
- 电化学 电化学 电化学
- 材料科学 材料科学 材料科学
- 催化剂是一种催化剂.
背景情况:
- 间歇性的可再生能源需要高效的储能解决方案.
- 将二氧化碳 (CO2) 转化为一氧化碳 (CO) 为可再生能源储能提供了一条道路.
- 将分子复合体固定在固体支上对于开发强大的催化剂至关重要.
研究的目的:
- 为了使固定下来 (I) 三碳基分子复合体,以减少二氧化碳.
- 为了研究绑定位置对催化剂性能和结构的影响.
- 评估异质化复合体的二氧化碳减排活性和稳定性.
主要方法:
- 通过 bis ((diazonium) 替代物的还原性合来合成和固定 (I) 复合物.
- 使用UV-Vis,ATR-IR,IRS和XPS进行表征.
- 电化学评估包括循环电压测量,控制电位电解和电化学阻抗光谱学.
主要成果:
- 在双二烯骨干的4,4'-位置固定复合体显示出出色的CO选择性 (>99%) 和高活性 (TON=3359,TOF=0.9 s-1).
- 催化剂在5小时的非水性流动细胞电解过程中表现出稳定性.
- 与5.5′位置相比,在4.4′位置的结合导致活动较低,这归因于聚合和Re-Re二元体的形成.
结论:
- 固定化复合体有效地将二氧化碳转化为二氧化碳,这是储存可再生能源的关键步骤.
- 连接位置显著影响催化剂形态,聚合,并最终减少二氧化碳的性能.
- 对碳布的最佳催化剂负荷被确定为44.6 ± 11nmol/cm2以实现高效性能.
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