阐明原子稀释铜中心的作用,使胺聚合物浸为 CO2 减排上的优先进化反应2
Monika Chaudhary1, Mrinal Kanti Adak1, Dhananjay1
1Department of Chemistry, Indian Institute of Technology Delhi, Hauz Khas, New Delhi 110016, India.
Inorganic chemistry
|December 25, 2023
概括
这项研究合成了一种新型聚合物 (PAP) 并加入铜,以创建一个高效的电催化剂. 由此产生的铜聚合物复合物 (Cu30@PAP) 显著提高了进化反应 (HER) 的性能.
科学领域:
- 材料科学 材料科学 材料科学
- 电化学 电化学 电化学
- 催化剂是一种催化剂.
背景情况:
- 有机聚合物被探索为电催化剂,但由于导电性差而受到影响.
- 无金属聚合物通常需要修改以改善其催化活性.
- 开发高效和选择性的电催化剂对于能源转化至关重要.
研究的目的:
- 合成一种富含和的聚合物 (PAP),具有胺功能.
- 研究PAP及其含铜形式 (Cu30@PAP) 的电催化活性,用于演化反应 (HER) 和二氧化碳减排.
- 阐明铜合并的作用和催化剂的结构-活性关系.
主要方法:
- 从二胺胺 (DAP) 和二 (PPDC) 中合成PAP.
- 在PAP中浸泡铜盐以形成Cu30@PAP.
- 电化学表征 (HER,CO2减排) 使用循环电压测量和时电压测量.
- 用于结构和机械分析的光谱,显微和密度功能理论 (DFT) 研究.
主要成果:
- 与PAP相比,Cu30@PAP的表现显著改善了HER的性能,具有较低的超电位 (114 mV在10 mA cm-2) 与PAP相比.
- 铜的加入增强了电动力学,并降低了电荷转移电阻 (Rct).
- 在二氧化碳和二碳酸盐溶液中,HER仍然占主导地位,二氧化碳降解成形有限;催化剂结构和铜价值状态在反应后稳定.
结论:
- 在Cu30@PAP中的铜位点对于电催化是至关重要的,促进水吸附.
- 确定了四重协调的铜中心是活跃的地点, [CuI-H] 形成是 HER 和 CO2 减少的速度限制步骤.
- 电解质pH显著影响反应选择性,有利于低pH的HER.
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