电气和光化学H2通过Co (ii) 基聚基催化剂产生,这些催化剂含有由ortho取代的pyridines
Fiorella Lucarini1, Jennifer Fize2, Adina Morozan2
1Université de Fribourg Ch. du Musée 9 1700 Fribourg Switzerland albert.ruggi@unifr.ch.
Sustainable energy & fuels
|July 13, 2023
概括
新的催化剂与氨基-多聚烯基连接体显示出高活性进化反应 (HER). 对连接体结构的修改,特别是正体替代,增强了分子内质子转移,提高了可持续生产的催化效率.
科学领域:
- 协调化学 协调化学
- 催化剂是一种催化剂.
- 电化学 电化学 电化学
- 可再生能源可再生能源是可再生能源.
背景情况:
- (II) 复合物与六酸氨基-基连接物是有效的进化反应 (HER) 催化剂.
- 高性能与皮里丁单元促进的分子内质子转移途径有关.
- 了解连接物修饰是优化催化剂效率的关键.
研究的目的:
- 为了合成和研究新的基于氨基-多聚烯联体的质子还原催化剂.
- 探索对二烯环的正位置换对增强分子内质子转移的作用.
- 阐明用于HER的新型复合物的催化机制和基准性能.
主要方法:
- 合成了三种新的复合物,其中含有碳酸盐 (C2) 和基 (C3,C4) 替代的基连接物.
- 电化学研究包括波浪脚和催化塔菲尔图谱分析在乙.
- 使用密度函数理论 (DFT) 计算和光化学研究的机械研究.
主要成果:
- 综合体C3表现出最高的催化活性,周转频率 (TOF) 为1.6 (±0.5) × 10^5 s^-1,尽管具有很大的超潜力.
- DFT分析显示了大多数催化剂的典型ECEC机制,而复杂C2显示了初始质子激发的 (C) ECEC机制.
- 光化学研究证实了C3在水溶液中的优越性能.
结论:
- 六酸合联体在促进质子继电器以有效消除气方面发挥着至关重要的作用.
- 灵活的聚二连接物对于设计高效的复合物对于进化反应至关重要.
- 连接体设计,特别是正体替代,可以调整催化通路并提高 HER 的效率.
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