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构建与主要组金属协调的单维共价有机框架,用于选择性电化学合成H₂O₂

Jinyan Wang¹, Huimin Sun¹, Shaoda Huang^1,2

¹Key Laboratory of Synthetic and Biological Colloids, Ministry of Education, School of Chemical and Material Engineering, Jiangnan University, Wuxi 214122, P. R. China.

ACS applied materials & interfaces

|October 8, 2024

概括

研究人员开发了使用主要组金属的新型共价有机框架 (COF),通过两电子氧降解反应 (2e− ORR) 通过高效的过氧化 (H2O2) 合成. 在绿色化学品生产中,安提蒙协调的COF表现出卓越的性能和稳定性.

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:

聚合有机框架 (COF) 显示了作为电催化剂的潜力,用于产生过氧化 (H2O2) 的两电子氧降解反应 (2e− ORR).
为选择性H2O2合成设计高效和稳定的COF电催化剂仍然是一个重大挑战.

研究的目的:

构建和评估使用主要组金属 (,锡,) 作为2e− ORR的电催化剂的新型1D COF.
为了研究这些金属协调COF在H2O2生产中的性能,结构-活动关系.

主要方法:

一个预先设计的基于1,10-phenanthroline的1D COF (PYTA-PTDE-COF) 的合成.
将 (In),锡 (Sn) 和反 (Sb) 协调到COF结构中,以创建PYTA-PTDE-M催化剂.
对2e−ORR活性,选择性和性条件下的稳定性的催化剂的电化学表征.
理论计算以阐明机制和结构-活动关系.

主要成果:

所有合成的PYTA-PTDE-M (M = In, Sn, Sb) 催化剂都表现出良好的结晶性和暴露的金属侧链.
在性介质中的所有催化剂中观察到对2e− ORR的满意活性和选择性.
PYTA-PTDE-Sb表现出最高的性能:0.765 V的发作潜力,96%的H2O2选择性,以及209.2 mmol g-1 h-1.1 的产率.
PYTA-PTDE-Sb表现出极好的长期稳定性,电流密度衰减最小.
理论计算表明,Sb位点的低*OOH吸附强度是其高选择性的关键.

结论:

开发的主要组金属协调1DCOF是通过2e− ORR选择性H2O2合成的有效电催化剂.
反协调COF (PYTA-PTDE-Sb) 提供了卓越的性能和稳定性,突出了金属选择的重要性.
这项研究为金属-COF系统中的2e− ORR的结构-活性关系提供了基本的见解.
对于集成的清洁能源供应和绿色化学品生产,PYTA-PTDE-Sb显示出有前途的前景,其在空气电池中的使用就是一个例子.

关键词:

电触媒溶解是一种电触媒.过氧化是一种过氧化.主要组金属金属一个维的COF.氧降解反应是一种氧降解反应.

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