Sarah Bimmermann , Daniel Siegmund , Kallol Ray , Ulf-Peter Apfel
{"title":"Investigation of m- and p-xylene linked bimetallic Ni-cyclam-complexes as potential electrocatalysts for the CO2 reduction","authors":"Sarah Bimmermann , Daniel Siegmund , Kallol Ray , Ulf-Peter Apfel","doi":"10.1016/j.mtcata.2024.100058","DOIUrl":null,"url":null,"abstract":"<div><p>Among the various molecular CO<sub>2</sub> reduction catalysts, the [Ni(cyclam)]<sup>2+</sup> (<strong>Ni-{N<sub>4</sub>})</strong> complex with its earth-abundant metal center and macrocyclic ligand proved to be efficient for the selective electrochemical conversion of CO<sub>2</sub> to CO. In the present study we now connected the two Ni-cyclam units by using <em>para</em>- and <em>meta</em>-xylene as organic linkers attached to the amines of the macrocycle to form the <em><strong>p</strong></em><strong>-{Ni<sub>2</sub>} and</strong> <em><strong>m</strong></em><strong>-{Ni<sub>2</sub>}</strong> complexes, respectively, and test them as catalysts for the electrochemical CO<sub>2</sub> reduction reactions. Notably, the <em><strong>p</strong></em><strong>-{Ni<sub>2</sub>}</strong> complex demonstrates a higher faraday efficiency in the electrochemical reduction of CO<sub>2</sub> to CO compared to the <em><strong>m</strong></em><strong>-{Ni<sub>2</sub>}</strong> complex. This finding highlights the significant role played by the M-M distance in influencing this catalytic process.</p></div>","PeriodicalId":100892,"journal":{"name":"Materials Today Catalysis","volume":"6 ","pages":"Article 100058"},"PeriodicalIF":0.0000,"publicationDate":"2024-06-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2949754X24000206/pdfft?md5=b643e202f5402da26a8e5f551eaf7f0d&pid=1-s2.0-S2949754X24000206-main.pdf","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Materials Today Catalysis","FirstCategoryId":"1085","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S2949754X24000206","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"","JCRName":"","Score":null,"Total":0}
引用次数: 0
Abstract
Among the various molecular CO2 reduction catalysts, the [Ni(cyclam)]2+ (Ni-{N4}) complex with its earth-abundant metal center and macrocyclic ligand proved to be efficient for the selective electrochemical conversion of CO2 to CO. In the present study we now connected the two Ni-cyclam units by using para- and meta-xylene as organic linkers attached to the amines of the macrocycle to form the p-{Ni2} andm-{Ni2} complexes, respectively, and test them as catalysts for the electrochemical CO2 reduction reactions. Notably, the p-{Ni2} complex demonstrates a higher faraday efficiency in the electrochemical reduction of CO2 to CO compared to the m-{Ni2} complex. This finding highlights the significant role played by the M-M distance in influencing this catalytic process.
在各种二氧化碳还原分子催化剂中,[Ni(cyclam)]2+(Ni-{N4})配合物以其富集的金属中心和大环配体被证明是将二氧化碳选择性电化学转化为一氧化碳的有效催化剂。在本研究中,我们使用对二甲苯和间二甲苯作为有机连接体,将两个 Ni 环单元连接到大环的胺上,分别形成了 p-{Ni2} 和 m-{Ni2} 复合物,并将它们作为电化学 CO2 还原反应的催化剂进行了测试。值得注意的是,与 m-{Ni2} 复合物相比,p-{Ni2} 复合物在电化学还原 CO2 到 CO 的过程中表现出更高的法拉第效率。这一发现凸显了 M-M 间距在影响这一催化过程中所起的重要作用。