4.5 Article

Chemical Method for Evaluating Catalytic Turnover Frequencies (TOF) of Moderate to Slow H2 Oxidation Electrocatalysts

期刊

ORGANOMETALLICS
卷 38, 期 6, 页码 1311-1316

出版社

AMER CHEMICAL SOC
DOI: 10.1021/acs.organomet.8b00580

关键词

-

资金

  1. Indian Institute of Technology (IIT) Gandhinagar

向作者/读者索取更多资源

Hydrogen has emerged as a long-term option for storing energy from renewable resources and has led the scientific community to develop enzyme-inspired catalysts for hydrogen oxidation and production. One of the most productive families of catalysts for H-2 oxidation is the pendant amine containing bis(diphosphine)nickel catalysts. Many derivatives of these nickel complexes have been prepared with varying peripheral functionalities to understand their structure-function relationship. Electrocatalysis is currently utilized as the primary tool to measure the catalytic turnover frequencies (TOFs) of these complexes; however, it does not allow accurate determination of TOFs for slow (<1 s(-1)) to moderately active (similar to 1-10 s(-1)) catalysts, and for the slowest catalysts, it can be difficult to determine if they are turning over at all. Further, it does not allow the determination of the TOF in bulk solution. In this work, we demonstrate that a redox chemical procedure involving a change between ferrocenium cation and ferrocene can be utilized to monitor H-2 oxidation catalysts. The ferrocenium cation reoxidizes the reduced nickel catalyst stoichiometrically in the presence of H-2. The change of ferrocenium cation to ferrocene can be monitored in both organic and aqueous solvents via either optical spectroscopy or NMR spectroscopy. Thus, this chemical method complements the existing electrocatalytic procedure and may help to unravel the intricate details of even the slowest H-2 oxidation catalysts.

作者

我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。

评论

主要评分

4.5
评分不足

次要评分

新颖性
-
重要性
-
科学严谨性
-
评价这篇论文

推荐

暂无数据
暂无数据