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Impact of the Dissolved Anion on the Electrocatalytic Reduction of CO 2 to CO with Ruthenium CNC Pincer Complexes
Author(s) -
Shirley Hunter,
Figgins Matthew T.,
Boudreaux Chance M.,
Liyanage Nalaka P.,
Lamb Robert W.,
Webster Charles Edwin,
Papish Elizabeth T.,
Delcamp Jared H.
Publication year - 2020
Publication title -
chemcatchem
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.497
H-Index - 106
eISSN - 1867-3899
pISSN - 1867-3880
DOI - 10.1002/cctc.202000742
Subject(s) - ruthenium , electrocatalyst , chemistry , catalysis , inorganic chemistry , electrolysis , pincer movement , halide , chloride , electrochemistry , selectivity , faraday efficiency , photochemistry , electrode , organic chemistry , electrolyte
Abstract The reactivity of three ruthenium electrocatalysts is shown to be modulated through the addition of anions for more selective and faster electrocatalysis. Controlled potential electrolysis studies confirm the generation of CO from CO 2 . The Faradaic efficiency increased for the three ruthenium catalysts studied through the introduction of Cl – to the reaction solution. Interestingly, a neutral ruthenium coordination complex with an associated chloride also gave equal or faster rates of catalysis upon Cl − addition. In this report, a systematic study on the effects of added halides (I − , Br − , Cl − , and F − ) with varied counter cations (K + and TBA + ) with and without water is examined. Computational analysis provides insights into this interesting increase in FE based on anion addition. These results show anion addition to electrocatalysis reaction mixtures add an additional parameter to increase both rate and selectivity of catalysis with one example improving from 19 % FE to 91 % FE for CO production.