Journal
CHEMISTRY-A EUROPEAN JOURNAL
Volume 26, Issue 44, Pages 9938-9944Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.202001289
Keywords
CO(2)reduction; electrocatalysis; hydrogen; pentlandite; sulfoselenides
Categories
Funding
- Deutsche Forschungsgemeinschaft (Emmy Noether grant) [AP242/2-1, AP242/6-1]
- Deutsche Forschungsgemeinschaft (Germany's Excellence Strategy-EXC-2033) [390677874]
- Fraunhofer Internal Programs [Attract 097-602175]
- Fraunhofer Cluster of Excellence CINES
- Bundesministerium fur Wirtschaft und Energie [03ET1642E]
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The electrochemical reduction of CO(2)is an attractive strategy towards the mitigation of environmental pollution and production of bulk chemicals as well as fuels by renewables. The bimetallic sulfide Fe4.5Ni4.5S8(pentlandite) was recently reported as a cheap and robust catalyst for electrochemical water splitting, as well as for CO(2)reduction with a solvent-dependent product selectivity. Inspired by numerous reports on monometallic sulfoselenides and selenides revealing higher catalytic activity for the CO(2)reduction reaction (CO2RR) than their sulfide counterparts, the authors investigated the influence of stepwise S/Se exchange in seleno-pentlandites Fe4.5Ni4.5S8-YSeY(Y=1-5) and their ability to act as CO(2)reducing catalysts. It is demonstrated that the incorporation of higher equivalents of selenium favors the CO2RR with Fe(4.5)Ni(4.5)S(4)Se(4)revealing the highest activity for CO formation. Under galvanostatic conditions in acetonitrile, Fe(4.5)Ni(4.5)S(4)Se(4)generates CO with a Faradaic Efficiency close to 100 % at applied current densities of -50 mA cm(-2)and -100 mA cm(-2). This work offers insight into the tunability of the pentlandite based electrocatalysts for the CO(2)reduction reaction.
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