Publication date: 6th November 2020
The electrochemical water splitting and electrocatalytic reduction of excess CO2 are attractive strategies towards the mitigation of environmental pollution and production of bulk chemicals and fuels by renewables. Currently, bulk catalysts are either financially unfavorable or suffer from low stability and selectivity, thus decelerating the large-scale application of these technologies. The bimetallic sulfide Fe4.5Ni4.5S8 (pentlandite) was recently reported as a cheap and robust catalyst for the electrochemical water splitting, as well as for the CO2 reduction with a solvent depended product selectivity.[1],[2] Recent reports on MoS2 and CoS2 showed that monometallic sulfoselenides and selenides show higher catalytic activity for the hydrogen evolution (HER) and CO2 reduction reaction (CO2RR) than their sulfide counterparts.[3],[4] We thus investigated the effect of successive substitution of sulfur with selenium within the pentlandite system and on the electrocatalytic activity of the catalyst for the two reductions reactions. Herein, the successful synthesis and characterization of the seleno‑pentlandites Fe4.5Ni4.5S8‑YSeY (Y=1‑5) as potential HER and CO2 reducing catalysts is reported. Under acidic HER conditions, the sulfoselenide Fe4.5Ni4.5S7Se1 outperforms the reference material, whereas higher selenium‑equivalents (Y=2-5) gradually lower the HER activity of the materials.[5] In contrast to the reduced HER activity, the incorporation of higher selenium equivalents, favors the CO2RR in organic solvent, with Fe4.5Ni4.5S4Se4 showing the highest activity, possessing almost a twofold higher selectivity and partial current density than Fe4.5Ni4.5S8 for CO formation. The increased activity is attributed to the increase of interatomic distances in the enlarged crystal lattice and to a synergistic effect between the two chalcogens in the catalytic active center. This work offers an insight on the tunability of pentlandite system based electrocatalysts, for the HER and CO2RR via S/Se substitution.
This work was supported by the Fonds der Chemischen Industrie (Liebig grant to U.-P.A.), the Deutsche
Forschungsgemeinschaft (Emmy Noether grant, AP242/2-1 and AP242/6-1) as well as the Fraunhofer
Internal Programs under Grant No. Attract 097-602175.
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