Journal
ACS CATALYSIS
Volume 12, Issue 21, Pages 13533-13541Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.2c02617
Keywords
CO2 electroreduction; SnS; heteroatom doping; catalyst stability; in situ Raman spectroscopy; electronic state modulation
Categories
Funding
- National Natural Science Foundation of China
- [52001227]
- [52122107]
- [51972224]
- [52231008]
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Heteroatom doping is a strategy to optimize the activity and stability of electrocatalysts for the CO2RR. In this study, In doping was proposed to reinforce the S atoms in SnS, inhibiting sulfur dissolution and optimizing the reaction pathway.
Heteroatom doping can facilitate intrinsic activity via the tuning of electronic states. However, it is still rare to elucidate the role of a specific metal sulfide electronic state and simultaneously enhance the CO2 electroreduction reaction (CO2RR) stability. SnS is well-known for its ability to produce HCOOH; however, its long-term operational stability is limited by sulfur dissolution. Herein, we propose a strategy to reinforce the S atoms via heteroatom (In) doping. In situ Raman tests and theoretical calculations demonstrate that In atoms with fewer valence electrons (compared with Sn) can tune the electronic state of SnS and strengthen the S-metal bond energy. Consequently, sulfur dissolution was inhibited, and the reaction pathway was optimized. Further, the In-SnS/C achieves a Faradaic efficiency of 96.6% for formate at -0.6 V vs RHE and a catalyst stability of 50 h at a current density of similar to 37 mA cm(-2). This study shows that altering the electronic structure of SnS via heteroatoms is a strategy to optimize both the activity and stability of electrocatalysts for the CO2RR.
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