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Electrolyte Effects in Ni–N–C Single-Metal-Site-Catalyzed Electrochemical CO2 Reduction
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DOI：10.1021/acscatal.6c02673.png)
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Abstract
En 中文
The catalytic performance of the electrochemical CO2 reduction reaction (CO2RR) is highly sensitive to the electrolyte microenvironment, including ion identity, concentration, and buffering chemistry. While such electrolyte effects are well established for metallic catalysts, their mechanistic roles in porous Ni–N–C systems remain less explored. Here, we systematically investigate the influence of cation (Li+, K+, Cs+, and tetramethylammonium, TMA+) and anion (phosphate, sulfate, and bicarbonate) identity and concentration on CO2-to-CO conversion. Contrary to expectations, Cs+ does not outperform K+, whereas TMAHCO3 electrolytes exhibit a pronounced enhancement in CO2RR activity, reaching a CO partial current density of 25 mA cm–2 at –0.7 VRHE in 0.5 M solution. Electrochemical impedance spectroscopy (EIS) and distribution of relaxation times (DRT) analysis reveal that this activity enhancement does not directly correlate with interfacial ion-/charge-transfer or mass transport behaviors. Instead, Fourier-transform infrared (FTIR) spectroscopy shows a significant increase in bulk CO2 availability in TMAHCO3 electrolytes. Overall, these results suggest that electrolyte composition affects both interfacial properties and CO2 availability in the bulk, influencing CO2RR activity within the porous Ni–N–C catalyst system.
Keywords:
Catalysts
Cations
Electrolytes
Inorganic carbon compounds
Oxides
electrochemical CO2 reduction
Ni–N–C catalysts
electrolyte microenvironment
electrochemical impedance spectra
interfacial kinetics
bulk CO2 availability
Journal
IF:
13.1
Papers:
1.6W
Citations:
15.0W
Organization
Cited Papers