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A facile strategy to boost the activity and preserve the selectivity of CO2 reduction to formate using organic‐functionalized metal catalysts, specifically 2‐methyl‐imidazole coordinated to Bi, Bi[2‐MeIm], is reported, and the active surfaces are investigated during structural transformation under the applied cathodic potential necessary for CO2 reduction. Operando Raman spectroscopy unveils the structure...
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