Low-Energy Electrocatalytic CO2 Reduction in Water over Mn-Complex Catalyst Electrode Aided by a Nanocarbon Support and K+ Cations
Shunsuke Sato, Kenichiro Saita, Keita Sekizawa, Satoshi Maeda, Takeshi Morikawa
Index: 10.1021/acscatal.8b01068
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Abstract
Electrocatalytic CO2 reduction over a Mn-complex catalyst in an aqueous solution was achieved at very low energy with a combination of multiwalled carbon nanotubes (MWCNTs) and K+ cations. Although the bare Mn-complex did not function as a catalyst in an aqueous solution, the combined Mn-complex/MWCNT cathode promoted electrocatalytic CO2 reduction at an overpotential of 100 mV where neither the bare MWCNTs nor bare Mn-complex were catalytically active. The Mn-complex/MWCNT produced CO at a constant rate for 48 h with a current density of greater than 2.0 mA cm–2 at −0.39 V (vs RHE). The MWCNTs with electron accumulation properties, together with surface adsorbed K+ ions, provided an environment to stabilize CO2 adjacent to the Mn-complex and significantly lowered the overpotential for CO2 reduction in an aqueous solution, and these results were consistent with density functional theory (DFT) calculations. Experiments clarified that the synergetic effect of the MWCNTs and K+ ions was also applicable to Co and Re complexes that were almost inert with regard to CO2 reduction in an aqueous solution.