Chloroplast-mimicking nanoreactor for enhanced CO2 electrocatalysis (IMAGE)
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In this paper, the authors reported the construction of a catalytic nanoreactor capable of achieving the highly selective and efficient reduction of CO2 to CO by mimicking chloroplasts in green plants. The chloroplast-mimicking nanoreactor is facilely obtained through the self-assembly of cetyltrimethylammonium bromide (CTAB) bilayer on the surface of a gold nanorod (GNR) electrocatalyst to form a core-shell structure. The CTAB bilayer mimics the chloroplast membrane to allow the simultaneous regulation of the transport of CO2 and protons to the GNR core and the GNR core imitates Rubisco enzymes to catalyze CO2 reduction reaction. Consequently, the selectivity of CO2 reduction to CO has been greatly enhanced.
Fig. 2. DFT investigation, structural characterization, Operando attenuated total reflection Fourier transform infrared spectroscopy (ATR-FTIR) and electrocatalytic performances of different catalysts for CO2RR. (a) Computational model of CO2-to-CO conversion experiencing six steps as labeled and described in the main text. (b) Calculated relative energy and ∠OCO angle at different states. (c) High-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) image of CMNR. (d) LSV curves of the CMNR and bare GNR catalysts in CO2-saturated 0.5 mol L-1 KHCO3 electrolyte. (e) The FECO of the CMNR and bare GNR catalysts at different applied potentials. (f) The FECO and FEH2 of CMNR catalysts modified with bipolar organic molecules with different anions at –0.57 V vs. Reversible Hydrogen Electrode (RHE). (g) Operando ATR-FTIR spectra of bare GNR and CMNR catalysts at open circuit potential in CO2-staturated 0.5 mol L-1 KHCO3 electrolyte. (h) Energy profile associated with the transfer of different H-forms, including H2O, H3O+, HBr, and HCO2+. O, C, H, Br, and Au are shown as red, grey, white, maroon, and yellow sticks or balls. The proton of interest is highlighted by the green line.
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