Catalytic CO2 Reduction Using an Atomically Precise, Cu-Coordinated, Crystalline Carbon Nitride

17 May 2023, Version 1

Abstract

Inherently disordered structures of carbon nitrides have hindered an atomic level tunability and understanding of their catalytic reactivity. Herein, coordination of copper cations within a crystalline carbon nitride, i.e., poly(triazine imide) or CNx, was found to yield two ordered structures for Cu-CNx wherein one or two Cu(I) cations coordinate to its intralayer N-triazine groups. The crystallites electrophoretically deposit from aqueous particle suspensions and yield current densities of ~10 to 50 mA/cm2 with a concomitant and increasing reduction of CO2 and H2O. Reduction of CO2 increases for smaller particles as mechanistic calculations reveal its catalysis mediated by two intralayer Cu atoms.

Keywords

CO2 Reduction
Carbon Nitride
Copper Catalysis

Supplementary materials

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Supporting Information
Description
Experimental and computational procedures, Rietveld refinements, elemental analysis, FT-IR, UV-Vis DRS, CO2R product distributions, frontier molecular orbitals of intermediates, and reaction coordinate diagram.
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