HKUST-1-derived highly ordered Cu nanosheets with enriched edge sites, stepped (211) surfaces and (200) facets for effective electrochemical CO2 reduction

Abstract

A novel electrode composed of Cu nanosheets constructed from nanoparticles was synthesized by in situ electrochemical derivation from the metal-organic framework (MOF) HKUST-1. The prepared derivative electrode (HE-Cu) exhibited higher Faradaic efficiency (FE, 56.0%) of electrochemical CO2 reduction (CO2R) compared with that of pristine Cu foil (p-Cu, 32.3%) at an overpotential of −1.03 V vs. a reversible hydrogen electrode (RHE). HE-Cu also exhibited lower onset potential of CO2R as well as inhibiting the H2 evolution reaction. Electrochemical measurements revealed that HE-Cu exhibited higher CO2 adsorption (1.58-fold) and a larger electrochemical active surface area (1.24-fold) compared with p-Cu. Physicochemical characterization and Tafel analysis showed that stepped Cu (211) surfaces, (200) facets and Cu edge atoms on HE-Cu contributed significantly to the enhanced CO2R activity and/or HCOOH and/or C2 product selectivity. The FEs of HCOOH and C2 products for HE-Cu increased 1.57-fold and 10.6-fold at an overpotential of −1.19 V vs. RHE compared with p-Cu. Although CH4 was produced on p-Cu, its formation was totally suppressed on HE-Cu due to the increase of edge sites and (200) facets. Our study demonstrates that electroreduction of MOFs is a promising method to prepare novel and stable electrochemical catalysts with unique surface structures. The fabricated derivative electrode not only promoted electrochemical CO2R activity but also exhibited high C2 product selectivity.