Journal
ADVANCED FUNCTIONAL MATERIALS
Volume 30, Issue 24, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adfm.201910118
Keywords
Ar plasma treatment; copper nanoparticles; electrochemical CO2 reduction; intrinsic carbon defects; vertical graphene
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Funding
- Australian Research Council (ARC) under the Laureate Fellowship Scheme [FL140100081]
- Australian Government
- CSC (China Scholarship Council) - UNSW (University of New South Wales) joint scholarship (CSC) [201706150042]
- UNSW Scientia Ph.D. Scholarship
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Defective 3D vertical graphene (VG) with a relatively large surface area, high defect density, and increased surface electrons is synthesized via a scalable plasma enhanced chemical vapor deposition method, together with a postsynthesis Ar-plasma treatment (VG-Ar). Subsequently, Cu@CuxO nanoparticles are deposited onto VG-Ar (Cu/VG-Ar) through a galvanostatic pulsed electrodeposition method. These Cu@CuxO nanocatalyst systems exhibit a superior electrochemical CO2 reduction performance when compared to Cu-based catalysts supported on commercial graphene paper or pristine VG without postsynthesis Ar-plasma treatment. The Cu/VG-Ar achieves the highest CO2 reduction Faradaic efficiency of 60.6% (83.5% of which are attributed to liquid products, i.e., formate, ethanol, and n-propanol) with a 5.6 mA cm(-2) partial current density at -1.2 V versus reversible hydrogen electrode (RHE). The improved CO2 reduction performance of Cu/VG-Ar originates from the well-dispersed Cu@CuxO nanoparticles deposited on the defective VG-Ar. The intrinsic carbon defects on VG-Ar can suppress the hydrogen evolution reaction as well as tune the interaction between VG and Cu@CuxO, thus impeding the excessive oxidation of Cu2O species deposited on VG-Ar. The defective VG-Ar and stabilized Cu@CuxO enhances CO2 adsorption and promotes electron transfer to the adsorbed CO2 and intermediates on the catalyst surface, thus improving the overall CO2 reduction performance.
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