Dataset Information

Facet-Dependent Selectivity of Cu Catalysts in Electrochemical CO2 Reduction at Commercially Viable Current Densities.

ABSTRACT: Despite substantial progress in the electrochemical conversion of CO2 into value-added chemicals, the translation of fundamental studies into commercially relevant conditions requires additional efforts. Here, we study the catalytic properties of tailored Cu nanocatalysts under commercially relevant current densities in a gas-fed flow cell. We demonstrate that their facet-dependent selectivity is retained in this device configuration with the advantage of further suppressing hydrogen production and increasing the faradaic efficiencies toward the CO2 reduction products compared to a conventional H-cell. The combined catalyst and system effects result in state-of-the art product selectivity at high current densities (in the range 100-300 mA/cm2) and at relatively low applied potential (as low as -0.65 V vs RHE). Cu cubes reach an ethylene selectivity of up to 57% with a corresponding mass activity of 700 mA/mg, and Cu octahedra reach a methane selectivity of up to 51% with a corresponding mass activity of 1.45 A/mg in 1 M KOH.

SUBMITTER: De Gregorio GL

PROVIDER: S-EPMC7199425 | biostudies-literature | 2020 May

REPOSITORIES: biostudies-literature

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Publications

Facet-Dependent Selectivity of Cu Catalysts in Electrochemical CO<sub>2</sub> Reduction at Commercially Viable Current Densities.

De Gregorio Gian Luca GL Burdyny Thomas T Loiudice Anna A Iyengar Pranit P Smith Wilson A WA Buonsanti Raffaella R

ACS catalysis 20200327 9

Despite substantial progress in the electrochemical conversion of CO<sub>2</sub> into value-added chemicals, the translation of fundamental studies into commercially relevant conditions requires additional efforts. Here, we study the catalytic properties of tailored Cu nanocatalysts under commercially relevant current densities in a gas-fed flow cell. We demonstrate that their facet-dependent selectivity is retained in this device configuration with the advantage of further suppressing hydrogen ...[more]

PMID: 32391186

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Project description:Metal-organic frameworks (MOFs) have been an excellent platform for carbon dioxide reduction reactions (CO2RR). In this work, the feasibility of electrochemical reduction of CO2 to obtain C2-deep value-added products was investigated by the preparation of Mg-containing MOF-74 samples combined with transition metal cations (Ni2+, Co2+ and Zn2+). The prepared MOFs were used as electrocatalysts in CO2RR. Chronoamperometric analysis coupled to ATR-FTIR spectroscopy was employed to characterize the CO2 reduction products and subsequently via 1H NMR. Although an isostructural crystalline structure was observed in all synthesized MOFs, the pore diameter distribution was significantly affected due to the Mg coordination along with each transition metal nuclei with the organic ligand to form the MOF-74. Our results showed that Mg-containing MOF-74 electrocatalysts combined with Ni, Co and Zn ions successfully reduced CO2 to C2-deep products, while the monometallic Mg-MOF-74 showed only CO2 mineralization. An ester acetate, isopropyl alcohol, and formic acid were produced by Mg/Ni-MOF-74; isopropyl alcohol was provided by Mg/Co-MOF-74, and ethanol was generated by Mg/Zn-MOF-74. We observed that the change of the transition cation was a key factor in the selectivity of the obtained products, while the degree of Mg ions effectively incorporated into the MOF structure tuned the porosity and the electrocatalytic activity. Among them, Mg/Zn-MFOF-74 showed the highest Mg content loaded after synthesis and thus the most favorable electrocatalytic behavior towards CO2 reduction. Highlights • CO2-derived C2-deep reduction products were obtained by Mg-containing MOF-74 bimetallic electrocatalysts.• Mg-containing MOF-74 bimetallic electrocatalysts reduced CO2 to ester acetate, isopropanol, formic acid, and ethanol.• Mg/Zn-MOF-74 displayed the highest current density at a lower onset potential in CO2-saturated electrolyte.• The pore network could be tuned by the effective Mg content on a MOF-74 bimetallic sample.• Mg/Zn-MOF-74 showed the highest Mg content among all bimetallic electrocatalysts after the synthesis.

Dataset Information

Facet-Dependent Selectivity of Cu Catalysts in Electrochemical CO2 Reduction at Commercially Viable Current Densities.

Publications

Facet-Dependent Selectivity of Cu Catalysts in Electrochemical CO<sub>2</sub> Reduction at Commercially Viable Current Densities.

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