Modification of CO2 Reduction Activity of Nanostructured Silver Electrocatalysts by Surface Halide Anions

Hsieh, Yu -Chi; Betancourt, Luis E.; Senanayake, Sanjaya D.; Hu, Enyuan; Zhang, Yu; Xu, Wenqian; Polyansky, Dmitry E.

doi:10.1021/acsaem.8b01692

Title: Modification of CO₂ Reduction Activity of Nanostructured Silver Electrocatalysts by Surface Halide Anions

Journal Article · Wed Dec 12 00:00:00 EST 2018 · ACS Applied Energy Materials

DOI:https://doi.org/10.1021/acsaem.8b01692· OSTI ID:1491130

Hsieh, Yu -Chi ^[1]; Betancourt, Luis E. ^[1];

^[1];

^[1]; Zhang, Yu ^[1]; Xu, Wenqian ^[2];

^[1]

Brookhaven National Lab. (BNL), Upton, NY (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States); Argonne National Lab. (ANL), Argonne, IL (United States)

This study describes the effect of halide anions (X = Cl, Br, I) immobilized on the surface of nanostructured silver electrocatalysts on the efficiency and the mechanism of CO₂ reduction to CO in aqueous carbonate solutions. A simple oxidation–reduction cycle on Ag foil in the presence of halide anions produces high-surface-area nanostructured catalysts mainly composed of metallic Ag with a small amount of halide anions attached to the electrode surface (X–Ag) as demonstrated by XPS, XRD, and SEM studies. The activity of X–Ag electrocatalysts in 0.1 M NaHCO₃ at pH 6.8 is significantly higher than that of Ag foil or Ag nanoparticles with comparable surface area and morphology. The activity enhancement is attributed to the formation of active catalytic sites, presumably Cl––Ag_n⁺ clusters on the surface of metallic Ag, as evidenced by XPS analysis. The activity of X–Ag catalysts is in the order Cl > Br > I, which is consistent with the proposed model of an active site. The Tafel analysis of electrochemical CO₂ reduction points to the sensitivity of the mechanism of electrocatalysis on the nature of X.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0012704

OSTI ID:: 1491130

Report Number(s):: BNL-210859-2019-JAAM

Journal Information:: ACS Applied Energy Materials, Vol. 2, Issue 1; ISSN 2574-0962

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 44 works

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An overview on the recent developments of Ag-based electrodes in the electrochemical reduction of CO ₂ to CO Mahyoub, Samah A.; Qaraah, Fahim A.; Chen, Chengzhen Sustainable Energy & Fuels, Vol. 4, Issue 1 https://doi.org/10.1039/c9se00594c	journal	January 2020
Catalyst–Electrolyte Interactions in Aqueous Reline Solutions for Highly Selective Electrochemical CO ₂ Reduction Garg, Sahil; Li, Mengran; Rufford, Thomas E. ChemSusChem, Vol. 13, Issue 2 https://doi.org/10.1002/cssc.201903390	journal	December 2019

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Title: Modification of CO2 Reduction Activity of Nanostructured Silver Electrocatalysts by Surface Halide Anions

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Title: Modification of CO₂ Reduction Activity of Nanostructured Silver Electrocatalysts by Surface Halide Anions