Electrolyte Competition Controls Surface Binding of CO Intermediates to CO2 Reduction Catalysts

2021 ◽  
Author(s):  
Anna Wuttig ◽  
Jaeyune Ryu ◽  
Yogesh Surendranath
Keyword(s):  
Co2 Reduction ◽  
Surface Binding ◽  
Reduction Catalysts

Electrolyte Competition Controls Surface Binding of CO Intermediates to CO2 Reduction Catalysts

2019 ◽  
Author(s):  
Anna Wuttig ◽  
Jaeyune Ryu ◽  
Yogesh Surendranath
Keyword(s):  
Variable Temperature ◽  
Co Adsorption ◽  
Co2 Reduction ◽  
Adsorbed Water ◽  
Fine Tuning ◽  
Design Parameters ◽  
Surface Binding ◽  
Cu Catalysts ◽  
Reduction Catalysts

Adsorbed CO is a critical intermediate in the electrocatalytic reduction of CO<sub>2</sub> to fuels. Contemporary methods for probing the thermodynamics of CO adsorption ignore the role of the electrolyte. Using in situ infrared spectroelectrochemistry, we disclose the contrasting influence of electrolyte competition on reversible CO binding to Au and Cu catalysts. Whereas reversible CO binding to Au surfaces is driven by substitution and reorientation of adsorbed water, CO binding to Cu requires the reductive displacement of adsorbed carbonate anions. Through variable temperature studies, we find that CO binding to Cu is enthalpically favored by ~36 kJ mol<sup>–1</sup> relative to CO adsorption on Au. The divergent CO adsorption stoichiometry on Au and Cu explains their disparate reactivity: water adsorption drives CO liberation from Au surfaces, impeding further reduction, whereas carbonate desorption drives CO accumulation on Cu, allowing for further reduction to hydrocarbons. These studies provide direct insight into how electrolyte constituents can serve as powerful design parameters for fine-tuning of CO surface populations and, thereby, CO2-to-fuels reactivity. <br>

Frontispiece: Judicious Ligand Design in Ruthenium Polypyridyl CO2 Reduction Catalysts to Enhance Reactivity by Steric and Electronic Effects

2016 ◽  
Vol 22 (42) ◽  
Author(s):  
Ben A. Johnson ◽  
Hemlata Agarwala ◽  
Travis A. White ◽  
Edgar Mijangos ◽  
Somnath Maji ◽  
...  
Keyword(s):  
Co2 Reduction ◽  
Ligand Design ◽  
Electronic Effects ◽  
Ruthenium Polypyridyl ◽  
Reduction Catalysts

Electrocatalytic CO2 reduction with nickel complexes supported by tunable bipyridyl-N-heterocyclic carbene donors: understanding redox-active macrocycles

2018 ◽  
Vol 54 (27) ◽  
pp. 3351-3354 ◽  
Author(s):  
Xiaojun Su ◽  
Kaitlin M. McCardle ◽  
Julien A. Panetier ◽  
Jonah W. Jurss
Keyword(s):  
Co2 Reduction ◽  
Nickel Complexes ◽  
Structure Activity Relationship ◽  
Activity Relationship ◽  
Structure Activity ◽  
Redox Active ◽  
Reduction Catalysts ◽  
Insight Into

A structure–activity relationship, revealed through a series of nickel-based CO2 reduction catalysts, provides insight into the role of redox-active macrocycles.

scholarly journals Publisher Correction: The role of reticular chemistry in the design of CO2 reduction catalysts

2018 ◽  
Vol 17 (10) ◽  
pp. 943-943 ◽  
Author(s):  
Christian S. Diercks ◽  
Yuzhong Liu ◽  
Kyle E. Cordova ◽  
Omar M. Yaghi
Keyword(s):  
Co2 Reduction ◽  
Reduction Catalysts

CO2 Reduction Catalysts on Gold Electrode Surfaces Influenced by Large Electric Fields

2018 ◽  
Vol 140 (50) ◽  
pp. 17643-17655 ◽  
Author(s):  
Melissa L. Clark ◽  
Aimin Ge ◽  
Pablo E. Videla ◽  
Benjamin Rudshteyn ◽  
Christopher J. Miller ◽  
...  
Keyword(s):  
Electric Fields ◽  
Gold Electrode ◽  
Co2 Reduction ◽  
Electrode Surfaces ◽  
Reduction Catalysts

scholarly journals Tuning redox potentials of CO2 reduction catalysts for carbon photofixation by Si nanowires

2015 ◽  
Vol 58 (7) ◽  
pp. 515-520 ◽  
Author(s):  
Rui Liu ◽  
Carolynn Stephani ◽  
Kian L. Tan ◽  
Dunwei Wang
Keyword(s):  
Co2 Reduction ◽  
Redox Potentials ◽  
Si Nanowires ◽  
Reduction Catalysts
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