Design of robust 2,2′-bipyridine ligand linkers for the stable immobilization of molecular catalysts on silicon(111) surfaces

Johnson, Samantha I.; Blakemore, James D.; Brunschwig, Bruce S.; Lewis, Nathan S.; Gray, Harry B.; Goddard, William A.; Persson, Petter

doi:10.1039/d1cp00545f

Cited by 6 publications

(1 citation statement)

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“…Si is an attractive semiconducting support because it is abundant, inexpensive, able to absorb light and separate charge, and its surface chemistry and electronic properties are well-studied . Nevertheless, reports of the immobilization of molecular catalysts on planar Si wafers are rare, and these systems often give poor and irreproducible catalytic performance due to their reactivity with oxygen, low surface area, modest catalyst surface coverages, and thus low activity …”

Section: Introductionmentioning

confidence: 99%

Photoelectrochemical CO₂ Reduction to CO Enabled by a Molecular Catalyst Attached to High-Surface-Area Porous Silicon

Jia,

Stewart-Jones,

Alvarez-Hernandez

et al. 2024

J. Am. Chem. Soc.

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A high-surface-area p-type porous Si photocathode containing a covalently immobilized molecular Re catalyst is highly selective for the photoelectrochemical conversion of CO 2 to CO. It gives Faradaic efficiencies of up to 90% for CO at potentials of −1.7 V (versus ferrocenium/ferrocene) under 1 sun illumination in an acetonitrile solution containing phenol. The photovoltage is approximately 300 mV based on comparisons with similar n-type porous Si cathodes in the dark. Using an estimate of the equilibrium potential for CO 2 reduction to CO under optimized reaction conditions, photoelectrolysis was performed at a small overpotential, and the onset of electrocatalysis in cyclic voltammograms occurred at a modest underpotential. The porous Si photoelectrode is more stable and selective for CO production than the photoelectrode generated by attaching the same Re catalyst to a planar Si wafer. Further, facile characterization of the porous Si-based photoelectrodes using transmission mode FTIR spectroscopy leads to highly reproducible catalytic performance.

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Section: Introductionmentioning

confidence: 99%

Photoelectrochemical CO₂ Reduction to CO Enabled by a Molecular Catalyst Attached to High-Surface-Area Porous Silicon

Jia,

Stewart-Jones,

Alvarez-Hernandez

et al. 2024

J. Am. Chem. Soc.

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Electrocatalytic Hydrogen Evolution Using A Molecular Antimony Complex under Aqueous Conditions: An Experimental and Computational Study on Main‐Group Element Catalysis

Williams

McCarver

Chaturvedi

et al. 2022

Chemistry A European J

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Electrocatalytic hydrogen gas production is considered a potential pathway towards carbon-neutral energy sources. However, the development of this technology is hindered by the lack of efficient, cost-effective, and environmentally benign catalysts. In this study, a main-groupelement-based electrocatalyst, SbSalen, is reported to catalyze the hydrogen evolution reaction (HER) in an aqueous medium. The heterogenized molecular system achieved a Faradaic efficiency of 100 % at À 1.4 V vs. NHE with a maximum current density of À 30.7 mA/cm 2 . X-ray photoelectron spectroscopy of the catalyst-bound working electrode before and after electrolysis confirmed the molecular stability during catalysis. The turnover frequency was calculated as 43.4 s À 1 using redox-peak integration. The kinetic and mechanistic aspects of the electrocatalytic reaction were further examined by computational methods. This study provides mechanistic insights into main-group-element electrocatalysts for heterogeneous small-molecule conversion.

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Synthesis and Chemosensory Properties of New Cyanosubstituted 2,2'-Bipyridine Derivatives

et al. 2022

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Design of robust 2,2′-bipyridine ligand linkers for the stable immobilization of molecular catalysts on silicon(111) surfaces

Abstract: The attachment of the 2,2´-bipyridine (bpy) moieties to the surface of planar silicon(111) (photo)electrodes was investigated using ab initio simulations performed on a new cluster model for methyl-terminated silicon. Density...

Cited by 6 publications

References 76 publications

Photoelectrochemical CO₂ Reduction to CO Enabled by a Molecular Catalyst Attached to High-Surface-Area Porous Silicon

Photoelectrochemical CO₂ Reduction to CO Enabled by a Molecular Catalyst Attached to High-Surface-Area Porous Silicon

Electrocatalytic Hydrogen Evolution Using A Molecular Antimony Complex under Aqueous Conditions: An Experimental and Computational Study on Main‐Group Element Catalysis

Synthesis and Chemosensory Properties of New Cyanosubstituted 2,2'-Bipyridine Derivatives

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Design of robust 2,2′-bipyridine ligand linkers for the stable immobilization of molecular catalysts on silicon(111) surfaces

Abstract: The attachment of the 2,2´-bipyridine (bpy) moieties to the surface of planar silicon(111) (photo)electrodes was investigated using ab initio simulations performed on a new cluster model for methyl-terminated silicon. Density...

Cited by 6 publications

References 76 publications

Photoelectrochemical CO2 Reduction to CO Enabled by a Molecular Catalyst Attached to High-Surface-Area Porous Silicon

Photoelectrochemical CO2 Reduction to CO Enabled by a Molecular Catalyst Attached to High-Surface-Area Porous Silicon

Electrocatalytic Hydrogen Evolution Using A Molecular Antimony Complex under Aqueous Conditions: An Experimental and Computational Study on Main‐Group Element Catalysis

Synthesis and Chemosensory Properties of New Cyanosubstituted 2,2'-Bipyridine Derivatives

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Product

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Photoelectrochemical CO₂ Reduction to CO Enabled by a Molecular Catalyst Attached to High-Surface-Area Porous Silicon

Photoelectrochemical CO₂ Reduction to CO Enabled by a Molecular Catalyst Attached to High-Surface-Area Porous Silicon