Photoelectrochemical reduction of CO<sub>2</sub>to HCOOH on silicon photocathodes with reduced SnO<sub>2</sub>porous nanowire catalysts

Rao, K. Ramachandra; Pishgar, Sahar; Strain, Jacob M.; Kumar, Bijandra; Atla, Veerendra; Kumari, Sudesh; Spurgeon, Joshua M.

doi:10.1039/c7ta09672k

Cited by 52 publications

(40 citation statements)

References 42 publications

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“…[18] Numerous experimental studies have focused on the selective CO 2 electroreduction to formic acid using tin dioxide nanoparticles. [19][20][21] Meyer and co-workers investigated this topic by controlling nanoparticle size and observed that a high current density of > 10 mA cm À 2 , corresponding to formate production, can be achieved at a lower overpotential of 340 meV. [22] In another study, Kumar et al discussed the activity of reduced SnO 2 nanowires towards the selectivity for HCOOH.…”

Section: Introductionmentioning

confidence: 99%

Hydride Pinning Pathway in the Hydrogenation of CO₂ to Formic Acid on Dimeric Tin Dioxide

et al. 2019

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Capture of CO2 and its conversion into organic feedstocks are increasingly needed as society moves towards a renewable energy economy. Here, a hydride‐assisted selective reduction pathway is proposed for the conversion of CO2 to formic acid (FA) over SnO2 monomers and dimers. Our density functional theory calculations infer a strong chemisorption of CO2 on SnO2 clusters forming a carbonate structure, whereas heterolytic cleavage of H2 provides a new pathway for the selective reduction of CO2 to formic acid at low overpotential. Among the two investigated pathways for reduction of CO2 to HCOOH, the hydride pinning pathway is found promising with a unique selectivity for HCOOH. The negatively‐charged hydride forms on the cluster during the dissociation of H2 and facilitates the formation of a formate intermediate, which determines the selectivity for FA over the alternative CO and H2 evolution reaction. It is confirmed that SnO2 clusters exhibit a different catalytic behaviour from their surface equivalents, thus offering promise for future work investigating the reduction of CO2 to FA via a hydride pinning pathway at low overpotential and CO2 capturing.

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Section: Introductionmentioning

confidence: 99%

Hydride Pinning Pathway in the Hydrogenation of CO₂ to Formic Acid on Dimeric Tin Dioxide

et al. 2019

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“…The Faradaic efficiency of direct CO 2 reduction at p‐Si was shown to be high when carried out in non‐aqueous electrolytes or at high pressure . To further improve the CO 2 reduction efficiency, cocatalysts such as reduced graphene oxide, Sn nanorods, silver nanowires, and gold mesh have been combined with the semiconductor. For Ag‐catalyzed CO 2 reduction, CO is regarded as a key target compound because of its favorable economics as a building block of chemicals and fuels .…”

Section: Introductionmentioning

confidence: 99%

2‐Aminobenzenethiol‐Functionalized Silver‐Decorated Nanoporous Silicon Photoelectrodes for Selective CO₂ Reduction

et al. 2020

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A molecularly thin layer of 2‐aminobenzenethiol (2‐ABT) was adsorbed onto nanoporous p‐type silicon (b‐Si) photocathodes decorated with Ag nanoparticles (Ag NPs). The addition of 2‐ABT alters the balance of the CO2 reduction and hydrogen evolution reactions, resulting in more selective and efficient reduction of CO2 to CO. The 2‐ABT adsorbate layer was characterized by Fourier transform infrared (FTIR) spectroscopy and modeled by density functional theory calculations. Ex situ X‐ray photoelectron spectroscopy (XPS) of the 2‐ABT modified electrodes suggests that surface Ag atoms are in the +1 oxidation state and coordinated to 2‐ABT via Ag−S bonds. Under visible light illumination, the onset potential for CO2 reduction was −50 mV vs. RHE, an anodic shift of about 150 mV relative to a sample without 2‐ABT. The adsorption of 2‐ABT lowers the overpotentials for both CO2 reduction and hydrogen evolution. A comparison of electrodes functionalized with different aromatic thiols and amines suggests that the primary role of the thiol group in 2‐ABT is to anchor the NH2 group near the Ag surface, where it serves to bind CO2 and also to assist in proton transfer.

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“…It is worth recognizing that higher photocurrent and lower onset potential values have generally been linked to catalytically-active materials which can overcome the high kinetic overpotential of the CO 2 reduction half-reaction, and by a lesser degree, the optical and charge transport properties of the photoelectrode. Single-junction expensive PV-grade materials such as Si (Fung et al, 2020;Hu et al, 2018;Rao et al, 2018), GaN (DuChene et al, 2018;Sekimoto et al, 2016), InP (Kaneco et al, 2006a;Kaneco et al, 2006b;Qiu et al, 2015;Zeng et al, 2015) and ZnTe (Jang et al, 2014;Jang et al, 2015) with excellent optical and charge transport properties have been extensively studied. Nevertheless, these materials possess poor catalytic sites for CO 2 reduction, which usually offer little to no redeeming improvements in the PEC activity as compared to those of more catalytically-active copper-based (Ghadimkhani et al, 2013;Won et al, 2014;de Brito et al, 2015;Kang et al, 2015;Kang and Park, 2017;Lee et al, 2018) or molecular metal-complex (Arai et al, 2011;Jeon et al, 2014;Huang et al, 2016;Kumagai et al, 2017) systems, whose activities have hitherto remained unparalleled.…”

Section: Pec Co 2 Reductionmentioning

confidence: 99%

Photo-Driven Reduction of Carbon Dioxide: A Sustainable Approach Towards Achieving Carbon Neutrality Goal

et al. 2021

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The photo-driven reduction of carbon dioxide (CO2) into green and valuable solar fuels could be a promising solution to simultaneously address energy- and environmental-related problems. This approach could play an integral role in achieving a sustainable energy economy by closing the carbon cycle and allowing the storage and transportation of intermittent solar energy within the chemical bonds of hydrocarbon molecules. This Perspective discusses the latest technological advancements in photo-driven CO2 conversion via various pathways, namely photocatalysis, photoelectrocatalysis and photovoltaic-integrated systems. In addition to providing an outlook on unresolved issues concerning the said technologies, this Perspective also spotlights new trends and strategies in the structural engineering of materials to meet the demands for prominent CO2 photoreduction activity as well as spearhead the ground-breaking advances in the field that lead to the translation of CO2 photo-driven technologies from the laboratory to industrial-scale applications.

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Photoelectrochemical reduction of CO₂to HCOOH on silicon photocathodes with reduced SnO₂porous nanowire catalysts

Abstract: High-quality Si photoelectrodes with novel Sn nanowire catalysts convert solar energy to reduce CO2 to formic acid with high selectivity.

Cited by 52 publications

References 42 publications

Hydride Pinning Pathway in the Hydrogenation of CO₂ to Formic Acid on Dimeric Tin Dioxide

Hydride Pinning Pathway in the Hydrogenation of CO₂ to Formic Acid on Dimeric Tin Dioxide

2‐Aminobenzenethiol‐Functionalized Silver‐Decorated Nanoporous Silicon Photoelectrodes for Selective CO₂ Reduction

Photo-Driven Reduction of Carbon Dioxide: A Sustainable Approach Towards Achieving Carbon Neutrality Goal

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Photoelectrochemical reduction of CO2to HCOOH on silicon photocathodes with reduced SnO2porous nanowire catalysts

Abstract: High-quality Si photoelectrodes with novel Sn nanowire catalysts convert solar energy to reduce CO2 to formic acid with high selectivity.

Cited by 52 publications

References 42 publications

Hydride Pinning Pathway in the Hydrogenation of CO2 to Formic Acid on Dimeric Tin Dioxide

Hydride Pinning Pathway in the Hydrogenation of CO2 to Formic Acid on Dimeric Tin Dioxide

2‐Aminobenzenethiol‐Functionalized Silver‐Decorated Nanoporous Silicon Photoelectrodes for Selective CO2 Reduction

Photo-Driven Reduction of Carbon Dioxide: A Sustainable Approach Towards Achieving Carbon Neutrality Goal

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Photoelectrochemical reduction of CO₂to HCOOH on silicon photocathodes with reduced SnO₂porous nanowire catalysts

Hydride Pinning Pathway in the Hydrogenation of CO₂ to Formic Acid on Dimeric Tin Dioxide

Hydride Pinning Pathway in the Hydrogenation of CO₂ to Formic Acid on Dimeric Tin Dioxide

2‐Aminobenzenethiol‐Functionalized Silver‐Decorated Nanoporous Silicon Photoelectrodes for Selective CO₂ Reduction