Identification of a new substrate effect that enhances the electrocatalytic activity of dendritic tin in CO2 reduction

Ying Zhang, Xiaolong Zhang, Alan M. Bond, Jie Zhang

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Abstract

In this study, a selective Sn based catalytic system that electrochemically reduces CO2 to formate has been developed based on a new substrate effect. Dendritic Sn catalysts were synthesised by hydrogen gas bubble assisted electrodeposition on Pt, Cu, Sn or In substrates and applied to electrocatalytic reduction of CO2. The four substrates exhibit a hydrogen evolution activity that follows the order Pt > Cu > Sn > In. However, the Cu supported dendritic Sn catalyst provides the best selectivity towards formate formation (67.3% at -0.95 V vs. RHE). A substrate induced local pH change is proposed as the origin of formate selectivity. This was confirmed by the bulk electrolysis results obtained from two electrolyte solutions with different buffer capacities. The high buffer capacity phosphate buffer electrolyte solution provides minimal local pH change while an electrolyte with a low buffer capacity such as NaHCO3 maximises this effect to enhance the selectivity towards formate. The strategy reported here does not only focus on the catalyst, but also takes into consideration the local chemical environment. Hence, this work provides an optimal approach to improving the catalytic performance of electrocatalysts for electrochemical CO2 reduction.

Original languageEnglish
Pages (from-to)5936-5941
Number of pages6
JournalPhysical Chemistry Chemical Physics
Volume20
Issue number8
DOIs
Publication statusPublished - 2018

Cite this

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title = "Identification of a new substrate effect that enhances the electrocatalytic activity of dendritic tin in CO2 reduction",
abstract = "In this study, a selective Sn based catalytic system that electrochemically reduces CO2 to formate has been developed based on a new substrate effect. Dendritic Sn catalysts were synthesised by hydrogen gas bubble assisted electrodeposition on Pt, Cu, Sn or In substrates and applied to electrocatalytic reduction of CO2. The four substrates exhibit a hydrogen evolution activity that follows the order Pt > Cu > Sn > In. However, the Cu supported dendritic Sn catalyst provides the best selectivity towards formate formation (67.3{\%} at -0.95 V vs. RHE). A substrate induced local pH change is proposed as the origin of formate selectivity. This was confirmed by the bulk electrolysis results obtained from two electrolyte solutions with different buffer capacities. The high buffer capacity phosphate buffer electrolyte solution provides minimal local pH change while an electrolyte with a low buffer capacity such as NaHCO3 maximises this effect to enhance the selectivity towards formate. The strategy reported here does not only focus on the catalyst, but also takes into consideration the local chemical environment. Hence, this work provides an optimal approach to improving the catalytic performance of electrocatalysts for electrochemical CO2 reduction.",
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Identification of a new substrate effect that enhances the electrocatalytic activity of dendritic tin in CO2 reduction. / Zhang, Ying; Zhang, Xiaolong; Bond, Alan M.; Zhang, Jie.

In: Physical Chemistry Chemical Physics, Vol. 20, No. 8, 2018, p. 5936-5941.

Research output: Contribution to journalArticleResearchpeer-review

TY - JOUR

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AU - Zhang, Ying

AU - Zhang, Xiaolong

AU - Bond, Alan M.

AU - Zhang, Jie

PY - 2018

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N2 - In this study, a selective Sn based catalytic system that electrochemically reduces CO2 to formate has been developed based on a new substrate effect. Dendritic Sn catalysts were synthesised by hydrogen gas bubble assisted electrodeposition on Pt, Cu, Sn or In substrates and applied to electrocatalytic reduction of CO2. The four substrates exhibit a hydrogen evolution activity that follows the order Pt > Cu > Sn > In. However, the Cu supported dendritic Sn catalyst provides the best selectivity towards formate formation (67.3% at -0.95 V vs. RHE). A substrate induced local pH change is proposed as the origin of formate selectivity. This was confirmed by the bulk electrolysis results obtained from two electrolyte solutions with different buffer capacities. The high buffer capacity phosphate buffer electrolyte solution provides minimal local pH change while an electrolyte with a low buffer capacity such as NaHCO3 maximises this effect to enhance the selectivity towards formate. The strategy reported here does not only focus on the catalyst, but also takes into consideration the local chemical environment. Hence, this work provides an optimal approach to improving the catalytic performance of electrocatalysts for electrochemical CO2 reduction.

AB - In this study, a selective Sn based catalytic system that electrochemically reduces CO2 to formate has been developed based on a new substrate effect. Dendritic Sn catalysts were synthesised by hydrogen gas bubble assisted electrodeposition on Pt, Cu, Sn or In substrates and applied to electrocatalytic reduction of CO2. The four substrates exhibit a hydrogen evolution activity that follows the order Pt > Cu > Sn > In. However, the Cu supported dendritic Sn catalyst provides the best selectivity towards formate formation (67.3% at -0.95 V vs. RHE). A substrate induced local pH change is proposed as the origin of formate selectivity. This was confirmed by the bulk electrolysis results obtained from two electrolyte solutions with different buffer capacities. The high buffer capacity phosphate buffer electrolyte solution provides minimal local pH change while an electrolyte with a low buffer capacity such as NaHCO3 maximises this effect to enhance the selectivity towards formate. The strategy reported here does not only focus on the catalyst, but also takes into consideration the local chemical environment. Hence, this work provides an optimal approach to improving the catalytic performance of electrocatalysts for electrochemical CO2 reduction.

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