High efficiency electrochemical reduction of CO2 beyond the two-electron transfer pathway on grain boundary rich ultra-small SnO2 nanoparticles

Chenglu Liang; Byoungsu Kim; Shize Yang; Liu Yang Liu; Cristiano Francisco Woellner; Zhengyuan Li; Robert Vajtai; Wei Yang; Jingjie Wu; Paul J.A. Kenis; Pulickel M. Ajayan

doi:10.1039/c8ta01367e

High efficiency electrochemical reduction of CO₂ beyond the two-electron transfer pathway on grain boundary rich ultra-small SnO₂ nanoparticles

Chenglu Liang, Byoungsu Kim, Shize Yang, Liu Yang Liu, Cristiano Francisco Woellner, Zhengyuan Li, Robert Vajtai, Wei Yang, Jingjie Wu, Paul J.A. Kenis, Pulickel M. Ajayan

Research output: Contribution to journal › Article › peer-review

Abstract

Well crystallized and interconnected SnO₂ nanoparticles (<5 nm) were synthesized via oxidation of exfoliated SnS₂ sheets. The SnO₂ nanoparticles exhibit a high total faradaic efficiency (FE) of 97% towards electrochemical reduction of CO₂ at -0.95 V vs. the reversible hydrogen electrode (RHE). The main product ratio of CO/HCOO^- which intrinsically correlates to the surface SnO_x/Sn ratio variation varies with the applied potential. Beyond CO and HCOO^- products formed via the two-electron transfer pathway, hydrocarbons and oxygenates are produced. The formation of hydrocarbon (CH₄) versus oxygenate (C₂H₅OH) depends on the choice of electrolyte (KOH vs. KHCO₃), both of which can reach a maximal faradaic efficiency of 10%. The distinctive grain boundary and exposed corner/step sites in the interconnected SnO₂ nanoparticles contribute to the high FE of CO₂ reduction and unique selectivity.

Original language	English (US)
Pages (from-to)	10313-10319
Number of pages	7
Journal	Journal of Materials Chemistry A
Volume	6
Issue number	22
DOIs	https://doi.org/10.1039/c8ta01367e
State	Published - 2018

ASJC Scopus subject areas

General Chemistry
Renewable Energy, Sustainability and the Environment
General Materials Science

Online availability

10.1039/c8ta01367e

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Cite this

Liang, C., Kim, B., Yang, S., Yang Liu, L., Francisco Woellner, C., Li, Z., Vajtai, R., Yang, W., Wu, J., Kenis, P. J. A., & Ajayan, P. M. (2018). High efficiency electrochemical reduction of CO₂ beyond the two-electron transfer pathway on grain boundary rich ultra-small SnO₂ nanoparticles. Journal of Materials Chemistry A, 6(22), 10313-10319. https://doi.org/10.1039/c8ta01367e

Liang, C, Kim, B, Yang, S, Yang Liu, L, Francisco Woellner, C, Li, Z, Vajtai, R, Yang, W, Wu, J, Kenis, PJA & Ajayan, PM 2018, 'High efficiency electrochemical reduction of CO₂ beyond the two-electron transfer pathway on grain boundary rich ultra-small SnO₂ nanoparticles', Journal of Materials Chemistry A, vol. 6, no. 22, pp. 10313-10319. https://doi.org/10.1039/c8ta01367e

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title = "High efficiency electrochemical reduction of CO2 beyond the two-electron transfer pathway on grain boundary rich ultra-small SnO2 nanoparticles",

abstract = "Well crystallized and interconnected SnO2 nanoparticles (<5 nm) were synthesized via oxidation of exfoliated SnS2 sheets. The SnO2 nanoparticles exhibit a high total faradaic efficiency (FE) of 97% towards electrochemical reduction of CO2 at -0.95 V vs. the reversible hydrogen electrode (RHE). The main product ratio of CO/HCOO- which intrinsically correlates to the surface SnOx/Sn ratio variation varies with the applied potential. Beyond CO and HCOO- products formed via the two-electron transfer pathway, hydrocarbons and oxygenates are produced. The formation of hydrocarbon (CH4) versus oxygenate (C2H5OH) depends on the choice of electrolyte (KOH vs. KHCO3), both of which can reach a maximal faradaic efficiency of 10%. The distinctive grain boundary and exposed corner/step sites in the interconnected SnO2 nanoparticles contribute to the high FE of CO2 reduction and unique selectivity.",

author = "Chenglu Liang and Byoungsu Kim and Shize Yang and {Yang Liu}, Liu and {Francisco Woellner}, Cristiano and Zhengyuan Li and Robert Vajtai and Wei Yang and Jingjie Wu and Kenis, {Paul J.A.} and Ajayan, {Pulickel M.}",

note = "Publisher Copyright: {\textcopyright} The Royal Society of Chemistry 2018.",

year = "2018",

doi = "10.1039/c8ta01367e",

language = "English (US)",

volume = "6",

pages = "10313--10319",

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AU - Liang, Chenglu

AU - Kim, Byoungsu

AU - Yang, Shize

AU - Yang Liu, Liu

AU - Francisco Woellner, Cristiano

AU - Li, Zhengyuan

AU - Vajtai, Robert

AU - Yang, Wei

AU - Wu, Jingjie

AU - Kenis, Paul J.A.

AU - Ajayan, Pulickel M.

PY - 2018

Y1 - 2018

N2 - Well crystallized and interconnected SnO2 nanoparticles (<5 nm) were synthesized via oxidation of exfoliated SnS2 sheets. The SnO2 nanoparticles exhibit a high total faradaic efficiency (FE) of 97% towards electrochemical reduction of CO2 at -0.95 V vs. the reversible hydrogen electrode (RHE). The main product ratio of CO/HCOO- which intrinsically correlates to the surface SnOx/Sn ratio variation varies with the applied potential. Beyond CO and HCOO- products formed via the two-electron transfer pathway, hydrocarbons and oxygenates are produced. The formation of hydrocarbon (CH4) versus oxygenate (C2H5OH) depends on the choice of electrolyte (KOH vs. KHCO3), both of which can reach a maximal faradaic efficiency of 10%. The distinctive grain boundary and exposed corner/step sites in the interconnected SnO2 nanoparticles contribute to the high FE of CO2 reduction and unique selectivity.

AB - Well crystallized and interconnected SnO2 nanoparticles (<5 nm) were synthesized via oxidation of exfoliated SnS2 sheets. The SnO2 nanoparticles exhibit a high total faradaic efficiency (FE) of 97% towards electrochemical reduction of CO2 at -0.95 V vs. the reversible hydrogen electrode (RHE). The main product ratio of CO/HCOO- which intrinsically correlates to the surface SnOx/Sn ratio variation varies with the applied potential. Beyond CO and HCOO- products formed via the two-electron transfer pathway, hydrocarbons and oxygenates are produced. The formation of hydrocarbon (CH4) versus oxygenate (C2H5OH) depends on the choice of electrolyte (KOH vs. KHCO3), both of which can reach a maximal faradaic efficiency of 10%. The distinctive grain boundary and exposed corner/step sites in the interconnected SnO2 nanoparticles contribute to the high FE of CO2 reduction and unique selectivity.

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