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

Library availability

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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 = "This research is nancially supported by SABIC. Chenglu Liang also would like to thank the nancial support from the China Scholarship Council during her study in Rice University. The electron microscopy (S. Z. Y.) was supported in part by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Science and Engineering Division and through a user proposal supported by ORNL's Center for Nanophase Materials Sciences, which is sponsored by the Scientic User Facilities Division of the U.S. Department of Energy.",

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AU - Liang, Chenglu

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AU - Francisco Woellner, Cristiano

AU - Li, Zhengyuan

AU - Vajtai, Robert

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AU - Wu, Jingjie

AU - Kenis, Paul J.A.

AU - Ajayan, Pulickel M.

N1 - This research is nancially supported by SABIC. Chenglu Liang also would like to thank the nancial support from the China Scholarship Council during her study in Rice University. The electron microscopy (S. Z. Y.) was supported in part by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Science and Engineering Division and through a user proposal supported by ORNL's Center for Nanophase Materials Sciences, which is sponsored by the Scientic User Facilities Division of the U.S. Department of Energy.

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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