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; 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,

‡^ab Byoungsu Kim,

‡^cd Shize Yang,

‡^e Yang Liu,

^ab Cristiano Francisco Woellner,

^b Zhengyuan Li,

^b Robert Vajtai,^b Wei Yang,

*^a Jingjie Wu,

*^f Paul J. A. Kenis*^cd and Pulickel M. Ajayan*^b

Author affiliations

* Corresponding authors

^a College of Polymer Science and Engineering, Sichuan University, State Key Laboratory of Polymer Materials Engineering, Chengdu 610065, Sichuan, China

^b Department of Materials Science and Nano Engineering, Rice University, 6100 Main Street, Houston, Texas 77005, USA

^c Department of Chemical & Biomolecular Engineering, University of Illinois at Urbana-Champaign, 600 South Mathews Avenue, Urbana, IL 61801, USA

^d International Institute for Carbon Neutral Energy Research (WPI-I2CNER), Kyushu University, 744 Moto-oka, Nishi-ku, Fukuoka, Japan

^e Materials Science and Technology Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, USA

^f Department of Chemical and Environmental Engineering, University of Cincinnati, Cincinnati, OH 45221, USA
E-mail: jingjie.wu@uc.edu

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.

Journal of Materials Chemistry A

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

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

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Journal of Materials Chemistry A