Tuning Gold Nanoparticles with Chelating Ligands for Highly Efficient Electrocatalytic CO2 Reduction

Zhi Cao; Samson B Zacate; Xiaodong Sun; Jinjia Liu; Elizabeth M Hale; William P Carson; Sam B Tyndall; Jun Xu; Xingwu Liu; Xingchen Liu; Chang Song; Jheng-Hua Luo; Mu-Jeng Cheng; Xiaodong Wen; Wei Liu

doi:10.1002/anie.201805696

Tuning Gold Nanoparticles with Chelating Ligands for Highly Efficient Electrocatalytic CO₂ Reduction

Angew Chem Int Ed Engl. 2018 Sep 24;57(39):12675-12679. doi: 10.1002/anie.201805696. Epub 2018 Aug 28.

Authors

Zhi Cao^{1

2

3}, Samson B Zacate⁴, Xiaodong Sun^{1

2}, Jinjia Liu^{1

2}, Elizabeth M Hale⁴, William P Carson⁴, Sam B Tyndall⁴, Jun Xu³, Xingwu Liu^{1

2}, Xingchen Liu^{1

2}, Chang Song^{1

2}, Jheng-Hua Luo⁵, Mu-Jeng Cheng⁵, Xiaodong Wen^{1

2}, Wei Liu⁴

Affiliations

¹ State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan, Shanxi, 030001, P.R.China.
² National Energy Center for Coal to Liquids, Synfuels China Technology Co., Ltd, Beijing, 101400, P.R.China.
³ Department of Chemistry, University of California, Berkeley, Berkeley, CA, 94720, USA.
⁴ Department of Chemistry and Biochemistry, Miami University, Oxford, OH, 45056, USA.
⁵ Department of Chemistry, National Cheng Kung University, Tainan, 701, Taiwan.

PMID: 30098083
DOI: 10.1002/anie.201805696

Abstract

Capped chelating organic molecules are presented as a design principle for tuning heterogeneous nanoparticles for electrochemical catalysis. Gold nanoparticles (AuNPs) functionalized with a chelating tetradentate porphyrin ligand show a 110-fold enhancement compared to the oleylamine-coated AuNP in current density for electrochemical reduction of CO₂ to CO in water at an overpotential of 340 mV with Faradaic efficiencies (FEs) of 93 %. These catalysts also show excellent stability without deactivation (<5 % productivity loss) within 72 hours of electrolysis. DFT calculation results further confirm the chelation effect in stabilizing molecule/NP interface and tailoring catalytic activity. This general approach is thus anticipated to be complementary to current NP catalyst design approaches.

Keywords: CO2 reduction; chelate effect; electrocatalysis; gold nanoparticles; porphyrins.

Abstract

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