Composition-dependent CO2 electrochemical reduction activity and selectivity on Au-Pd core-shell nanoparticles

Zhu, Shangqian1; Qin, Xueping1; Wang, Qi2; Li, Tiehuai1; Tao, Ran1; Gu, Meng2; Shao, Minhua1,3

2019-07-28

10.1039/c9ta05325e

Journal of Materials Chemistry A   影响因子和分区

2050-7488

2050-7496

Achieving a high faradaic efficiency and mass activity simultaneously on catalysts is critical in accelerating the practical application of CO2 electrochemical reduction. In this study, Au-Pd core-shell nanoparticles consisting of an ultrathin Pd-rich shell and an Au-Pd alloy core are developed by a simple one-pot synthesis method and evaluated for CO2-to-CO conversion. By adjusting the Au : Pd feeding ratio, the shell thickness and composition in the nanoparticle can be tuned. Significantly improved CO selectivity as compared to pure Au and Pd counterparts can be obtained on all the synthesized Au-Pd core-shell nanoparticles with a maximum faradaic efficiency of 96.7% at -0.6 V. The Au94Pd6 catalyst shows an ultrahigh mass activity of 99.8 A g(Pd+Au)(-1) for CO production at an overpotential of merely 390 mV. Combined in situ infrared absorption spectroscopy and density functional theory studies reveal that the easier desorption of *CO due to the more balanced *COOH/*CO adsorption energies on Au-Pd core-shell surfaces is responsible for the improved catalytic performance.

SCI ; EI

英语

通讯

Development and Reform Commission of Shenzhen Municipality 2017[1106] ; Development and Reform Commission of Shenzhen Municipality 2017[1181]

Chemistry ; Energy & Fuels ; Materials Science

Chemistry, Physical ; Energy & Fuels ; Materials Science, Multidisciplinary

WOS:000476599900034

ROYAL SOC CHEMISTRY

20192907210370

Absorption spectroscopy ; Binary alloys ; Carbon dioxide ; Catalyst activity ; Catalyst selectivity ; Density functional theory ; Efficiency ; Electrolytic reduction ; Gold alloys ; Light absorption ; Nanoparticles ; Palladium alloys ; Shells (structures) ; Synthesis (chemical)

Structural Members and Shapes:408.2 ; Precious Metals:547.1 ; Light/Optics:741.1 ; Nanotechnology:761 ; Chemical Reactions:802.2 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Inorganic Compounds:804.2 ; Production Engineering:913.1 ; Probability Theory:922.1 ; Solid State Physics:933

Web of Science

1.Hong Kong Univ Sci & Technol, Dept Chem & Biol Engn, Kowloon, Clear Water Bay, Hong Kong, Peoples R China
2.Southern Univ Sci & Technol, Dept Mat Sci & Engn, Shenzhen 518055, Peoples R China
3.Hong Kong Univ Sci & Technol, Energy Inst, Kowloon, Clear Water Bay, Hong Kong, Peoples R China

Zhu, Shangqian,Qin, Xueping,Wang, Qi,et al. Composition-dependent CO2 electrochemical reduction activity and selectivity on Au-Pd core-shell nanoparticles[J]. Journal of Materials Chemistry A,2019,7(28):16954-16961.

Zhu, Shangqian.,Qin, Xueping.,Wang, Qi.,Li, Tiehuai.,Tao, Ran.,...&Shao, Minhua.(2019).Composition-dependent CO2 electrochemical reduction activity and selectivity on Au-Pd core-shell nanoparticles.Journal of Materials Chemistry A,7(28),16954-16961.

Zhu, Shangqian,et al."Composition-dependent CO2 electrochemical reduction activity and selectivity on Au-Pd core-shell nanoparticles".Journal of Materials Chemistry A 7.28(2019):16954-16961.