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

Shangqian Zhu; Xueping Qin; Qi Wang; Tiehuai Li; Ran Tao; Meng Gu; Minhua Shao

doi:10.1039/c9ta05325e

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

Shangqian Zhu
, Xueping Qin
, Qi Wang
, Tiehuai Li
, Ran Tao
, Meng Gu
, Minhua Shao

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

76 Citations (Scopus)

Abstract

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. © 2019 The Royal Society of Chemistry.

Original language	English
Pages (from-to)	16954-16961
Journal	Journal of Materials Chemistry A
Volume	7
Issue number	28
DOIs	https://doi.org/10.1039/c9ta05325e
Publication status	Published - Jun 2019
Externally published	Yes

Bibliographical note

Publication details (e.g. title, author(s), publication statuses and dates) are captured on an “AS IS” and “AS AVAILABLE” basis at the time of record harvesting from the data source. Suggestions for further amendments or supplementary information can be sent to [email protected].

Funding

This work was supported by the Research Grant Council of the Hong Kong Special Administrative Region (26206115 and 16309418), the computational resources from Tianhe-2 Supercomputer Center in Guangzhou, and Development and Reform Commission of Shenzhen Municipality 2017 (no. 1106) and 2017 (no. 1181). The STEM work was performed at the SUSTech Pico center that receives funding from the Shenzhen government. S. Zhu thanks HKJEBN Group for providing the PhD scholarship.

RGC Funding Information

RGC-funded

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Cite this

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abstract = "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 gPd+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. {\textcopyright} 2019 The Royal Society of Chemistry.",

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T1 - Composition-dependent CO2 electrochemical reduction activity and selectivity on Au-Pd core-shell nanoparticles

AU - Zhu, Shangqian

AU - Qin, Xueping

AU - Wang, Qi

AU - Li, Tiehuai

AU - Tao, Ran

AU - Gu, Meng

AU - Shao, Minhua

N1 - Publication details (e.g. title, author(s), publication statuses and dates) are captured on an “AS IS” and “AS AVAILABLE” basis at the time of record harvesting from the data source. Suggestions for further amendments or supplementary information can be sent to [email protected].

PY - 2019/6

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N2 - 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 gPd+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. © 2019 The Royal Society of Chemistry.

AB - 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 gPd+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. © 2019 The Royal Society of Chemistry.

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DO - 10.1039/c9ta05325e

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