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Tuning Structural and Compositional Effects in Pd–Au Nanowires for Highly Selective and Active CO2 Electrochemical Reduction Reaction

CO2 electrochemical reduction is a promising technology to control the concentration of atmospheric CO2 and store renewable energy. However, it is extremely challenging to selectively produce important chemicals such as CO with reasonable low overpotentials and high reaction rates. In this study, tw... Full description

Journal Title: Advanced Energy Materials Nov 2018, Vol.8(32)
Main Author: Zhu, Shangqian
Other Authors: Wang, Qi , Qin, Xueping , Gu, Meng , Tao, Ran , Brennan, Peter , Zhang, Lulu , Yao, Yuze , Li, Tiehuai , Shao, Minhua
Format: Electronic Article Electronic Article
Language: English
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ID: ISSN: 16146832 ; E-ISSN: 16146840 ; DOI: 10.1002/aenm.201802238
Link: http://search.proquest.com/docview/2133302875/?pq-origsite=primo
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title: Tuning Structural and Compositional Effects in Pd–Au Nanowires for Highly Selective and Active CO2 Electrochemical Reduction Reaction
format: Article
creator:
  • Zhu, Shangqian
  • Wang, Qi
  • Qin, Xueping
  • Gu, Meng
  • Tao, Ran
  • Brennan, Peter
  • Zhang, Lulu
  • Yao, Yuze
  • Li, Tiehuai
  • Shao, Minhua
subjects:
  • Gold
  • Palladium
  • Grain Boundaries
  • Organic Chemistry
  • Nanowires
  • Carbon Dioxide
  • Nanoparticles
  • Density Functional Theory
  • Chemical Reduction
  • Nanowires
  • Selectivity
  • Adsorption Energies
  • CO 2 Reduction
  • Electrocatalysis
  • IR Spectroscopy
  • Palladium
ispartof: Advanced Energy Materials, Nov 2018, Vol.8(32)
description: CO2 electrochemical reduction is a promising technology to control the concentration of atmospheric CO2 and store renewable energy. However, it is extremely challenging to selectively produce important chemicals such as CO with reasonable low overpotentials and high reaction rates. In this study, twisted Pd–Au nanowires with a unique core–shell and grain boundary‐rich structure are developed. Compared with Pd nanoparticles, the synthesized nanowires have a significantly improved CO selectivity. A maximum CO faradaic efficiency (FE) of 94.3% (at −0.6 V), and an extremely low overpotential of 90 mV for CO formation with an FE of 8.5% can be achieved on Pd0.8Au nanowires. The Pd0.8Au nanowires also show superior specific and mass activities especially at low overpotentials. The low overpotential and high selectivity for CO2‐to‐CO electrocatalytic conversion are achieved simultaneously for the first time on Pd‐based nanocatalysts. Combined in situ infrared spectroscopic studies with an attenuated total reflection configuration and density function theory calculations reveal that surface CO could be more facilely generated at much lower overpotentials on nanowires as compared with that on particles. Additionally, the Au atoms in Pd–Au nanowires promote the formation of linearly bonded CO, which is easier to desorb, resulting in a fast reaction rate.
language: eng
source:
identifier: ISSN: 16146832 ; E-ISSN: 16146840 ; DOI: 10.1002/aenm.201802238
fulltext: fulltext
issn:
  • 16146832
  • 1614-6832
  • 16146840
  • 1614-6840
url: Link


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titleTuning Structural and Compositional Effects in Pd–Au Nanowires for Highly Selective and Active CO2 Electrochemical Reduction Reaction
creatorZhu, Shangqian ; Wang, Qi ; Qin, Xueping ; Gu, Meng ; Tao, Ran ; Brennan, Peter ; Zhang, Lulu ; Yao, Yuze ; Li, Tiehuai ; Shao, Minhua
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subjectGold ; Palladium ; Grain Boundaries ; Organic Chemistry ; Nanowires ; Carbon Dioxide ; Nanoparticles ; Density Functional Theory ; Chemical Reduction ; Nanowires ; Selectivity ; Adsorption Energies ; CO 2 Reduction ; Electrocatalysis ; IR Spectroscopy ; Palladium
descriptionCO2 electrochemical reduction is a promising technology to control the concentration of atmospheric CO2 and store renewable energy. However, it is extremely challenging to selectively produce important chemicals such as CO with reasonable low overpotentials and high reaction rates. In this study, twisted Pd–Au nanowires with a unique core–shell and grain boundary‐rich structure are developed. Compared with Pd nanoparticles, the synthesized nanowires have a significantly improved CO selectivity. A maximum CO faradaic efficiency (FE) of 94.3% (at −0.6 V), and an extremely low overpotential of 90 mV for CO formation with an FE of 8.5% can be achieved on Pd0.8Au nanowires. The Pd0.8Au nanowires also show superior specific and mass activities especially at low overpotentials. The low overpotential and high selectivity for CO2‐to‐CO electrocatalytic conversion are achieved simultaneously for the first time on Pd‐based nanocatalysts. Combined in situ infrared spectroscopic studies with an attenuated total reflection configuration and density function theory calculations reveal that surface CO could be more facilely generated at much lower overpotentials on nanowires as compared with that on particles. Additionally, the Au atoms in Pd–Au nanowires promote the formation of linearly bonded CO, which is easier to desorb, resulting in a fast reaction rate.
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titleTuning Structural and Compositional Effects in Pd–Au Nanowires for Highly Selective and Active CO2 Electrochemical Reduction Reaction
descriptionCO2 electrochemical reduction is a promising technology to control the concentration of atmospheric CO2 and store renewable energy. However, it is extremely challenging to selectively produce important chemicals such as CO with reasonable low overpotentials and high reaction rates. In this study, twisted Pd–Au nanowires with a unique core–shell and grain boundary‐rich structure are developed. Compared with Pd nanoparticles, the synthesized nanowires have a significantly improved CO selectivity. A maximum CO faradaic efficiency (FE) of 94.3% (at −0.6 V), and an extremely low overpotential of 90 mV for CO formation with an FE of 8.5% can be achieved on Pd0.8Au nanowires. The Pd0.8Au nanowires also show superior specific and mass activities especially at low overpotentials. The low overpotential and high selectivity for CO2‐to‐CO electrocatalytic conversion are achieved simultaneously for the first time on Pd‐based nanocatalysts. Combined in situ infrared spectroscopic studies with an attenuated total reflection configuration and density function theory calculations reveal that surface CO could be more facilely generated at much lower overpotentials on nanowires as compared with that on particles. Additionally, the Au atoms in Pd–Au nanowires promote the formation of linearly bonded CO, which is easier to desorb, resulting in a fast reaction rate.
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titleTuning Structural and Compositional Effects in Pd–Au Nanowires for Highly Selective and Active CO2 Electrochemical Reduction Reaction
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abstractCO2 electrochemical reduction is a promising technology to control the concentration of atmospheric CO2 and store renewable energy. However, it is extremely challenging to selectively produce important chemicals such as CO with reasonable low overpotentials and high reaction rates. In this study, twisted Pd–Au nanowires with a unique core–shell and grain boundary‐rich structure are developed. Compared with Pd nanoparticles, the synthesized nanowires have a significantly improved CO selectivity. A maximum CO faradaic efficiency (FE) of 94.3% (at −0.6 V), and an extremely low overpotential of 90 mV for CO formation with an FE of 8.5% can be achieved on Pd0.8Au nanowires. The Pd0.8Au nanowires also show superior specific and mass activities especially at low overpotentials. The low overpotential and high selectivity for CO2‐to‐CO electrocatalytic conversion are achieved simultaneously for the first time on Pd‐based nanocatalysts. Combined in situ infrared spectroscopic studies with an attenuated total reflection configuration and density function theory calculations reveal that surface CO could be more facilely generated at much lower overpotentials on nanowires as compared with that on particles. Additionally, the Au atoms in Pd–Au nanowires promote the formation of linearly bonded CO, which is easier to desorb, resulting in a fast reaction rate.
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date2018-11-01