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author:

Chuhao Liu (Chuhao Liu.) [1] | Yifan Bu (Yifan Bu.) [2] | Yifei Xu (Yifei Xu.) [3] | Azhar Mahmood (Azhar Mahmood.) [4] | Jisheng Xie (Jisheng Xie.) [5] | Yifan Fu (Yifan Fu.) [6] | Shiyun Li (Shiyun Li.) [7] | Cheng Peng (Cheng Peng.) [8] | Yue Wu (Yue Wu.) [9] (Scholars:吴悦) | Xiao Liang (Xiao Liang.) [10] | Ruilong Zong (Ruilong Zong.) [11] | Wan-Lu Li (Wan-Lu Li.) [12] | Jihan Zhou (Jihan Zhou.) [13] | Bingjun Xu (Bingjun Xu.) [14] | Li Niu (Li Niu.) [15] | Mufan Li (Mufan Li.) [16]

Abstract:

Unravelling the influence of strain and geometric effects on the electrochemical reduction of carbon dioxide(CO2RR)on Cu-based(or Pd-based)alloys remains challenging due to complex local microenvironment variables.Herein,we employ two PdCu alloys(nanoparticles and nanodendrites)to demonstrate how CO2RR selectivity can shift from CO to HCOO-.Despite sharing consistent phases,exposed crystal facets,and overall oxidative states,these alloys exhibit different local strain profiles due to their distinct geometries.By integrating experimental data,in-situ spectroscopy,and density functional theory calculations,we revealed that CO2 prefers adsorption on tensile-strained areas with carbon-side geometry,following a*COOH-to-CO pathway.Conversely,on some compressive-strained regions induced by the dendrite-like morphology,CO2 adopts an oxygen-side geometry,favoring an *OCHO-to-HCOO pathway due to the downshift of the d-band center.Notably,our findings elucidate a dominant *OCHO-to-HCOO-pathway in catalysts when featuring both adsorption geometries.This research provides a comprehensive model for local environment of bimetallic alloys,and establishes a clear relationship between the CO2RR pathway shift and variation in local strain environments of PdCu alloys.

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Community:

  • [ 1 ] [Yue Wu]福州大学
  • [ 2 ] [Jihan Zhou]北京大学
  • [ 3 ] [Cheng Peng]北京大学
  • [ 4 ] [Li Niu]广州大学
  • [ 5 ] [Bingjun Xu]北京大学
  • [ 6 ] [Yifei Xu]北京大学
  • [ 7 ] [Yifan Fu]北京大学
  • [ 8 ] [Xiao Liang]清华大学
  • [ 9 ] [Shiyun Li]北京大学
  • [ 10 ] [Mufan Li]北京大学
  • [ 11 ] [Azhar Mahmood]广州大学
  • [ 12 ] [Yifan Bu]北京大学
  • [ 13 ] [Jisheng Xie]北京大学
  • [ 14 ] [Ruilong Zong]清华大学
  • [ 15 ] [Chuhao Liu]北京大学
  • [ 16 ] [Wan-Lu Li]Department of NanoEngineering,University of California,San Diego,La Jolla 92093,USA

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国家科学评论(英文版)

ISSN: 2095-5138

Year: 2024

Issue: 12

Volume: 11

Page: 14-21

1 6 . 3 0 0

JCR@2023

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ESI Highly Cited Papers on the List: 0 Unfold All

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30 Days PV: 0

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