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author:

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

Indexed by:

EI Scopus SCIE

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.

Keyword:

CO2 electroreduction local strain pathway shift PdCu alloys

Community:

  • [ 1 ] [Liu, Chuhao]Peking Univ, Coll Chem & Mol Engn, Beijing 100871, Peoples R China
  • [ 2 ] [Bu, Yifan]Peking Univ, Coll Chem & Mol Engn, Beijing 100871, Peoples R China
  • [ 3 ] [Xu, Yifei]Peking Univ, Coll Chem & Mol Engn, Beijing 100871, Peoples R China
  • [ 4 ] [Xie, Jisheng]Peking Univ, Coll Chem & Mol Engn, Beijing 100871, Peoples R China
  • [ 5 ] [Fu, Yifan]Peking Univ, Coll Chem & Mol Engn, Beijing 100871, Peoples R China
  • [ 6 ] [Li, Shiyun]Peking Univ, Coll Chem & Mol Engn, Beijing 100871, Peoples R China
  • [ 7 ] [Peng, Cheng]Peking Univ, Coll Chem & Mol Engn, Beijing 100871, Peoples R China
  • [ 8 ] [Zhou, Jihan]Peking Univ, Coll Chem & Mol Engn, Beijing 100871, Peoples R China
  • [ 9 ] [Xu, Bingjun]Peking Univ, Coll Chem & Mol Engn, Beijing 100871, Peoples R China
  • [ 10 ] [Li, Mufan]Peking Univ, Coll Chem & Mol Engn, Beijing 100871, Peoples R China
  • [ 11 ] [Mahmood, Azhar]Guangzhou Univ, Sch Chem & Chem Engn, Guangzhou 510006, Peoples R China
  • [ 12 ] [Niu, Li]Guangzhou Univ, Sch Chem & Chem Engn, Guangzhou 510006, Peoples R China
  • [ 13 ] [Wu, Yue]Fuzhou Univ, Coll Mat Sci & Engn, Fuzhou 350108, Peoples R China
  • [ 14 ] [Liang, Xiao]Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China
  • [ 15 ] [Zong, Ruilong]Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China
  • [ 16 ] [Li, Wan-Lu]Univ Calif San Diego, Dept NanoEngn, La Jolla, CA 92093 USA

Reprint 's Address:

  • [Li, Mufan]Peking Univ, Coll Chem & Mol Engn, Beijing 100871, Peoples R China;;[Mahmood, Azhar]Guangzhou Univ, Sch Chem & Chem Engn, Guangzhou 510006, Peoples R China;;[Niu, Li]Guangzhou Univ, Sch Chem & Chem Engn, Guangzhou 510006, Peoples R China;;

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Source :

NATIONAL SCIENCE REVIEW

ISSN: 2095-5138

Year: 2024

Issue: 12

Volume: 11

1 6 . 3 0 0

JCR@2023

Cited Count:

WoS CC Cited Count:

SCOPUS Cited Count:

ESI Highly Cited Papers on the List: 0 Unfold All

WanFang Cited Count:

Chinese Cited Count:

30 Days PV: 0

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