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author:

Zhao, Jiwu (Zhao, Jiwu.) [1] | Jin, Mengtian (Jin, Mengtian.) [2] | Huang, Haowei (Huang, Haowei.) [3] | Guo, Haoquan (Guo, Haoquan.) [4] | Han, Yu (Han, Yu.) [5] | Huang, Liang (Huang, Liang.) [6] | Yuan, You-You (Yuan, You-You.) [7] | Wang, Qingxiao (Wang, Qingxiao.) [8] | Liang, Jie (Liang, Jie.) [9] | Gao, Xinhua (Gao, Xinhua.) [10] | Long, Jinlin (Long, Jinlin.) [11] | Tsubaki, Noritatsu (Tsubaki, Noritatsu.) [12] | Lu, Xu (Lu, Xu.) [13]

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EI

Abstract:

Liquid metals (LMs) exhibit superior conductivity, flexibility, and malleability, empowering their versatility across multiple fields. It was prevalently believed, albeit lacking in-depth mechanistic insights, that these features stem from high atomic degrees of freedom. In this work, we substantiate the intense and random atomic motion in LMs through the interplay of theory and in situ/operando experiments. In particular, we visualize structural oscillations and crystallographic orientation variations in near-melting LMs; the disordered LM atoms are not confined by rigid crystal lattices, in contrast to their solid counterparts. Owing to the high atomic degrees of freedom, LMs possess adaptive surfaces capable of dynamically conforming to adsorbate configurations during electrocatalysis, especially electrochemical CO2 reduction (CO2R) that has been hindered by the hardship of key species adsorption/activation/desorption on solid-state catalysts. We then pressurize the CO2 to further enhance the adaptability of the LM surface in its interactions with adsorbates. As a result, the reactants and key intermediates are greatly enriched on the liquid metal surface, yielding an even higher CO2R reactivity compared to the ambient-pressure scenario and reaffirming the mechanistic insights. © 2025 The Authors. Published by American Chemical Society.

Keyword:

Adsorbates Bioremediation Crystal lattices Crystal orientation Degrees of freedom (mechanics) Electrolytic reduction Photodissociation Reaction intermediates

Community:

  • [ 1 ] [Zhao, Jiwu]CERP, Division of Physical Sciences and Engineering, King Abdullah University of Science and Technology (KAUST), Thuwal; 23955-6900, Saudi Arabia
  • [ 2 ] [Zhao, Jiwu]Key Laboratory of Applied Surface and Colloid Chemistry, Ministry of Education, School of Chemistry and Chemical Engineering, Shaanxi Normal University, Xi’an; 710119, China
  • [ 3 ] [Jin, Mengtian]CERP, Division of Physical Sciences and Engineering, King Abdullah University of Science and Technology (KAUST), Thuwal; 23955-6900, Saudi Arabia
  • [ 4 ] [Huang, Haowei]School of Energy and Environment, Southeast University, Nanjing; 210096, China
  • [ 5 ] [Guo, Haoquan]Department of Applied Chemistry, School of Engineering, University of Toyama, Toyama; 930-8555, Japan
  • [ 6 ] [Han, Yu]Electron Microscopy Center, South China University of Technology, Guangzhou; 510640, China
  • [ 7 ] [Huang, Liang]CERP, Division of Physical Sciences and Engineering, King Abdullah University of Science and Technology (KAUST), Thuwal; 23955-6900, Saudi Arabia
  • [ 8 ] [Yuan, You-You]Imaging and Characterization Core Lab, King Abdullah University of Science and Technology (KAUST), Thuwal; 23955-6900, Saudi Arabia
  • [ 9 ] [Wang, Qingxiao]Imaging and Characterization Core Lab, King Abdullah University of Science and Technology (KAUST), Thuwal; 23955-6900, Saudi Arabia
  • [ 10 ] [Liang, Jie]State Key Laboratory of High-Efficiency Utilization of Coal and Green Chemical Engineering, College of Chemistry & Chemical Engineering, Ningxia University, Yinchuan; 750021, China
  • [ 11 ] [Gao, Xinhua]State Key Laboratory of High-Efficiency Utilization of Coal and Green Chemical Engineering, College of Chemistry & Chemical Engineering, Ningxia University, Yinchuan; 750021, China
  • [ 12 ] [Long, Jinlin]State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou; 350116, China
  • [ 13 ] [Tsubaki, Noritatsu]Department of Applied Chemistry, School of Engineering, University of Toyama, Toyama; 930-8555, Japan
  • [ 14 ] [Lu, Xu]CERP, Division of Physical Sciences and Engineering, King Abdullah University of Science and Technology (KAUST), Thuwal; 23955-6900, Saudi Arabia

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Source :

ACS Catalysis

Year: 2025

Issue: 4

Volume: 15

Page: 3505-3514

1 1 . 7 0 0

JCR@2023

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ESI Highly Cited Papers on the List: 0 Unfold All

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Chinese Cited Count:

30 Days PV: 2

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