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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] (Scholars:龙金林) | Tsubaki, Noritatsu (Tsubaki, Noritatsu.) [12] | Lu, Xu (Lu, Xu.) [13]

Indexed by:

EI Scopus SCIE

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.

Keyword:

CO2 reduction High degree of freedom High-pressureelectrocatalysis Liquid metals Structural oscillation Surface adaptability

Community:

  • [ 1 ] [Zhao, Jiwu]King Abdullah Univ Sci & Technol KAUST, CERP, Div Phys Sci & Engn, Thuwal 239556900, Saudi Arabia
  • [ 2 ] [Jin, Mengtian]King Abdullah Univ Sci & Technol KAUST, CERP, Div Phys Sci & Engn, Thuwal 239556900, Saudi Arabia
  • [ 3 ] [Huang, Liang]King Abdullah Univ Sci & Technol KAUST, CERP, Div Phys Sci & Engn, Thuwal 239556900, Saudi Arabia
  • [ 4 ] [Lu, Xu]King Abdullah Univ Sci & Technol KAUST, CERP, Div Phys Sci & Engn, Thuwal 239556900, Saudi Arabia
  • [ 5 ] [Zhao, Jiwu]Shaanxi Normal Univ, Sch Chem & Chem Engn, Key Lab Appl Surface & Colloid Chem, Minist Educ, Xian 710119, Peoples R China
  • [ 6 ] [Huang, Haowei]Southeast Univ, Sch Energy & Environm, Nanjing 210096, Peoples R China
  • [ 7 ] [Guo, Haoquan]Univ Toyama, Sch Engn, Dept Appl Chem, Toyama 9308555, Japan
  • [ 8 ] [Tsubaki, Noritatsu]Univ Toyama, Sch Engn, Dept Appl Chem, Toyama 9308555, Japan
  • [ 9 ] [Han, Yu]South China Univ Technol, Electron Microscopy Ctr, Guangzhou 510640, Peoples R China
  • [ 10 ] [Yuan, You-You]King Abdullah Univ Sci & Technol KAUST, Imaging & Characterizat Core Lab, Thuwal 239556900, Saudi Arabia
  • [ 11 ] [Wang, Qingxiao]King Abdullah Univ Sci & Technol KAUST, Imaging & Characterizat Core Lab, Thuwal 239556900, Saudi Arabia
  • [ 12 ] [Liang, Jie]Ningxia Univ, Coll Chem & Chem Engn, State Key Lab High Efficiency Utilizat Coal & Gree, Yinchuan 750021, Peoples R China
  • [ 13 ] [Gao, Xinhua]Ningxia Univ, Coll Chem & Chem Engn, State Key Lab High Efficiency Utilizat Coal & Gree, Yinchuan 750021, Peoples R China
  • [ 14 ] [Long, Jinlin]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350116, Peoples R China

Reprint 's Address:

  • [Lu, Xu]King Abdullah Univ Sci & Technol KAUST, CERP, Div Phys Sci & Engn, Thuwal 239556900, Saudi Arabia

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Source :

ACS CATALYSIS

ISSN: 2155-5435

Year: 2025

Issue: 4

Volume: 15

Page: 3505-3514

1 1 . 7 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: 1

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