Boosting the reaction kinetics in aprotic lithium-carbon dioxide batteries with unconventional phase metal nanomaterials

Jingwen Zhou; Tianshuai Wang; Lin Chen; Lingwen Liao; Yunhao Wang; Shibo Xi; Bo Chen; Ting Lin; Qinghua Zhang; Chenliang Ye; Xichen Zhou; Zhiqiang Guan; Li Zhai; Zhen He; Gang Wang; Juan Wang; Jinli Yu; Yangbo Ma; Pengyi Lu; Yuecheng Xiong; Shiyao Lu; Ye Chen; Bin Wang; Chun-Sing Lee; Jianli Cheng; Lin Gu; Tianshou Zhao; Zhanxi Fan

doi:10.1073/pnas.2204666119

Boosting the reaction kinetics in aprotic lithium-carbon dioxide batteries with unconventional phase metal nanomaterials

Proc Natl Acad Sci U S A. 2022 Oct 4;119(40):e2204666119. doi: 10.1073/pnas.2204666119. Epub 2022 Sep 26.

Authors

Jingwen Zhou^{1

2

3}, Tianshuai Wang⁴, Lin Chen³, Lingwen Liao¹, Yunhao Wang¹, Shibo Xi⁵, Bo Chen¹, Ting Lin^{6

7}, Qinghua Zhang^{6

7}, Chenliang Ye⁸, Xichen Zhou¹, Zhiqiang Guan¹, Li Zhai^{1

2}, Zhen He^{1

2}, Gang Wang⁹, Juan Wang¹, Jinli Yu¹, Yangbo Ma¹, Pengyi Lu^{1

2}, Yuecheng Xiong¹, Shiyao Lu¹, Ye Chen⁹, Bin Wang¹⁰, Chun-Sing Lee^{1

11}, Jianli Cheng³, Lin Gu^{6

7}, Tianshou Zhao⁴, Zhanxi Fan^{1

2

12}

Affiliations

¹ Department of Chemistry, City University of Hong Kong, Kowloon, Hong Kong SAR 999077, China.
² Hong Kong Branch of National Precious Metals Material Engineering Research Center (NPMM), City University of Hong Kong, Kowloon, Hong Kong SAR 999077, China.
³ Institute of Chemical Materials, China Academy of Engineering Physics, Mianyang 621900, Sichuan, China.
⁴ Department of Mechanical and Aerospace Engineering, The Hong Kong University of Science and Technology, Clear Water Bay, Hong Kong SAR 999077, China.
⁵ Institute of Chemical and Engineering Sciences, A*STAR, 1 Pesek Road, Jurong Island, Singapore 627833, Singapore.
⁶ Institute of Physics, Beijing National Laboratory for Condensed Matter Physics, Chinese Academy of Sciences, Beijing 100190, China.
⁷ School of Physical Sciences, University of Chinese Academy of Sciences, Beijing 100049, China.
⁸ Department of Chemistry, Tsinghua University, Beijing 100084, China.
⁹ Department of Chemistry, The Chinese University of Hong Kong, Shatin, Hong Kong SAR 999077, China.
¹⁰ Institute of Fundamental and Frontiers Sciences, University of Electronic Sciences and Technology of China, Chengdu 611731, China.
¹¹ Center of Super-Diamond and Advanced Films (COSDAF), City University of Hong Kong, Kowloon, Hong Kong SAR 999077, China.
¹² City University of Hong Kong Shenzhen Research Institute, Shenzhen 518057, China.

Abstract

Given the high energy density and eco-friendly characteristics, lithium-carbon dioxide (Li-CO₂) batteries have been considered to be a next-generation energy technology to promote carbon neutral and space exploration. However, Li-CO₂ batteries suffer from sluggish reaction kinetics, causing large overpotential and poor energy efficiency. Here, we observe enhanced reaction kinetics in aprotic Li-CO₂ batteries with unconventional phase 4H/face-centered cubic (fcc) iridium (Ir) nanostructures grown on gold template. Significantly, 4H/fcc Ir exhibits superior electrochemical performance over fcc Ir in facilitating the round-trip reaction kinetics of Li⁺-mediated CO₂ reduction and evolution, achieving a low charge plateau below 3.61 V and high energy efficiency of 83.8%. Ex situ/in situ studies and theoretical calculations reveal that the boosted reaction kinetics arises from the highly reversible generation of amorphous/low-crystalline discharge products on 4H/fcc Ir via the Ir-O coupling. The demonstration of flexible Li-CO₂ pouch cells with 4H/fcc Ir suggests the feasibility of using unconventional phase nanomaterials in practical scenarios.

Keywords: Ir nanostructures; Li-CO2 battery; electrochemical mechanism; reaction kinetics; unconventional phase.

Abstract

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