Theory-Guided Design of Unconventional Phase Metal Heteronanostructures for Higher-Rate Stable Li-CO2 and Li-Air Batteries

Jingwen Zhou; Zhihang Xu; Kai Cui; Jian-An Yin; Hsiao-Chien Chen; Yunhao Wang; Fu Liu; Tianshuai Wang; Fengkun Hao; Yuecheng Xiong; Cheng Wang; Yangbo Ma; Pengyi Lu; Jinwen Yin; Liang Guo; Xiang Meng; Chenliang Ye; Hao Ming Chen; Ye Zhu; Jian Lu; Zhanxi Fan

doi:10.1002/anie.202416947

Theory-Guided Design of Unconventional Phase Metal Heteronanostructures for Higher-Rate Stable Li-CO₂ and Li-Air Batteries

Jingwen Zhou (Co-first Author)
, Zhihang Xu (Co-first Author)
, Kai Cui (Co-first Author)
, Jian-An Yin (Co-first Author)
, Hsiao-Chien Chen^*
, Yunhao Wang
, Fu Liu
, Tianshuai Wang^*
, Fengkun Hao
, Yuecheng Xiong
, Cheng Wang
, Yangbo Ma
, Pengyi Lu
, Jinwen Yin
, Liang Guo
, Xiang Meng
, Chenliang Ye
, Hao Ming Chen
, Ye Zhu^*
, Jian Lu^*

Zhanxi Fan^*

^*Corresponding author for this work

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

33 Citations (Scopus)

Abstract

Lithium-carbon dioxide (Li-CO₂) and Li-air batteries hold great potential in achieving carbon neutral given their ultrahigh theoretical energy density and eco-friendly features. However, these Li-gas batteries still suffer from low discharging-charging rate and poor cycling life due to sluggish decomposition kinetics of discharge products especially Li₂CO₃. Here we report the theory-guided design and preparation of unconventional phase metal heteronanostructures as cathode catalysts for high-performance Li-CO₂/air batteries. The assembled Li-CO₂ cells with unconventional phase 4H/face-centered cubic (fcc) ruthenium-nickel heteronanostructures deliver a narrow discharge-charge gap of 0.65 V, excellent rate capability and long-term cycling stability over 200 cycles at 250 mA g⁻¹. The constructed Li-air batteries can steadily run for above 150 cycles in ambient air. Electrochemical mechanism studies reveal that 4H/fcc Ru−Ni with high-electroactivity facets can boost redox reaction kinetics and tune discharge reactions towards Li₂C₂O₄ path, alleviating electrolyte/catalyst failures induced by the aggressive singlet oxygen from solo decomposition of Li₂CO₃. © 2024 Wiley-VCH GmbH.

Original language	English
Article number	e202416947
Journal	Angewandte Chemie - International Edition
Volume	64
Issue number	5
Online published	29 Sept 2024
DOIs	https://doi.org/10.1002/anie.202416947
Publication status	Published - 27 Jan 2025

Funding

The authors acknowledge the financial supports by grants (Project No. 22175148 and 52102320) from National Natural Science Foundation of China, grants (Project No. 21309322 and 15307522) from Research Grants Council of Hong Kong, grant (Project No. JCYJ20220530140815035) from Shenzhen Science and Technology Program, ITC via Hong Kong Branch of National Precious Metals Material Engineering Research Center (NPMM), and grants (Project No. 9610480, 9610663, 7020103, 7006007 and 9680301) from City University of Hong Kong. The TEM facility is funded by the Research Grants Council of Hong Kong (Project No. C5029-18E). The Simulation studies are supported by the Fundamental Research Funds for the Central Universities (No. D5000220443), the Natural Science Foundation of Chongqing (No. CSTB2023NSCQ-MSX0538), Natural Science Basic Research Program of Shaanxi (Program No. 2024JC-YBQN-0073) and Young Talent Fund of Association for Science and Technology in Shaanxi, China.

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

SDG 7 Affordable and Clean Energy

Research Keywords

Electrocatalysis
Electrochemical mechanism
Li-CO2 battery
Metal heteronanostructures
Unconventional phase

RGC Funding Information

RGC-funded

Access Output

10.1002/anie.202416947

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Cite this

Zhou, J., Xu, Z., Cui, K., Yin, J.-A., Chen, H.-C., Wang, Y., Liu, F., Wang, T., Hao, F., Xiong, Y., Wang, C., Ma, Y., Lu, P., Yin, J., Guo, L., Meng, X., Ye, C., Ming Chen, H., Zhu, Y., ... Fan, Z. (2025). Theory-Guided Design of Unconventional Phase Metal Heteronanostructures for Higher-Rate Stable Li-CO₂ and Li-Air Batteries. Angewandte Chemie - International Edition, 64(5), Article e202416947. https://doi.org/10.1002/anie.202416947

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title = "Theory-Guided Design of Unconventional Phase Metal Heteronanostructures for Higher-Rate Stable Li-CO2 and Li-Air Batteries",

abstract = "Lithium-carbon dioxide (Li-CO2) and Li-air batteries hold great potential in achieving carbon neutral given their ultrahigh theoretical energy density and eco-friendly features. However, these Li-gas batteries still suffer from low discharging-charging rate and poor cycling life due to sluggish decomposition kinetics of discharge products especially Li2CO3. Here we report the theory-guided design and preparation of unconventional phase metal heteronanostructures as cathode catalysts for high-performance Li-CO2/air batteries. The assembled Li-CO2 cells with unconventional phase 4H/face-centered cubic (fcc) ruthenium-nickel heteronanostructures deliver a narrow discharge-charge gap of 0.65 V, excellent rate capability and long-term cycling stability over 200 cycles at 250 mA g−1. The constructed Li-air batteries can steadily run for above 150 cycles in ambient air. Electrochemical mechanism studies reveal that 4H/fcc Ru−Ni with high-electroactivity facets can boost redox reaction kinetics and tune discharge reactions towards Li2C2O4 path, alleviating electrolyte/catalyst failures induced by the aggressive singlet oxygen from solo decomposition of Li2CO3. {\textcopyright} 2024 Wiley-VCH GmbH.",

keywords = "Electrocatalysis, Electrochemical mechanism, Li-CO2 battery, Metal heteronanostructures, Unconventional phase",

author = "Jingwen Zhou and Zhihang Xu and Kai Cui and Jian-An Yin and Hsiao-Chien Chen and Yunhao Wang and Fu Liu and Tianshuai Wang and Fengkun Hao and Yuecheng Xiong and Cheng Wang and Yangbo Ma and Pengyi Lu and Jinwen Yin and Liang Guo and Xiang Meng and Chenliang Ye and \{Ming Chen\}, Hao and Ye Zhu and Jian Lu and Zhanxi Fan",

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doi = "10.1002/anie.202416947",

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Zhou, J, Xu, Z, Cui, K, Yin, J-A, Chen, H-C, Wang, Y , Liu, F, Wang, T, Hao, F , Xiong, Y, Wang, C, Ma, Y , Lu, P , Yin, J , Guo, L , Meng, X, Ye, C, Ming Chen, H, Zhu, Y, Lu, J & Fan, Z 2025, 'Theory-Guided Design of Unconventional Phase Metal Heteronanostructures for Higher-Rate Stable Li-CO₂ and Li-Air Batteries', Angewandte Chemie - International Edition, vol. 64, no. 5, e202416947. https://doi.org/10.1002/anie.202416947

Theory-Guided Design of Unconventional Phase Metal Heteronanostructures for Higher-Rate Stable Li-CO₂ and Li-Air Batteries. / Zhou, Jingwen (Co-first Author); Xu, Zhihang (Co-first Author); Cui, Kai (Co-first Author) et al.
In: Angewandte Chemie - International Edition, Vol. 64, No. 5, e202416947, 27.01.2025.

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

TY - JOUR

T1 - Theory-Guided Design of Unconventional Phase Metal Heteronanostructures for Higher-Rate Stable Li-CO2 and Li-Air Batteries

AU - Zhou, Jingwen

AU - Xu, Zhihang

AU - Cui, Kai

AU - Yin, Jian-An

AU - Chen, Hsiao-Chien

AU - Wang, Yunhao

AU - Liu, Fu

AU - Wang, Tianshuai

AU - Hao, Fengkun

AU - Xiong, Yuecheng

AU - Wang, Cheng

AU - Ma, Yangbo

AU - Lu, Pengyi

AU - Yin, Jinwen

AU - Guo, Liang

AU - Meng, Xiang

AU - Ye, Chenliang

AU - Ming Chen, Hao

AU - Zhu, Ye

AU - Lu, Jian

AU - Fan, Zhanxi

PY - 2025/1/27

Y1 - 2025/1/27

N2 - Lithium-carbon dioxide (Li-CO2) and Li-air batteries hold great potential in achieving carbon neutral given their ultrahigh theoretical energy density and eco-friendly features. However, these Li-gas batteries still suffer from low discharging-charging rate and poor cycling life due to sluggish decomposition kinetics of discharge products especially Li2CO3. Here we report the theory-guided design and preparation of unconventional phase metal heteronanostructures as cathode catalysts for high-performance Li-CO2/air batteries. The assembled Li-CO2 cells with unconventional phase 4H/face-centered cubic (fcc) ruthenium-nickel heteronanostructures deliver a narrow discharge-charge gap of 0.65 V, excellent rate capability and long-term cycling stability over 200 cycles at 250 mA g−1. The constructed Li-air batteries can steadily run for above 150 cycles in ambient air. Electrochemical mechanism studies reveal that 4H/fcc Ru−Ni with high-electroactivity facets can boost redox reaction kinetics and tune discharge reactions towards Li2C2O4 path, alleviating electrolyte/catalyst failures induced by the aggressive singlet oxygen from solo decomposition of Li2CO3. © 2024 Wiley-VCH GmbH.

AB - Lithium-carbon dioxide (Li-CO2) and Li-air batteries hold great potential in achieving carbon neutral given their ultrahigh theoretical energy density and eco-friendly features. However, these Li-gas batteries still suffer from low discharging-charging rate and poor cycling life due to sluggish decomposition kinetics of discharge products especially Li2CO3. Here we report the theory-guided design and preparation of unconventional phase metal heteronanostructures as cathode catalysts for high-performance Li-CO2/air batteries. The assembled Li-CO2 cells with unconventional phase 4H/face-centered cubic (fcc) ruthenium-nickel heteronanostructures deliver a narrow discharge-charge gap of 0.65 V, excellent rate capability and long-term cycling stability over 200 cycles at 250 mA g−1. The constructed Li-air batteries can steadily run for above 150 cycles in ambient air. Electrochemical mechanism studies reveal that 4H/fcc Ru−Ni with high-electroactivity facets can boost redox reaction kinetics and tune discharge reactions towards Li2C2O4 path, alleviating electrolyte/catalyst failures induced by the aggressive singlet oxygen from solo decomposition of Li2CO3. © 2024 Wiley-VCH GmbH.

KW - Electrocatalysis

KW - Electrochemical mechanism

KW - Li-CO2 battery

KW - Metal heteronanostructures

KW - Unconventional phase

UR - https://www.scopus.com/pages/publications/85208198712

UR - https://www.scopus.com/record/pubmetrics.uri?eid=2-s2.0-85208198712&origin=recordpage

U2 - 10.1002/anie.202416947

DO - 10.1002/anie.202416947

M3 - RGC 21 - Publication in refereed journal

SN - 1433-7851

VL - 64

JO - Angewandte Chemie - International Edition

JF - Angewandte Chemie - International Edition

IS - 5

M1 - e202416947

ER -

Theory-Guided Design of Unconventional Phase Metal Heteronanostructures for Higher-Rate Stable Li-CO₂ and Li-Air Batteries

Abstract

Funding

UN SDGs

Research Keywords

RGC Funding Information

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ECS: Controlled Synthesis of Unconventional Phase Copper-based Janus Nanostructures for Tandem Electrocatalytic Carbon Dioxide Reduction

Cite this

Theory-Guided Design of Unconventional Phase Metal Heteronanostructures for Higher-Rate Stable Li-CO2 and Li-Air Batteries

Abstract

Funding

UN SDGs

Research Keywords

RGC Funding Information

Access Output

Other Access Options

Permanent Link

Other Files and Links

Fingerprint

Projects

ECS: Controlled Synthesis of Unconventional Phase Copper-based Janus Nanostructures for Tandem Electrocatalytic Carbon Dioxide Reduction

Cite this

Theory-Guided Design of Unconventional Phase Metal Heteronanostructures for Higher-Rate Stable Li-CO₂ and Li-Air Batteries