Electrolyte-Impregnated Mesoporous Hollow Microreactor to Supplement an Inner Reaction Pathway for Boosting the Cyclability of Li-CO2 Batteries

Yuqing Bai; Le Wei; Yuebin Lian; Zhihe Wei; Daqi Song; Yanhui Su; Xiong Zhu; Wenxuan Huo; Jian Cheng; Yang Peng; Zhao Deng

doi:10.1021/acsami.3c05778

Electrolyte-Impregnated Mesoporous Hollow Microreactor to Supplement an Inner Reaction Pathway for Boosting the Cyclability of Li-CO₂ Batteries

ACS Appl Mater Interfaces. 2023 Sep 6;15(35):41457-41465. doi: 10.1021/acsami.3c05778. Epub 2023 Aug 24.

Authors

Yuqing Bai^{1

2}, Le Wei³, Yuebin Lian⁴, Zhihe Wei^{1

2}, Daqi Song^{1

2}, Yanhui Su^{1

2}, Xiong Zhu¹, Wenxuan Huo¹, Jian Cheng^{1

2}, Yang Peng^{1

2}, Zhao Deng^{1

2}

Affiliations

¹ Soochow Institute for Energy and Materials Innovations, College of Energy, Soochow University, Suzhou 215006, P. R. China.
² Key Laboratory of Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu Province, Suzhou 215006, P. R. China.
³ Beijing Key Laboratory of Microstructure and Properties of Solids, Faculty of Materials and Manufacturing, Beijing University of Technology, Beijing 100124, China.
⁴ School of Photoelectric Engineering, Changzhou Institute of Technology, Changzhou 213032, China.

PMID: 37615533
DOI: 10.1021/acsami.3c05778

Abstract

Li-CO₂ batteries that integrate energy storage with greenhouse gas fixation have received a great deal of attention in the pursuit of carbon neutrality. However, cyclic accumulation of the insulative and insoluble Li₂CO₃ on the cathode surface severely restrains the battery cyclability, especially under a high depth of discharge/charge. Herein, we design and fabricate a microreactor-type catalyst by embedding Ru nanoparticles into the shells of mesoporous hollow carbon spheres. We show that both the hollow cavity and mesoporous shell are indispensable for concertedly furnishing a high activity to catalyze reversible Li₂CO₃ formation/decomposition. This unique structure ensures that the Ru sites masked by exterior Li₂CO₃ deposits during charging can resume the redox process of discharge by working with the prestored electrolyte to establish an inner reaction path. The thus fabricated Li-CO₂ batteries demonstrate remarkable cyclability of 1085 cycles under 0.5 Ah g^-1 and 326 cycles under 2 Ah g^-1 at 1 A g^-1, outshining most of the literature reports. This study highlights a smart catalyst design to boost the reversibility and cyclability of Li-CO₂ batteries through an "in & out" strategy.

Keywords: Li-CO2 batteries; cyclability; lithium carbonate; microreactor; porous hollow carbon sphere.