Nitrogen-anchored boridene enables Mg-CO2 batteries with high reversibility.

Wang, Yangyang; Sun, Yong; Wu, Fengqi; Zou, Guodong; Gaumet, Jean-Jacques; Li, Jinyu; Fernandez, Carlos; Wang, Yong; Peng, Qiuming

Abstract

Nanoscale defect engineering plays a crucial role in incorporating extraordinary catalytic properties in two-dimensional materials by varying the surface groups or site interactions. Herein, we synthesized high-loaded nitrogen-doped Boridene (N-Boridene (Mo4/3(BnN1-n)2-mTz), N-doped concentration up to 26.78 at %) nanosheets by chemical exfoliation followed by cyanamide intercalation. Three different nitrogen sites are observed in N-Boridene, wherein the site of boron vacancy substitution mainly accounts for its high chemical activity. Attractively, as a cathode for Mg-CO2 batteries, it delivers a long-term lifetime (305 cycles), high-energy efficiency (93.6%), and ultralow overpotential (~0.09 V) at a high current of 200 mA g-1, which overwhelms all Mg-CO2 batteries reported so far. Experimental and computational studies suggest that N-Boridene can remarkably change the adsorption energy of the reaction products and lower the energy barrier of the rate-determining step (*MgCO2 → *MgCO3·xH2O), resulting in the rapid reversible formation/decomposition of new MgCO3·5H2O products. The surging Boridene materials with defects provide substantial opportunities to develop other heterogeneous catalysts for efficient capture and converting of CO2.

Citation

WANG, Y., SUN, Y., WU, F., ZOU, G., GAUMET, J.-J., LI, J., FERNANDEZ, C., WANG, Y. and PENG, Q. 2024. Nitrogen-anchored boridene enables Mg−CO2 batteries with high reversibility. Journal of the American Chemical Society [online], 146(14), pages 9967–9974. Available from: https://doi.org/10.1021/jacs.4c00630

• Journal Article Type: Article
• Acceptance Date: Feb 22, 2024
• Online Publication Date: Mar 5, 2024
• Publication Date: Apr 10, 2024
• Deposit Date: Mar 25, 2024
• Publicly Available Date: Mar 6, 2025
• Journal: Journal of the American Chemical Society
• Print ISSN: 0002-7863
• Electronic ISSN: 1520-5126
• Publisher: American Chemical Society
• Peer Reviewed: Peer Reviewed
• Volume: 146
• Issue: 14
• Pages: 9967–9974
• DOI: https://doi.org/10.1021/jacs.4c00630
• Keywords: Batteries; Catalysts; Defects in solids; Diffraction; Energy
• Public URL: https://rgu-repository.worktribe.com/output/2271796
• Additional Information: This article has been published with separate supporting information. This supporting information has been incorporated into a single file on this repository and can be found at the end of the file associated with this output.