Issue 38, 2024

Boosted Li2CO3 reversible conversion utilizing Cu-doped TiB MBene/graphene for Li–CO2 batteries

Abstract

Two-dimensional transition metal borides (MBenes), particularly TiB, hold promise as electrocatalysts for CO2-related reactions. However, their bifunctional catalytic performance for reversible Li2CO3 conversion in Li–CO2 batteries remains inferior to that of Ru-based catalysts. We addressed this issue by introducing tensile strain and doping late transition metal atoms (Mn, Fe, Co, Ni, Cu) into the basal plane of a TiB MBene/graphene heterostructure. Spin-polarized density functional theory (DFT) calculations revealed that the Cu-doped TiB/graphene catalyst (Cu/Ti17B18/G) exhibits an ultralow CO2 reduction and evolution overpotential of 0.66 V, enhancing Li2CO3 nucleation and reversible conversion with carbon products. This improvement is attributed to weakened adsorption of O-containing intermediates on the Cu-doped surface, facilitated by the down-shifted d-band center and increased antibonding state occupancy. Consequently, Cu/Ti17B18/G emerges as a promising bifunctional electrocatalyst for Li–CO2 batteries, outperforming pristine TiB/G and other reported catalysts. Furthermore, its bifunctional activity can be further improved by applying x-direction tensile strain. Molecular dynamics simulations combined with explicit solvent models further confirmed the catalytic durability and stability of Cu/Ti17B18/G in solution. This work provides valuable atomic-scale insights for exploring advanced Li–CO2 battery catalysts.

Graphical abstract: Boosted Li2CO3 reversible conversion utilizing Cu-doped TiB MBene/graphene for Li–CO2 batteries

Supplementary files

Article information

Article type
Paper
Submitted
31 Jul 2024
Accepted
02 Sep 2024
First published
02 Sep 2024

J. Mater. Chem. A, 2024,12, 25887-25895

Boosted Li2CO3 reversible conversion utilizing Cu-doped TiB MBene/graphene for Li–CO2 batteries

T. Luo, Q. Peng, M. Yang, H. Hu, J. Ding, Y. Chen, X. Gong, J. Yang, Y. Qu, Z. Zhou, X. Qi and Z. Sun, J. Mater. Chem. A, 2024, 12, 25887 DOI: 10.1039/D4TA05343E

To request permission to reproduce material from this article, please go to the Copyright Clearance Center request page.

If you are an author contributing to an RSC publication, you do not need to request permission provided correct acknowledgement is given.

If you are the author of this article, you do not need to request permission to reproduce figures and diagrams provided correct acknowledgement is given. If you want to reproduce the whole article in a third-party publication (excluding your thesis/dissertation for which permission is not required) please go to the Copyright Clearance Center request page.

Read more about how to correctly acknowledge RSC content.

Social activity

Spotlight

Advertisements