Journal Article

PUBDB-2023-07729

http://join2-wiki.gsi.de/foswiki/pub/Main/Artwork/join2_logo100x88.png Reversible Metal and Ligand Redox Chemistry in Two-Dimensional Iron–Organic Framework for Sustainable Lithium-Ion Batteries

Geng, J. ; Ni, Y. ; Zhu, Z. ; Wu, Q. ; Gao, S. ; Hua, W.Extern* ; Indris, S.Extern* ; Chen, J. ; Li, F. (Corresponding author)

2023
ACS Publications Washington, DC

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Please use a persistent id in citations: doi:10.1021/jacs.2c08273

Abstract: Metal–organic frameworks (MOFs) are emerging as attractive electrode materials for lithium-ion batteries, owing to their fascinating features of sustainable resources, tunable chemical components, flexible molecular skeletons, and renewability. However, they are faced with a limited number of redox-active sites and unstable molecular frameworks during electrochemical processes. Herein, we design a novel two-dimensional (2D) iron(III)-tetraamino-benzoquinone (Fe-TABQ) with dual redox centers of Fe cations and TABQ ligands for high-capacity and stable lithium storage. It is constructed of square-planar Fe–N$_2$O$_2$ linkages and phenylenediamine building blocks, between which the Fe-TABQ chains are connected by multiple hydrogen bonds, and then featured as an extended π–d-conjugated 2D structure. The redox chemistry of both Fe$^{3+}$ cations and TABQ anions is revealed to render its remarkable specific capacity of 251.1 mAh g$^{–1}$. Benefiting from the intrinsic robust Fe–N(O) bonds and reinforced Li–N(O) bonds during cycling, Fe-TABQ delivers high capacity retentions over 95% after 200 cycles at various current densities. This work will enlighten more investigations for the molecular designs of advanced MOF-based electrode materials.

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Contributing Institute(s):

1. DOOR-User (DOOR ; HAS-User)

Research Program(s):

1. 6G3 - PETRA III (DESY) (POF4-6G3) (POF4-6G3)

Experiment(s):

1. PETRA Beamline P64 (PETRA III)

Appears in the scientific report 2023

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