Versatility of <i>π-d</i> Conjugated Coordination Nickel Metal-Organic Frameworks as Electrode Materials of Metal-Ion Batteries
Zaohong Zhang, Kaihui Xu, Jing Yang, Zhuoyu Ji, Yunchen Ge, Zhicong Shi, Yongwei Zhang, Kai Zhang, Chuan Wu, Jia Hong Pan
Abstract
Metal–organic frameworks have emerged as promising electrode materials for metal-ion batteries due to their superior structural customizability. However, they face challenges such as poor reversibility and easy degradation during electrochemical redox processes. Here, we report the synthesis of π-d conjugated coordination polymers through NH 3 -vapor-assisted self-polymerization of NiCl 2 ·6H 2 O with 1,2,4,5-benzenetetramine tetrahydrochloride (namely, Ni-BTA). The synthesized Ni-BTA exhibits an open lattice structure that enhances the capacity for metal-ion diffusion, ensuring prolonged electrochemical cycling stability. Moreover, electrochemical characterizations reveal that Ni-BTA functions as a bifunctional material, serving as both cathode and anode materials for lithium-ion batteries (LIBs). After 1,000 cycles at 1.0 A g −1 , the cathode and anode show high discharge capacities of 199.7 and 338.4 mAh g −1 , respectively. Additionally, symmetrical all-organic batteries constructed with Ni-BTA exhibit a high specific capacity of 30.6 mAh g –1 and an ultrastable coulombic efficiency of approximately ≈100% after 6,000 cycles at 1.0 A g −1 . Furthermore, Ni-BTA exhibits versatility as a robust cathode for aluminum ion batteries (AIBs), delivering a discharge capacity of 18.7 mAh g −1 after 10,000 cycles at 1.0 A g −1 . These findings highlight the potential of Ni-BTA as a versatile and durable electrode materials for both LIBs and AIBs.