Abstract

Conjugated coordination polymers attract attention as materials for electrochemical energy storage, mostly as cathode materials for supercapacitors. Faradaic capacity may be introduced to such materials using redox-active building blocks, metals, or ligands. Using this strategy, a novel hybrid cathode material was developed based on a Ni2+ metal-organic polymer. The proposed material, in addition to double-layer capacitance, shows high pseudocapacitance, which arises from the contributions of both the metal center and ligand. A tailoring strategy in the ligand design allows us to minimize the molecular weight of the ligand, which increases its gravimetric energy. According to computational results, the ligand makes the prevailing contribution to the pseudocapacitance of the material. Different approaches to metal–organic polymer (MOP) synthesis were implemented, and the obtained materials were examined by FTIR, Raman spectroscopy, powder XRD, SEM/EDX (energy-dispersive X-ray spectroscopy), TEM, and thermal analysis. Energy-storage performance was comparatively studied with cyclic voltammetry (CV) and galvanostatic charge–discharge (GCD). As a result, materials with an excellent discharge capacity were obtained, reaching the gravimetric energy density of common inorganic cathode materials.

Highlights

  • The development of electric transportation, mobile electronic devices, the Internet of Things network, and renewable energy sources require new types of energy-storage devices with increased values of both energy and power density [1]

  • The bottleneck limiting the specific energy and power of whole lithium-ion batteries (LIBs) is the galvanostatic charge–discharge (GCD) performance of traditional oxide cathode materials, so the development of fast cathode materials is the first task to be solved in this way

  • The material combining the advantages of both metal–organic polymer (MOP) and polyNiSalens was synthesized. The performance of this MOP as a cathode material for LIB was examined by cyclic voltammetry (CV) and galvanostatic charge–discharge (GCD)

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Summary

Introduction

The development of electric transportation, mobile electronic devices, the Internet of Things network, and renewable energy sources require new types of energy-storage devices with increased values of both energy and power density [1]. The bottleneck limiting the specific energy and power of whole LIB is the galvanostatic charge–discharge (GCD) performance of traditional oxide cathode materials, so the development of fast cathode materials is the first task to be solved in this way. In this course, hybrid materials combining redox- and double-layer capacitance are sought. A special class of conductive polymers, polymeric bis (salicylideniminato) nickel complexes (polyNiSalens, Figure 1b) perfectly fits the above requirements [18] It possesses high electronic conductivity [19], excellent cyclability as a cathode material for LIBs, and increased thermal stability. The performance of this MOP as a cathode material for LIB was examined by cyclic voltammetry (CV) and galvanostatic charge–discharge (GCD)

General Considerations
Synthesis
Half-Cell Fabrication
Electrochemical Studies
Computations
Results and Discussion

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