Dual-Redox-Sites Enable Two-Dimensional Conjugated Metal-Organic Frameworks with Large Pseudocapacitance and Wide Potential Window

Zhang P, Wang M, Liu Y, Yang S, Wang F, Li Y, Chen G, Li Z, Wang G, Zhu M, Dong R, Yu M, Schmidt OG, Feng X (2021)

Publication Type: Journal article

Publication year: 2021

Journal

Journal of the American Chemical Society American Chemical Society

Book Volume: 143

Pages Range: 10168-10176

Journal Issue: 27

DOI: 10.1021/jacs.1c03039

Abstract

Advanced supercapacitor electrodes require the development of materials with dense redox sites embedded into conductive and porous skeletons. Two-dimensional (2D) conjugated metal-organic frameworks (c-MOFs) are attractive supercapacitor electrode materials due to their high intrinsic electrical conductivities, large specific surface areas, and quasi-one-dimensional aligned pore arrays. However, the reported 2D c-MOFs still suffer from unsatisfying specific capacitances and narrow potential windows because large and redox-inactive building blocks lead to low redox-site densities of 2D c-MOFs. Herein, we demonstrate the dual-redox-site 2D c-MOFs with copper phthalocyanine building blocks linked by metal-bis(iminobenzosemiquinoid) (M2[CuPc(NH)8], M = Ni or Cu), which depict both large specific capacitances and wide potential windows. Experimental results accompanied by theoretical calculations verify that phthalocyanine monomers and metal-bis(iminobenzosemiquinoid) linkages serve as respective redox sites for pseudocapacitive cation (Na+) and anion (SO42-) storage, enabling the continuous Faradaic reactions of M2[CuPc(NH)8] occurring in a large potential window of -0.8 to 0.8 V vs Ag/AgCl (3 M KCl). The decent conductivity (0.8 S m-1) and high active-site density further endow the Ni2[CuPc(NH)8] with a remarkable specific capacitance (400 F g-1 at 0.5 A g-1) and excellent rate capability (183 F g-1 at 20 A g-1). Quasi-solid-state symmetric supercapacitors are further assembled to demonstrate the practical application of Ni2[CuPc(NH)8] electrode, which deliver a state-of-the-art energy density of 51.6 Wh kg-1 and a peak power density of 32.1 kW kg-1.

Involved external institutions

Technische Universität Dresden DE Germany (DE) Technische Universität Chemnitz DE Germany (DE) Helmholtz-Zentrum Dresden-Rossendorf (HZDR) DE Germany (DE)

How to cite

APA:

Zhang, P., Wang, M., Liu, Y., Yang, S., Wang, F., Li, Y.,... Feng, X. (2021). Dual-Redox-Sites Enable Two-Dimensional Conjugated Metal-Organic Frameworks with Large Pseudocapacitance and Wide Potential Window. Journal of the American Chemical Society, 143(27), 10168-10176. https://doi.org/10.1021/jacs.1c03039

MLA:

Zhang, Panpan, et al. "Dual-Redox-Sites Enable Two-Dimensional Conjugated Metal-Organic Frameworks with Large Pseudocapacitance and Wide Potential Window." Journal of the American Chemical Society 143.27 (2021): 10168-10176.

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