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.
| Identifer | oai:union.ndltd.org:DRESDEN/oai:qucosa:de:qucosa:80113 |
| Date | 26 July 2022 |
| Creators | Zhang, Panpan, Wang, Mingchao, Liu, Yannan, Yang, Sheng, Wang, Faxing, Li, Yang, Chen, Guangbo, Li, Zichao, Wang, Gang, Zhu, Minshen, Dong, Renhao, Yu, Minghao, Schmidt, Oliver G., Feng, Xinliang |
| Publisher | American Chemical Society |
| Source Sets | Hochschulschriftenserver (HSSS) der SLUB Dresden |
| Language | English |
| Detected Language | English |
| Type | info:eu-repo/semantics/acceptedVersion, doc-type:article, info:eu-repo/semantics/article, doc-type:Text |
| Rights | info:eu-repo/semantics/openAccess |
| Relation | 1520-5126, 10.1021/jacs.1c03039, info:eu-repo/grantAgreement/European Commission/H2020 SGA-RIA/881603//Graphene Flagship Core Project 3/GrapheneCore3, info:eu-repo/grantAgreement/European Commission/H2020 ERC ERC-COG/819698//Development of Thiophene Based Conjugated Polymers in Two Dimensions/T2DCP, info:eu-repo/grantAgreement/European Commission/H2020 ERC ERC-STG/852909//Development of Functional Conjugated Two-Dimensional Metal-Organic Frameworks/FC2DMOF, info:eu-repo/grantAgreement/Deutsche Forschungsgemeinschaft/Sachbeihilfen/399684426//MXen–Organische Halbleiter-Verschnitte mit hohen Ladungsträgermobilitäten für die Anwendung in gedruckter Organischer Elektronik/MX-OSMOPED, info:eu-repo/grantAgreement/Sächsisches Staatsministerium für Wissenschaft und Kunst/M-ERA-NET/100478697//Synthesis and characterization of novel 2D hybrid materials for supercapacitors/HYSUCAP, info:eu-repo/grantAgreement/Deutsche Forschungsgemeinschaft/Sonderforschungsbereiche/417590517//Chemie der synthetischen zweidimensionalen Materialien/SFB 1415, info:eu-repo/grantAgreement/Deutsche Forschungsgemeinschaft/Schwerpunktprogramme/422726248//Polymer-basierte Batterien/SPP 2248, info:eu-repo/grantAgreement/Deutsche Forschungsgemeinschaft/Schwerpunktprogramme/441208651//Redox-aktive kovalente organische Gerüstverbindungen für die Einlagerung mehrwertiger Metallione/RACOF-MMIS, info:eu-repo/grantAgreement/Deutsche Forschungsgemeinschaft/Schwerpunktprogramme/273920491//Koordinationsnetzwerke als Bausteine für Funktionssysteme/SPP 1928 |
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