Tailoring Electronic Structure and Size of Ultrastable Metalated Metal–Organic Frameworks with Enhanced Electroconductivity for High‐Performance Supercapacitors
Utilization of metal–organic frameworks (MOFs) as electrodes for energy storage/conversion is challenging because of the low chemical stability and poor electrical conductivity of MOFs in electrolytes. A nanoscale MOF, Co0.24Ni0.76‐bpa‐200, possessing ultrahigh stability with uncommon semiconductor...
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Published in | Angewandte Chemie International Edition Vol. 60; no. 18; pp. 10228 - 10238 |
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Main Authors | , , , , , , , , , , |
Format | Journal Article |
Language | English |
Published |
Germany
Wiley Subscription Services, Inc
26.04.2021
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Edition | International ed. in English |
Subjects | |
Online Access | Get full text |
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Summary: | Utilization of metal–organic frameworks (MOFs) as electrodes for energy storage/conversion is challenging because of the low chemical stability and poor electrical conductivity of MOFs in electrolytes. A nanoscale MOF, Co0.24Ni0.76‐bpa‐200, possessing ultrahigh stability with uncommon semiconductor behavior (σ=4.2×10−3 S m−1) was fabricated. The MOF comprises a robust hydrophobic paddlewheel and an optimized Co/Ni ratio, with consequent control over MOF size and the degree of conjugation of the coligand. A DFT study revealed that appropriate Ni2+ doping reduces the activation energy of the system, thus providing a higher carrier concentration, and the strongly delocalized N‐donor ligand notably increases the metal–ligand orbital overlap to achieve efficient charge migration, leading to continuous through‐bond (‐CoNi‐N‐CoNi‐)∞ conduction paths. These structural features endow the MOF with a good cycling stability of 86.5 % (10 000 cycles) and a high specific capacitance of 1927.14 F g−1 among pristine MOF‐based electrodes.
An elaborately designed 3D metal–organic framework (MOF) integrating excellent chemical stability and good conductivity was obtained through a combination of ligand delocalization, activation energy, and morphology parameters. The superiority of the as‐prepared pristine MOF‐based supercapacitor electrode was structurally and electrochemically identified in detail. |
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Bibliography: | These authors contributed equally to this work. ObjectType-Article-1 SourceType-Scholarly Journals-1 ObjectType-Feature-2 content type line 23 |
ISSN: | 1433-7851 1521-3773 |
DOI: | 10.1002/anie.202100123 |