Journal
NANO LETTERS
Volume 18, Issue 5, Pages 3297-3302Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.8b01264
Keywords
Supercapacitors; semiconductor nanocrystals; electronic doping; aliovalent doping
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Funding
- U.S. National Science Foundation through the University of Washington Molecular Engineering Materials Center, a Materials Research Science and Engineering Center [DMR-1719797]
- U.S. National Science Foundation [CHE-1506014, CHE-1454930, CHE-1565520]
- State of Washington through the University of Washington Clean Energy Institute
- Washington Research Foundation
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Colloidal ZnO semiconductor nanocrystals have previously been shown to accumulate multiple delocalized conduction-band electrons under chemical, electrochemical, or photochemical reducing conditions, leading to emergent semimetallic characteristics such as quantum plasmon resonances and raising prospects for application in multielectron redox transformations. Here, we demonstrate a dramatic enhancement in the capacitance of colloidal ZnO nanocrystals through aliovalent Fe3+-doping. Very high areal and volumetric capacitances (33 mu F cm(-2), 233 F cm(-3)) are achieved in Zn-0.99 Fe0.01O nanocrystals that rival those of the best supercapacitors used in commercial energy-storage devices. The redox properties of these nanocrystals are probed by potentiometric titration and optical spectroscopy. These data indicate an equilibrium between electron localization by Fe3+ dopants and electron delocalization within the ZnO conduction band, allowing facile reversible charge storage and removal. As soluble supercapacitors, colloidal iron-doped ZnO nanocrystals constitute a promising class of solution-processable electronic materials with large charge-storage capacity attractive for future energy-storage applications.
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