Journal article
Mechanistic Understanding of the Interactions and Pseudocapacitance of Multi-Electron Redox Organic Molecules Sandwiched between MXene Layers
Advanced electronic materials, v 7(4), 2001202
Apr 2021
Featured in Collection : UN Sustainable Development Goals @ Drexel
Abstract
Using a combined theoretical and experimental approach, a mechanistic understanding of the interactions and pseudocapacitance of different quinone-coupled viologen and pyridiniumium molecules sandwiched between titanium carbide (Ti3C2Tx) MXene layers has been provided. Three different derivatives of quinone-coupled viologen and pyridiniumium are synthesized using nucleophilic substitution reaction and subsequently hybridized with Ti3C2Tx MXene (organic@Ti3C2Tx) using self-assembly approach. The atomic structure of pristine Ti3C2Tx and organic@Ti3C2Tx hybrid films is investigated using grazing incidence X-ray diffraction and X-ray pair distribution function analysis using synchrotron radiation. Spectroscopic results confirm the coupling of quinones with viologen and pyridiniumium molecules and their non-covalent functionalization to the MXene without their catalytic decomposition. First-principles calculations confirm that the preferred orientation of organic molecules upon intercalation/adsorption is horizontal to the Ti3C2Tx surface. The authors reveal that these molecules attach to the Ti3C2Tx surface with a significantly high binding energy (up to -2.77 eV) via a charge transfer mechanism. The electronic structure calculations show that all organic@Ti3C2Tx hybrids preserved their metallic behavior. Free-standing organic@Ti3C2Tx hybrid films show a more than three times higher capacitance at ultra-high scan rates (up to 20 V s(-1)) compared to their pristine counterpart due to molecular pillaring of organic molecules between Ti3C2Tx layers via strong binding energies and charge transfer.
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Details
- Title
- Mechanistic Understanding of the Interactions and Pseudocapacitance of Multi-Electron Redox Organic Molecules Sandwiched between MXene Layers
- Creators
- Muhammad BootaTanveer Hussain - University of QueenslandLong Yang - Columbia Univ, Dept Appl Phys & Appl Math, New York, NY 10027 USAMatthieu BecuweWilliam Porzio - Consiglio Nazl Ric SCI TEC, Inst Chem Sci & Technol G Natta, A Corti 12, I-20133 Milan, ItalyLuisa Barba - Elettra-Sincrotrone Trieste S.C.p.A.Rajeev Ahuja - Royal Inst Technol, KTH, S-10044 Stockholm, Sweden
- Publication Details
- Advanced electronic materials, v 7(4), 2001202
- Publisher
- Wiley
- Grant note
- The authors thank Prof. Yury Gogotsi for guiding this work. This work was supported as part of the Fluid Interface Reactions, Structures and Transport (FIRST) Center, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, and Office of Basic Energy Sciences. L.Y.'s effort on PDF analysis and modeling was supported by the NSF MRSEC program through Columbia in the Center for Precision Assembly of Superstratic and Superatomic Solids (DMR-1420634). X-ray PDF measurements were conducted on beamline 28-ID-2 of the National Synchrotron Light Source II (NSLS-II), a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under Contract No. DE-SC0012704. R.A. thanks Swedish Research Council (VR-2016-06014) for financial support. SNIC and HPC2N are acknowledged for providing the computing facilities.
- Resource Type
- Journal article
- Language
- English
- Academic Unit
- Drexel University
- Web of Science ID
- WOS:000629302100001
- Scopus ID
- 2-s2.0-85102497084
- Other Identifier
- 991021860750604721
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- Collaboration types
- Domestic collaboration
- International collaboration
- Web of Science research areas
- Materials Science, Multidisciplinary
- Nanoscience & Nanotechnology
- Physics, Applied