Redox‐Active Metaphosphate‐Like Terminals Enable High‐Capacity MXene Anodes for Ultrafast Na‐Ion Storage
Advanced Materials, vol. 34, pp. e2108682
Abstract
Abstract 2D transition metal carbides and/or nitrides, so‐called MXenes, are noted as ideal fast‐charging cation‐intercalation electrode materials, which nevertheless suffer from limited specific capacities. Herein, it is reported that constructing redox‐active phosphorus−oxygen terminals can be an attractive strategy for Nb4C3 MXenes to remarkably boost their specific capacities for ultrafast Na+ storage. As revealed, redox‐active terminals with a stoichiometric formula of PO2‐ display a metaphosphate‐like configuration with each P atom sustaining three PO bonds and one PO dangling bond. Compared with conventional O‐terminals, metaphosphate‐like terminals empower Nb4C3 (denoted PO2‐Nb4C3) with considerably enriched carrier density (fourfold), improved conductivity (12.3‐fold at 300 K), additional redox‐active sites, boosted Nb redox depth, nondeclined Na+‐diffusion capability, and buffered internal stress during Na+ intercalation/de‐intercalation. Consequently, compared with O‐terminated Nb4C3, PO2‐Nb4C3 exhibits a doubled Na+‐storage capacity (221.0 mAh g‐1), well‐retained fast‐charging capability (4.9 min at 80% capacity retention), significantly promoted cycle life (nondegraded capacity over 2000 cycles), and justified feasibility for assembling energy−power‐balanced Na‐ion capacitors. This study unveils that the molecular‐level design of MXene terminals provides opportunities for developing simultaneously high‐capacity and fast‐charging electrodes, alleviating the energy−power tradeoff typical for energy‐storage devices.
Authors 20
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Shanghai Jiao Tong University · State Key Laboratory of Metal Matrix Composites · Center for Advancing Electronics Dresden · Technische Universität Dresden
Affiliation as printed
Faculty of Chemistry and Food Chemistry & Center for Advancing Electronics Dresden (cfaed) Technische Universität Dresden 01062 Dresden Germany
State Key Laboratory of Metal Matrix Composites School of Materials Science and Engineering Shanghai Jiao Tong University Shanghai 200240 China
State Key Laboratory of Metal Matrix Composites, School of Materials Science and Engineering, Shanghai Jiao Tong University, Shanghai, 200240 China
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Leibniz Institute for Solid State and Materials Research
Affiliation as printed
Leibniz Institute for Solid State and Materials Research (IFW) Dresden e.V. 01069 Dresden Germany
Leibniz Institute for Solid State and Materials Research (IFW) Dresden e.V., 01069 Dresden, Germany
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Kaixuan Chen Aachen Chair of Solid‐State and Quantum Chemistry Institute of Inorganic Chemistry Chair of Solid-State and Quantum Chemistry Institute of Inorganic Chemistry
Affiliation as printed
Chair of Solid‐State and Quantum Chemistry Institute of Inorganic Chemistry RWTH Aachen University D‐52056 Aachen Germany
Chair of Solid-State and Quantum Chemistry, Institute of Inorganic Chemistry, RWTH Aachen University, D-52056 Aachen, Germany
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Max Planck Institute for Polymer Research
Affiliation as printed
Max Planck Institute for Polymer Research Ackermannweg 10 D‐55128 Mainz Germany
Max Planck Institute for Polymer Research, Ackermannweg 10, D-55128 Mainz, Germany
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Fraunhofer Institute for Ceramic Technologies and Systems
Affiliation as printed
Fraunhofer Institute for Ceramic Technologies and Systems (IKTS) Maria‐Reiche‐Strasse 2 01109 Dresden Germany
Fraunhofer Institute for Ceramic Technologies and Systems (IKTS), Maria-Reiche-Strasse 2, 01109 Dresden, Germany
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Technische Universität Dresden
Affiliation as printed
Chair of Bioanalytical Chemistry Faculty of Chemistry and Food Chemistry Technische Universität Dresden 01062 Dresden Germany
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Center for Advancing Electronics Dresden · Technische Universität Dresden
Affiliation as printed
Faculty of Chemistry and Food Chemistry & Center for Advancing Electronics Dresden (cfaed) Technische Universität Dresden 01062 Dresden Germany
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Leibniz Institute for Solid State and Materials Research
Affiliation as printed
Leibniz Institute for Solid State and Materials Research (IFW) Dresden e.V. 01069 Dresden Germany
Leibniz Institute for Solid State and Materials Research (IFW) Dresden e.V., 01069 Dresden, Germany
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Helmholtz-Zentrum Dresden-Rossendorf
Affiliation as printed
Institute of Ion Beam Physics and Materials Research Helmholtz‐Zentrum Dresden‐Rossendorf 01328 Dresden Germany
Institute of Ion Beam Physics and Materials Research, Helmholtz-Zentrum Dresden-Rossendorf, 01328 Dresden, Germany
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Max Planck Institute for Polymer Research
Affiliation as printed
Max Planck Institute for Polymer Research Ackermannweg 10 D‐55128 Mainz Germany
Max Planck Institute for Polymer Research, Ackermannweg 10, D-55128 Mainz, Germany
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University of Chemistry and Technology, Prague
Affiliation as printed
Department of Inorganic Chemistry University of Chemistry and Technology Prague Technická 5 Prague 6 166 28 Czech Republic
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Technische Universität Dresden
Affiliation as printed
Chair of Bioanalytical Chemistry Faculty of Chemistry and Food Chemistry Technische Universität Dresden 01062 Dresden Germany
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Affiliation as printed
Faculty of Chemistry University of Warsaw ul. Żwirki i Wigury 101 Warsaw 02‐089 Poland
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Max Planck Institute for Polymer Research
Affiliation as printed
Max Planck Institute for Polymer Research Ackermannweg 10 D‐55128 Mainz Germany
Max Planck Institute for Polymer Research, Ackermannweg 10, D-55128 Mainz, Germany
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Richard Dronskowski Aachen Chair of Solid‐State and Quantum Chemistry Institute of Inorganic Chemistry Chair of Solid-State and Quantum Chemistry Institute of Inorganic Chemistry
Affiliation as printed
Chair of Solid‐State and Quantum Chemistry Institute of Inorganic Chemistry RWTH Aachen University D‐52056 Aachen Germany
Chair of Solid-State and Quantum Chemistry, Institute of Inorganic Chemistry, RWTH Aachen University, D-52056 Aachen, Germany
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Leibniz Institute for Solid State and Materials Research
Affiliation as printed
Leibniz Institute for Solid State and Materials Research (IFW) Dresden e.V. 01069 Dresden Germany
Leibniz Institute for Solid State and Materials Research (IFW) Dresden e.V., 01069 Dresden, Germany
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Qinglei Liu corresponding
Shanghai Jiao Tong University · State Key Laboratory of Metal Matrix Composites
Affiliation as printed
State Key Laboratory of Metal Matrix Composites School of Materials Science and Engineering Shanghai Jiao Tong University Shanghai 200240 China
State Key Laboratory of Metal Matrix Composites, School of Materials Science and Engineering, Shanghai Jiao Tong University, Shanghai, 200240 China
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Shanghai Jiao Tong University · State Key Laboratory of Metal Matrix Composites
Affiliation as printed
State Key Laboratory of Metal Matrix Composites School of Materials Science and Engineering Shanghai Jiao Tong University Shanghai 200240 China
State Key Laboratory of Metal Matrix Composites, School of Materials Science and Engineering, Shanghai Jiao Tong University, Shanghai, 200240 China
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Minghao Yu corresponding
Center for Advancing Electronics Dresden · Technische Universität Dresden
Affiliation as printed
Faculty of Chemistry and Food Chemistry & Center for Advancing Electronics Dresden (cfaed) Technische Universität Dresden 01062 Dresden Germany
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Xinliang Feng corresponding
Max Planck Institute of Microstructure Physics · Center for Advancing Electronics Dresden · Technische Universität Dresden
Affiliation as printed
Faculty of Chemistry and Food Chemistry & Center for Advancing Electronics Dresden (cfaed) Technische Universität Dresden 01062 Dresden Germany
Max Planck Institute of Microstructure Physics Weinberg 2 06120 Halle Germany
Faculty of Chemistry and Food Chemistry & Center for Advancing Electronics Dresden (cfaed) Technische Universität Dresden 01062 Dresden Germany
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