Redox-Active Metaphosphate-Like Terminals Enable High-Capacity MXene Anodes for Ultrafast Na-Ion Storage,Advanced Materials

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Redox-Active Metaphosphate-Like Terminals Enable High-Capacity MXene Anodes for Ultrafast Na-Ion Storage
Advanced Materials ( IF 27.4 ) Pub Date : 2022-02-11 , DOI: 10.1002/adma.202108682
Boya Sun _{1,

2} , Qiongqiong Lu ₃ , Kaixuan Chen ₄ , Wenhao Zheng ₅ , Zhongquan Liao ₆ , Nikolaj Lopatik ₇ , Dongqi Li ₂ , Martin Hantusch ₃ , Shengqiang Zhou ₈ , Hai I Wang ₅ , Zdeněk Sofer ₉ , Eike Brunner ₇ , Ehrenfried Zschech ₁₀ , Mischa Bonn ₅ , Richard Dronskowski ₄ , Daria Mikhailova ₃ , Qinglei Liu ₁ , Di Zhang ₁ , Minghao Yu ₂ , Xinliang Feng _{2,

11}

Affiliation

State Key Laboratory of Metal Matrix Composites, School of Materials Science and Engineering, Shanghai Jiao Tong University, Shanghai, 200240, China.
Faculty of Chemistry and Food Chemistry & Center for Advancing Electronics Dresden (cfaed), Technische Universität Dresden, 01062, Dresden, Germany.
Leibniz Institute for Solid State and Materials Research (IFW) Dresden e.V., 01069, Dresden, Germany.
Chair of Solid-State and Quantum Chemistry, Institute of Inorganic Chemistry, RWTH Aachen University, D-52056, Aachen, Germany.
Max Planck Institute for Polymer Research, Ackermannweg 10, D-55128, Mainz, Germany.
Fraunhofer Institute for Ceramic Technologies and Systems (IKTS), Maria-Reiche-Strasse 2, 01109, Dresden, Germany.
Chair of Bioanalytical Chemistry, Faculty of Chemistry and Food Chemistry, Technische Universität Dresden, 01062, Dresden, Germany.
Institute of Ion Beam Physics and Materials Research, Helmholtz-Zentrum Dresden-Rossendorf, 01328, Dresden, Germany.
Department of Inorganic Chemistry, University of Chemistry and Technology Prague, Technická 5, Prague 6, 166 28, Czech Republic.
Faculty of Chemistry, University of Warsaw, ul. Żwirki i Wigury 101, Warsaw, 02-089, Poland.
Max Planck Institute of Microstructure Physics, Weinberg 2, 06120, Halle, Germany.

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 PO bonds and one PO 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.

中文翻译：

氧化还原活性类偏磷酸盐端子使高容量 MXene 阳极可用于超快钠离子存储

二维过渡金属碳化物和/或氮化物，即所谓的 MXene，被认为是理想的快速充电阳离子插层电极材料，但其比容量有限。在此，据报道，构建具有氧化还原活性的磷-氧末端可能是 Nb ₄ C ₃ MXenes 显着提高其超快 Na ⁺存储比容量的一种有吸引力的策略。_{如所揭示的，具有 PO 2}化学计量式的氧化还原活性末端显示出类似偏磷酸盐的构型，其中每个 P 原子维持三个P O 键和一个 PO 悬空键。与传统的O-末端相比，类偏磷酸盐末端赋予Nb ₄ C ₃（表示为 PO ₂ -Nb ₄ C ₃）具有显着丰富的载流子密度（四倍）、提高的电导率（在 300 K 时为 12.3 倍）、额外的氧化还原活性位点、提高的 Nb 氧化还原深度、不下降的 Na ⁺扩散能力和缓冲Na ⁺嵌入/脱嵌过程中的内应力。因此，与O-封端的Nb ₄ C ₃相比，PO ₂ -Nb ₄ C ₃表现出两倍的Na ⁺ -存储容量（221.0 mAh g ^-1）、良好的快速充电能力（80% 容量保持时 4.9 分钟）、显着提高循环寿命（超过 2000 次循环的非退化容量）以及组装能量-功率平衡的钠离子电容器的合理可行性。这项研究揭示了 MXene 终端的分子级设计为同时开发高容量和快速充电电极提供了机会，从而缓解了储能设备典型的能量-功率权衡。

更新日期：2022-02-11

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