Recent advances in MXene-based nanomaterials for high-performance lithium metal anodes
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摘要: 锂金属负极由于其具有高的理论容量和低的电化学电势，被认为是高能量密度可充电电池中最具吸引力和前景的负极。然而，其在镀/脱锂过程中，锂枝晶的不可控生长导致了电极的快速退化和严重的安全问题，严重阻碍了其实际应用。为了解决这些问题，使用具有高电导率、优异机械性能和丰富表面官能团的二维过渡金属碳化物/氮化物（MXenes）来诱导锂均匀成核并缓解体积变化，最终抑制锂枝晶的形成。本文综述了用于金属锂负极的MXene基纳米材料的最新进展。首先介绍了金属锂负极的技术挑战。然后从三个方面总结了MXene基纳米材料用于抑制锂枝晶生长和构建稳定金属锂负极的设计和使用：（1）使用结构化负极，如MXene/锂负极、MXene/金属/锂负极、MXene/碳/锂负极、MXene/氧化物/锂负极等；（2）构建人工SEI膜；（3）修饰电解液成分。最后，简要讨论了MXene基纳米材料在下一代锂金属电池应用中的挑战和前景。Abstract: To tackle the issues of rapid electrode degradation and severe safety issues caused by the uncontrollable growth of lithium dendrites in Li metal anodes (LMAs), two-dimensional transition metal carbides/nitrides (MXenes) with a high electrical conductivity, excellent mechanical properties, and abundant surface functional groups have been used as hosts to induce uniform Li nucleation and alleviate the volume changes, eventually inhibiting the formation of Li dendrites. Recent advances in the use of MXene-based nanomaterials in LMAs are summarized. The problems with using LMAs are first considered, and the ways of using MXene-based nanomaterials for suppressing Li dendrite growth and constructing stable LMAs are then summarized. These include the use of MXenes, MXene-metal hybrids, MXene-carbon hybrids, and MXene derivatives as hosts for the anodes and as additives to modify the electrolyte compositions to increase ionic conductivity and inhibit polymer crystallization. Finally, the challenges and prospects for using MXene-based nanomaterials in next-generation LMAs are briefly discussed.
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Key words:
- Lithium metal anodes /
- MXene /
- Dendrites /
- Lithium metal batteries
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Figure 1. Schematic diagram of the applications of MXene-based nanomaterials for lithium metal anodes
Figure 2. (a) Schematic illustration of the synthesis of Ti3C2 MXene (graphene, BN)-lithium films[66]; (b) SEM image of the Ti3C2-Li composite anode[66]; (c) Cross-sectional SEM image of the Ti3C2-Li composite anode[66]; (d) Schematic showing the sufficient transport pathways for electron and Li-ion in Ti3C2-Li composite anode[66]; (e) Schematic illustration of lithium plating on bare lithium and parallelly aligned MXene (PA-MXene) layers[67]; (f) Typical SEM images of PA-MXene layers on lithium. Inset in (f) is the top view of PA-MXene[67]; (g) Two-side press of MXene stacks onto a thin Li host[69]; (h) SEM images of the ILC-Li electrode upon plating at 3 mA cm−2 and 3 mAh cm−2[69]; (i) SEM images of the ILC-Li electrode upon stripping at 3 mA cm−2 and 3 mAh cm−2[69]. Reprinted with permission
Figure 3. (a) The synthesis schematic diagram of v-Ti3C2Tx electrodes[70]; (b-c) Top view SEM image of v-Ti3C2Tx electrodes[70]; (d) Cross-section SEM image of v-Ti3C2Tx electrodes[70]; (e) Coulombic efficiencies of v-Ti3C2Tx and h-Ti3C2Tx electrodes at 1.0 mA cm−2 for 1.0 mAh cm−2[70]; (f) Schematic illustration of the stripping and plating states of perpendicular MXene-Li and rGO-Li arrays. The left bottom in a) is the SEM images of as-prepared perpendicular MXene-Li arrays. The middle bottom in panel (a) is the SEM image of perpendicular MXene-Li arrays after lithium stripping for 20 mAh cm−271; (g) Top view SEM images of perpendicular MXene-Li arrays[71]; (h) Top view SEM images of rGO-Li[71]; (i) Scheme of the fabrication of Ti3C2Tx MXene and a high-concentration MXene ink (~300 mg mL−1)[75]; (j) Scheme of 3D printing MXene arrays and lattices to guide the nucleation and growth of lithium[75]. Reprinted with permission
Figure 4. (a) The Top view SEM images of MXene paper[81]; (b) The Top view SEM images of MXene@Au paper[81]; (c) Cross-sectional SEM image of MXene@Au paper[81]; (d) TEM image of Ti3C2Tx@Au paper[81]; (e) HRTEM image of Ti3C2Tx@Au paper[81]; (f) Cross-sectional SEM image a of Ti3C2Tx MXene@Zn paper[83]; (g) Top view SEM images of MXene@RP paper[85]; (h) TEM images of MXene@RP paper[85]; (i) SEM image of NS-Nb2C[86]. Reprinted with permission
Figure 5. (a) Schematic illustration of Li deposition in the lamellar-structured CNT/MXene/SnO2 composite host based on lithiophilic gradient[93]; (b) Cross-sectional SEM image of the CNT/MXene/SnO2 host[93]; (c) Schematic illustration of lithium plating on MXene@CNF film[94]; (d) Magnified SEM image of MXene@CNF film[94]; (e) Schematic illustration of the C-MXene/AgNW scaffold fabrication[95]; (f) Magnified SEM image showing a joint of the C0.5-MXene/AgNW scaffold[95]; (g) The schematic diagram for the Li stripping-plating process of Ti3C2-LiB-Li hybrid and LiB-Li[96]; (h) The corresponding cross-section image of the Ti3C2-LiB-Li[96]. Reprinted with permission
Figure 6. (a) The Ti3C2 MXene aerogel scaffolds for Li metal anodes[98]; (b) SEM image of the MXene/rGO aerogel. Inset: a photograph of the aerogel[98]; (c) Schematic diagram of Li-Ti3C2Tx-rGO preparation[99]; (d) SEM cross-section images of Ti3C2Tx-rGO[99]; (e) Schematic illustration of the fabrication process of the 3D MG-Li anode and corresponding photographs of the MGO film, MG film, and MG-Li anode[100]; (f) SEM image of the MG film. Inset is a photograph of the bent MG film[100]; (g) Schematic illustration of the fabrication process of the 3D MXene-MF for the alkali-metal anode[101]; (h) SEM image of MXene-MF[101]. Reprinted with permission
Figure 7. (a) Schematic illustration of the fabrication process of Ti3C2Tx/g-C3N4 hybrid[104]; (b) SEM image of Ti3C2Tx/g-C3N4[104]; (c) Voltage-time profiles of Li plating/stripping in different symmetric cells with the capacity of 0.5 mAh cm−2 at 0.5 mA cm−2 and Detailed voltage profiles for selective cycles in panel[104]; (d) Schematic diagram of the in-situ generation process of MA-SEI in the Li metal anode interface[105]; (e) Schematic illustration for the Li deposition and migration processes occurring at the Nb2CTX Li-In alloy anode[106]. Reprinted with permission
Table 1. Summary of the MXene-based nanomaterials for Li-metal anodes
Electrodes Current density/(mA cm−2) Capacity/(mAh cm−2) Electrolyte Overpotential/mV Cycle life/h Ref. Ti3C2 MXene
(graphene, BN)1 mA cm−2 1 mAh cm−2 1 M LiPF6 in EC/DMC
(1∶1, v/v)32 mV 400 h [66] ILC-Li 3 mA cm−2 3 mAh cm−2 1 M LiPF6 in EC/EMC
(3∶7, weight/weight) with 2wt% VC15-20 mV 2250 h [69] 3DP-MXene arrays 1 mA cm−2 1 mAh cm−2 1 M LiTFSI in DOL/DME
(1∶1, v/v) with 1wt% LiNO310 mV 1200 h [75] MXene@Au 1 mA cm−2 1 mAh cm−2 1 M LiTFSI in DOL/DME
(1∶1, v/v) with 2wt% LiNO3/ 650 h [81] Zn-MXene 1 mA cm−2 1 mAh cm−2 1 M LiTFSI in DOL/DME
(1∶1, v/v).16 mV 1200 h [82] MXene/ZnO 1 mA cm−2 1 mAh cm−2 2 M LiTFSI in DME
with 1wt% FEC37±6 mV 250 h [84] CNT/MXene/SnO2 40 mA cm−2 1 mAh cm−2 1 M LiPF6 in EC/EMC
(1∶1, v/v) with 15wt% FEC85 mV 500 cycles [93] MXene@CNF 0.5 mA cm−2 1 mAh cm−2 1 M LiTFSI in DOL/DME
(1∶1, v/v) with 1wt% LiNO347 mV 1300 h [94] Ti3C2-LiB-Li 1 mA cm−2 1 mAh cm−2 1 M LiTFSI in DOL/DME
(1∶1, v/v) with 1wt% LiNO3/ 1000 h [96] Ti3C2Tx-rGO 1 mA cm−2 1 mAh cm−2 1M LiPF6 in EC/DMC/EMC
(1∶1:1, v/v/v) with 5.0% FEC36 mV 1400 h [99] 3D MG 5 mA cm−2 1 mAh cm−2 1 M LiTFSI in DOL/DME
(1∶1, v/v) with 1wt% LiNO325 mV 400 h [100] MXene-MF 5 mA cm−2 5 mAh cm−2 1 M LiTFSI in DOL/DME
(1∶1, v/v) with 1wt% LiNO3.13 mV 700 h [101] Note: M: mol L−1 
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