MXene量子点(Ti3C2): 性质、合成及其在能源领域的应用

doi:10.1016/S1872-2067(22)64102-0

催化学报 ›› 2022, Vol. 43 ›› Issue (10): 2484-2499.DOI: 10.1016/S1872-2067(22)64102-0

MXene量子点(Ti₃C₂): 性质、合成及其在能源领域的应用

关晨^a^,^b, 岳晓阳^a^,^b, 范佳杰^c, 向全军^a^,^b^,^*()

^a电子科技大学长三角研究院(湖州), 浙江湖州 313001
^b电子科技大学电子科学与工程学院, 电子薄膜与集成器件国家重点实验室, 四川成都 610054
^c郑州大学材料科学与工程学院, 河南郑州 450002

收稿日期:2022-02-28 接受日期:2022-04-04 出版日期:2022-10-18 发布日期:2022-09-30
通讯作者: 向全军
基金资助:
国家自然科学基金(51672099);国家自然科学基金(52073263);四川科技项目(2021JDTD0026);中央高校基础研究基金(2017-QR-25)

MXene quantum dots of Ti₃C₂: Properties, synthesis, and energy-related applications

Chen Guan^a^,^b, Xiaoyang Yue^a^,^b, Jiajie Fan^c, Quanjun Xiang^a^,^b^,^*()

^aYangtze Delta Region Institute (Huzhou), University of Electronic Science and Technology of China, Huzhou 313001, Zhejiang, China
^bState Key Laboratory of Electronic Thin Film and Integrated Devices, School of Electronic Science and Engineering, University of Electronic Science and Technology of China, Chengdu 610054, Sichuan, China
^cSchool of Materials Science and Engineering, Zhengzhou University, Zhengzhou 450002, Henan, China

Received:2022-02-28 Accepted:2022-04-04 Online:2022-10-18 Published:2022-09-30
Contact: Quanjun Xiang
Supported by:
National Natural Science Foundation of China(51672099);National Natural Science Foundation of China(52073263);Sichuan Science and Technology Program(2021JDTD0026);Fundamental Research Funds for the Central Universities(2017-QR-25)

摘要/Abstract

摘要：

随着化石燃料的日益枯竭, 能源危机成为社会可持续发展所面临的主要难题和巨大挑战. 因此, 开发一种能够实现高能量转换、具备高储存效率的先进材料显得尤为迫切. MXene量子点, 一种由二维过渡金属(MXene)衍生而来的新兴材料, 因具有丰富的活性边缘原子、较好的导电性和出色的光学特性而成为能源储存与转换领域的研究热点. 一般而言, 当MXene的横向尺寸小于10 nm时, 将这种半导体纳米结构命名为MXene量子点. MXene量子点具有诸多优异的性质, 其不仅保留有二维MXene的固有特性, 同时强大的尺寸效应和量子限制效应还赋予了其更多独特的性能, 例如更强的光吸收能力、更好的导电性及生物相容性等, 从而使得MXene量子点在光催化、检测、储能、生物医学等领域表现出巨大应用潜力.

本文综述了有关MXene量子点在能源相关领域应用的最新研究进展, 包括: (1) MXene量子点在结构、电学和光学方面的基本特性; (2) MXene量子点的制备方法, 如水热/溶剂热法、熔融盐法、声微流体法、直接超声法等, 并给出了各方法的机理、制备步骤(包括具体参数)及优缺点; (3) MXene量子点与二维MXene在不同方面的比较：包括官能团、光吸收能力、能带结构、稳定性以及辅助增强光催化机理等. 重点介绍了MXene量子点在能源储存与转换领域中的应用, 包括光催化(光催化分解水产氢、光催化CO₂还原、光催化固氮)、电池和超级电容器, 同时深入探究了MXene量子点在这些应用中发挥的关键作用. 分析了MXene量子点基材料在能源储存与转换领域面临的问题和挑战, 并对未来发展趋势进行了展望, 主要观点包括: (1)目前, MXene量子点的制备主要通过传统的化学法制备, 即用强腐蚀性的酸性溶液(氢氟酸或氢氟酸替代物)刻蚀, 而关于新型物理法或者无氟制备方法的研究较少, 需要进一步拓展; (2) MXene量子点的磁性、化学发光以及透明光学特性等基本性质仍处于理论预测阶段, 需采用更先进仪器设备及实验对其进行更深入的研究; (3)引入新的改性策略如核壳结构、等离子体共振效应, 单原子催化、缺陷调控等来提高MXene量子点基光催化剂的催化性能, 是未来MXene量子点基复合催化剂的发展方向.

关键词: MXene量子点, 能量储存与转换, 合成方法, 光催化, 基本性质

Abstract:

The emerging two-dimensional MXene-derived quantum dots (MQDs) have garnered considerable research interest owing to their abundant active edge atoms, excellent electrical conductivity, and remarkable optical properties. Compared with their two-dimensional (2D) counterpart MXene, MQDs with forceful size and quantum confinement effects exhibit more unparalleled properties and have considerably contributed to the advanced photocatalysis, detection, energy storage, and biomedicine fields. This critical review summarizes the fundamental properties of MQDs in terms of structure, electricity, and optics. The mechanism, characteristics, and comparisons of two typical synthesis strategies (traditional chemical method and novel fluorine-free or chemical-free method) are also presented. Furthermore, the similarities and differences between MQDs and 2D MXenes are introduced in terms of their functional groups, light absorption capacity, energy band structure, and other properties. Moreover, recent advances in the applications of MQD-based materials for energy conversion and storage (ECS) are discussed, including photocatalysis, batteries, and supercapacitors. Finally, current challenges and future opportunities for advancing MQD-based materials in the promising ECS field are presented.

Key words: MXene quantum dots, Energy conversion and storage, Synthesis method, Photocatalysis, Fundamental property

关晨, 岳晓阳, 范佳杰, 向全军. MXene量子点(Ti₃C₂): 性质、合成及其在能源领域的应用[J]. 催化学报, 2022, 43(10): 2484-2499.

Chen Guan, Xiaoyang Yue, Jiajie Fan, Quanjun Xiang. MXene quantum dots of Ti₃C₂: Properties, synthesis, and energy-related applications[J]. Chinese Journal of Catalysis, 2022, 43(10): 2484-2499.

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图/表 20

Fig. 1. Panoramic review of properties, synthesis, comparison, and energy-related applications of MXene quantum dots.

Fig. 2. Preparation mechanism and application of MXene quantum dots. Oxygen-containing functional groups are formed on 2D MXenes, possibly generating defects and allowing the 2D MXene to be cut into quantum dots.

Fig. 3. Schematic of the energy-level structure and carrier transfer processes of MQDs and N-MQDs. Nitrogen doping-introduced trap states close to the LUMO, achieving rapid electron migration and increasing the carrier lifetime.

Fig. 4. Charge density difference between the pure MXene QDs and heteroatom-functionalized MXene QDs. (a) Pure Ti3C2 MXene QDs. (b) N-functionalized Ti3C2 MXene. (c) P-functionalized Ti3C2 MXene QDs. (d) N-P-functionalized MQDs. Red and blue isosurfaces represent electron accumulation and depletion during the chemical bond formation process, respectively. In (b-d), the enhanced blue color indicates electron depletion, demonstrating that impurity atoms cause charge transfer and increase the PLQYs of the N-P-functionalized MQDs. Reprinted with permission from Ref. [49]. Copyright 2019, Royal Society of Chemistry.

Table 1 Methods for preparing MQDs and differences between different routes.

Synthesis method	Applicable MXene (published)	Advantage	Disadvantage
Hydrothermal method	Ti₃C₂ MQDs	concise operation, large-scale production	oxidation, HF, high temperature
Solvothermal method	Ti₃C₂T_x QDs	better morphology control	oxidation, HF, high temperature
Hydrothermal/solvothermal- ultrasound method	Ti₃C₂ MQDs	accelerate the fragmentation of MXene into MQDs, suppress MXene oxidation	time-consuming, cumbersome process
Molten salt synthesis	Mo₂C MQDs	high atom usage, precise morphology control	high temperature, low production yield
Acoustomicrofluidic method	Ti₃C₂T_z QDs	chemical-free method, preserve the structural integrity of the material	—
Direct ultrasound method	Ti₃C₂ MQDs	safe, simple, fluorine-free method	time-consuming

Fig. 5. Comparison of three MQD synthesis methods. (a) Hydrothermal and solvothermal synthesis processes. (b) Hydrothermal/solvother- mal-ultrasound synthesis process. (c) Molten salt synthesis process.

Fig. 6. (a) XRD patterns of the initial Mo2C/C sample without centrifugal treatment and the final Mo2C/C sample with centrifugal treatment. STEM (b) and EDS (d,e) images of Mo2C/C nanosheets. (c) HRTEM image of Mo2C QD/C nanosheets. (f) Nitrogen adsorption energy of Mo2C and C. (g) Atomic structure scheme showing the reaction pathway of N2 reduction on Mo2C sites. Green, gray, blue, and white balls represent Mo, C, N, and H atoms, respectively. Reprinted with permission from Ref. [65]. Copyright 2018, Wiley-VCH.

Fig. 7. (a) Schematic of the experimental setup: the multilayer Ti3C2Tz MXene sample is atomized on the SRBW device with the formation of layered and cracked Ti3C2Tz aerosol droplets. (b) Condensate (MXene nanosheets and MQDs) collected under different cycles (evolution along with increasing cycles). (c) Atomic force microscopic (AFM) images (including sample thickness profiles) and the corresponding thickness and mean lateral-diameter measurement distributions of the acoustically synthesized MXene nanosheets and MQDs after 10 nebulization cycles. Reprinted with permission from Ref. [67]. Copyright 2021, American Chemical Society.

Fig. 8. TEM (a) and HRTEM (b) images of Ti3C2 QD/Cu2O NW/Cu heterostructure. UV-vis diffuse reflectance spectra (c) and yields of methanol as a function of time (d). Reprinted with permission from Ref. [13]. Copyright 2018, Wiley-VCH.

Fig. 9. Energy-level diagram of MQDs and MXenes and schematic of redox potential energy for various products via photocatalysis (vs. NHE, pH = 7).

Table 2 Comparisons of MQDs and MXenes.

Synthesis method	Crystal structure	Functional group	Fermi level (V)	Optical absorption ability
MQD	Hexagonal symmetry	-O, -F, -OH, etc.	-0.523	Red shift
MXene	Hexagonal symmetry	-O, -F, -OH, etc.	0.71	Blue shift

Fig. 10. (a) Scanning Kelvin probe maps of BiVO4, Ti3C2 QD/BiVO4 (TC QD/BV), BiVO4@ZnIn2S4(BV@ZIS), and BiVO4@ZnIn2S4/Ti3C2 QDs (BV@ZIS/TC QDs). (b) Steady-state PL spectra. (c) Schematic of the band structure and electron-hole transfer mechanism for BV@ZIS/TC QDs. Reprinted with permission from Ref. [73]. Copyright 2021, Elsevier.

Fig. 11. (a) Simulated electron density distribution at the interface between Ti3C2Tx and ZnIn2S4 nanosheets. (Ti blue, C brown, O red, Bi purple, Mo silver, and S yellow balls. Yellow and blue areas in (a) represent higher and lower electron densities, respectively). (b) Energy band diagram of Ti3C2Tx and ZnIn2S4. Reprinted with permission from Ref. [74]. Copyright 2020, Wiley-VCH.

Table 3 Summary of applications of various MQD-based photocatalysts.

MQD-based material	Type of MQDs	Composite structure	Application	Performance	Ref.
Cu₂O NW/Ti₃C₂	Ti₃C₂	one dimension (1D)/ zero dimension (0D)	CO₂ reduction	CH₃OH (78.50 μmol g^-1 h^-1);	[13]
TiO₂/C₃N₄/Ti₃C₂	Ti₃C₂	2D/2D/0D	CO₂ reduction	CO (4.39 μmol g^-1 h^-1); CH₄ (1.20 μmol g^-1 h^-1)	[135]
g-C₃N₄/Ti₃C₂	Ti₃C₂	2D/0D	H₂ evolution	H₂ (5111.8 μmol g^-1 h^-1)	[14]
CdS/Ti₃C₂	Ti₃C₂	0D/0D	H₂ evolution	H₂ (14342 μmol g^-1 h^-1)	[136]
Ti₃C₂/Ni MOF	Ti₃C₂	0D/2D	N₂ photoreduction	NH₃ (88.79 μmol g_cat^-1 h^-1)	[15]
Ti₃C₂/ZnIn₂S₄/BiVO₄	Ti₃C₂	0D/2D/three dimension (3D)	photocatalytic overall water splitting	O₂ (50.83 μmol g^-1 h^-1), H₂(102.67 μmol g^-1 h^-1)	[75]
Ti₃C₂/SiC	Ti₃C₂	0D/2D	photocatalytic NO pollutant removal	NO pollutant removal efficiency 74.6%	[49]
Ti₃C₂T_x/Ti₃C₂T_x/S	Ti₃C₂T_x	0D/2D	lithium-sulfur batteries	when sulfur loading is 13.8 mg cm^-2, volumetric capacity is 1957 mA h cm^-3 and areal capacity is 13.7 mA h cm^-2	[16]
Ti₃C₂T_x/Ti₃C₂T_x/RGO	Ti₃C₂T_x		supercapacitors	volumetric capacity (542 F cm^-3)	[17]
Ti₃C₂	Ti₃C₂	0D	multicolor cellular imaging		[29]
N-Ti₃C₂	Ti₃C₂	0D	Fe³⁺ detection	detectable concentration (2-500 μmol L^-1), limit of detection (2 μmol L^-1)	[137]
Ti₃C₂	Ti₃C₂	0D	immunomodulation	—	[138]
V₂C	V₂C	0D	nucleus-target low-temperature photothermal therapy	—	[139]
MoS₂ QD@Ti₃C₂T_x QD@MWCNTs	Ti₃C₂T_x		electrocatalytic methanol oxidation	maximum methanol oxidation current density at 2.2 V of 160 A g^-1	[140]
Co-Ti₃C₂	Ti₃C₂	0D	photoelectrochemical water oxidation	water oxidation performance (2.99 mA cm^-2 at 1.23 V vs. RHE)	[141]

Fig. 12. Mechanism diagram of the photocatalytic hydrogen production of Ti3C2 QD/g-C3N4 NSs.

Fig. 13. (a) Energy band positions of Ti3C2 QD/Ni MOF. (b) Scheme of the spatial charge separation and transportation during photocatalytic N2 reduction using Ti3C2 QD/Ni MOF. (c) HRTEM images of Ti3C2 QD/Ni MOF nanosheets. (d) Change in the N-N bond length and free energy against the reaction coordinate during the reaction process. Reprinted with permission from Ref. [15]. Copyright 2020, American Chemical Society.

Fig. 14. Synthetic mechanism of Ti3C2Tx QD-Ti3C2Tx sheets (TCD-TCS) and TCD-TCS/S.

Fig. 15. Schematic of the evolution of active materials during the discharge process for TC-100/S cathodes. Process 1: more active material accumulation on TCS is beneficial for penetrating electrolytes and transferring electrons and ions in TCD-TCS. Process 2: as lithiation progresses, the outstanding LiPS capture ability of TCD-TCS effectively inhibits the occurrence of the LiPS shuttle effect.

Fig. 16. (a) Preparation schematic of all-solid-state asymmetric fiber supercapacitors. (b) SEM image of the fiber electrode. (c) Galvanostatic charge-discharge curves at 0.25 A cm-3. (d) Specific capacitance at different current densities. Reprinted with permission from Ref. [17]. Copyright 2020, American Chemical Society.

Fig. 17. (a) Schematic of the synthesis of Ti3C2 QDs using a hydrothermal method for bioimaging. (b,c) HRTEM and AFM images of Ti3C2 QDs. (d) Bioimaging image of RAW264.7 cells after Ti3C2 QD uptake. Reprinted with permission from Ref. [29]. Copyright 2017, Wiley-VCH.

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MXene量子点(Ti₃C₂): 性质、合成及其在能源领域的应用

MXene quantum dots of Ti₃C₂: Properties, synthesis, and energy-related applications

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