MXene材料用于柔性传感器的研究进展

姜晶; 陈星; 牛夷; 何欣芮; 胡娅林; 王超

doi:10.1016/S1872-5805(22)60589-4

MXene材料用于柔性传感器的研究进展

doi: 10.1016/S1872-5805(22)60589-4

电子科技大学电子科学与工程学院，四川成都 611731

详细信息

作者简介:
^†姜晶、陈星为共同第一作者

通讯作者:
王　超，教授. E-mail：cwang@uestc.edu.cn

中图分类号: TB381
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出版历程
- 收稿日期: 2021-06-25
- 修回日期: 2021-09-07
- 网络出版日期: 2021-12-17
- 刊出日期: 2022-03-30

Advances in flexible sensors with MXene materials

School of Electronic Science and Engineering, University of Electronic Science and Technology of China, Chengdu 611731, China

Funds: National Key Research and Development Program of China (2017YFC0602102), National Natural Science Foundation of China (U20A20213 and 61727818), the Department of Science and Technology of Sichuan Province (2021JDTD0030) and AECC Sichuan Gas Turbine Research Establishment （WDZC-2020-3-2）.

More Information

Corresponding author: WANG Chao, Professor. E-mail: cwang@uestc.edu.cn

摘要

摘要: 随着柔性电子学的快速发展，有望实现具有高灵敏度和宽检测范围的柔性传感器。近年来，二维层状过渡金属碳氮材料MXene由于具有高导电性、高比表面积、优异的亲水性及良好的机械性能等特点，且能够与包括炭材料（碳纳米管、炭纤维、石墨烯等）在内的多种材料形成性能优异的复合材料，在柔性传感器领域受到众多研究者们的关注。本综述首先介绍MXene材料的结构、合成等内容，随后总结MXene柔性传感器的结构、性能指标和常用制备工艺。在此基础上，回顾了多种MXene柔性传感器，详细介绍其传感机制和制备技术。最后，总结MXene材料用于柔性传感器的研究趋势。
- MXene /
- 柔性传感器 /
- 复合材料 /
- 传感性能
Abstract: The rapid development of flexible electronics has made it possible to realize flexible sensors with high sensitivity and a wide detection range. In recent years, the two-dimensional MXene layer materials composed of transition metals, carbon and/or nitrogen have attracted the attention of many researchers in the field of flexible sensors, because of their high conductivity, high specific surface area, outstanding hydrophilicity, excellent mechanical properties and other characteristics. They can be composited with other materials, such as carbon nanotubes, carbon fibers and graphene, to form a variety of materials. Here, the structure and synthesis of MXene materials are introduced, followed by a summary of their preparation methods, structures, performance and sensing mechanisms as flexible sensors. Finally, research trends for flexible sensors using MXene materials are discussed.
- MXene /
- Flexible sensor /
- Composite materials /
- Sensor performance

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FIG. 1397. FIG. 1397.

FIG. 1397.. FIG. 1397.

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图 1 MXene结构及合成示意图

Figure 1. Structure and synthesis of MXene materials.

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图 2 不同MXene的球棒模型^[31]

Figure 2. Ball-and-stick model of different MXene materials^[31]. Reprinted with permission.

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图 3 通过改变外部过渡金属M层元素改变MXene电学性质^[41]：（a）Mo₂TiC₂T_x（红色）、Mo₂Ti₂C₃T_x（蓝色）和Ti₃C₂T_x（黑色）的电阻率随温度的变化，（b）电阻率比较结果，电阻率曲线下面的彩色三角形（红色和黑色）说明了dρ/dT的差异

Figure 3. The electrical properties of MXene changed by changing the external transition metal M layer elements ^[41]: (a) Temperature dependence of resistivity for a Mo₂TiC₂T_x (red), Mo₂Ti₂C₃T_x (blue), and Ti₃C₂T_x (black). (b) Comparison of resistivity. The colored triangles (red and black) below each resistivity curve illustrate the differences in dρ/dT. Reprinted with permission.

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图 4 拉伸载荷期间Ti_n+1C_n样品的应变-应力曲线^[44]

Figure 4. Strain–stress curves of the Ti_n+1C_n samples during tensile loading^[44]. Reprinted with permission.

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图 5 MXene薄膜的机械强度^[47]：（a）不同Ti₃C₂T_x含量的Ti₃C₂T_x/PVA混合薄膜的应力应变曲线，（b）Ti₃C₂T_x薄膜制成的圆柱体支撑起自身重量4000倍的重量，（c）90%含量的Ti₃C₂T_x/PVA混合薄膜制成的圆柱体支撑起自身重量15000倍的重物

Figure 5. Mechanical strength of MXene films ^[47]: (a) Stress–strain curves for Ti₃C₂T_x/PVA films with different Ti₃C₂T_x contents. (b) The cylinder made from Ti₃C₂T_x films can support 4000 times its own weight. (c) The cylinder made from 90% Ti₃C₂T_x/PVA can support 15000 times its own weight. Reprinted with permission.

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图 6 迟滞效应^[67]

Figure 6. Hysteresis effects^[67]. Reprinted with permission.

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图 7 滴涂、浸涂和旋涂的示意图

Figure 7. Process of drop-casting, dip-coating, and spin-coating.

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图 8 夹层状MXene/CNT感应层的制备过程^[74]

Figure 8. Fabrication process of a sandwich-like Ti₃C₂T_x MXene/CNT layer ^[74]. Reprinted with permission.

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图 9 MXene/PANIF柔性传感器用于应变检测^[75]：（a-f） MXene/PANIF应变传感器检测喉部发声、扬声器声波手腕处脉搏、皱眉、手指弯曲及肘部弯曲，（g）无线传输示意图：通过与手机的无线通信实现的遥感性能，（h）在手机上获得的检测10%应变的感测性能

Figure 9. Strain measurement of the MXene/PANIF flexible sensor ^[75]: (a-f) The MXene/PANIF strain sensor detects throat during speaking, sound waves of the loudspeaker, human wrist pulse, frowning, finger bending and elbow bending. (g) The concept of wireless transmission: remote sensing performance by wireless communication to the mobile phone. (h) The sensing performance obtained on the mobile phone for detecting 10% strain. Reprinted with permission.

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图 10 Ti₃C₂T_x/PDMS 柔性传感器用于距离检测和温度检测^[86]：（a）手指与Ti₃C₂T_x膜之间的不同距离使温度传感器的电阻发生变化，（b）温度传感器的可重复性，循环三次接近至0.3 cm，（c）随着装有冰、温水和热水的小瓶的接近，温度传感器的电阻变化，（d）使用不同功率的红外激光持续照射温度传感器得到的电阻变化

Figure 10. Distance and temperature measurement of Ti₃C₂T_x/PDMS flexible sensor ^[86]: (a) Resistance variation of the temperature sensor at different distances between the finger and the Ti₃C₂T_x film. (b) The repeatability of the proximity temperature sensor for 0.3 cm with 3 circles. (c) Resistance variation of the temperature sensor with the approach of vials containing ice, warm and hot water. (d) Resistance variation of the temperature sensor using infrared lasers with different powers. Reprinted with permission.

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图 11 MXene-PDMAEMA薄膜（绿色）和原始MXene薄膜（橙色）以及MXene-PDMAEMA悬浮液的电导率随温度变化曲线^[99]. 蓝色和红色点分别标记了25至40 °C之间的测量温度范围. 测量循环了至少3次，并且每次测量产生的变化的误差相对较小

Figure 11. Conductivity results measured on thin films of hybrid MXene (green) and pristine MXene (orange) as well as a suspension of hybrid MXene (black) ^[99]. Blue and red dots mark the temperature range for the measurement between 25 and 40 °C, respectively. The measurements have been repeated at least three times, and the resulting variations from measurement to measurement (error bars) are relatively small. Reprinted with permission.

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图 12 柔性传感器的汗液监测实验，用于检测pH值、乳酸和葡萄糖浓度^[100]：（a）柔性汗液传感器贴片连接到便携式电化学分析仪，该分析仪可供电并控制柔性传感器，并可以通过蓝牙进行无线通信；（b）柔性汗液传感器贴片连接到皮肤上的便携式电化学分析仪；（c）骑行强度变化曲线；（d）用3种不同的葡萄糖传感器在饭前和饭后测得的葡萄糖传感器的电流响应和pH值变化；（e）pH传感器在运动过程中的不同时间测得的pH值；（f）乳酸传感器在运动过程中的不同时间测得的电流响应；（g）用3种不同的葡萄糖和pH传感器比较饭前和饭后的葡萄糖浓度和pH值；（h）使用3种不同的pH传感器比较运动过程中不同时间的pH值；（i）使用3种不同的乳酸传感器比较运动过程中不同时间的乳酸水平

Figure 12. The sweat monitoring of flexible sensor, to detect pH, lactate and glucose concentrations^[100]: (a) The flexible sweat-monitoring patch is connected to a portable electrochemical analyzer that supplies power and controls the patch and can wirelessly communicate with commercial mobile phones via Bluetooth. (b) The flexible sweat-monitoring patch is connected to a portable electrochemical analyzer on the skin. (c) Cycling resistance profile for on-body tests. (d) Measured chronoamperometric responses of glucose sensors and pH changes before and after meals with 3 different glucose sensors. (e) Measured pH level of pH sensor at different times during the exercise. (f) Measured chronoamperometric responses of lactate sensor at different times during the exercise. (g) Comparison of glucose and pH levels before and after meals with 3 different glucose and pH sensors. (h) Comparison of pH levels at different times during the exercise with 3 different pH sensors. (i) Comparison of lactate levels at different times during the exercise with lactate sensors. Reprinted with permission.

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图 13 V₂CT_x传感器在室温（23 ℃）下的气敏特性^[108]：（a）传感器暴露于不同气体中的电阻变化，（b）传感器对100 ×10⁻⁶的氢气、乙醇、丙酮、甲烷、氨气和硫化氢的气体响应，（c-f）V₂CT_x气体传感器在不同浓度下的氢气、丙酮、甲烷和硫化氢的气体响应

Figure 13. Gas sensing properties of a V₂CT_x sensor at RT (23 ℃) ^[108]: (a) The resistance variation of the sensor when exposed to different gases. (b) Gas response toward 100 ppm of hydrogen, ethanol, acetone, methane, ammonia, and hydrogen sulfide. (c-f) Sensing response of V₂CT_x gas sensors at varying concentrations of hydrogen, acetone, methane and hydrogen sulfide. Reprinted with permission.

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图 14 MXene/GO杂化纤维合成及实物展示^[109]：（a）MXene/GO杂化纤维的合成示意图，（b）MXene/GO凝胶状纤维从喷头到凝固浴的状态，（c）超过1.2米长的MXene/GO杂化纤维绕成的线轴，（d）MXene/GO杂化纤维（40%MXene）的柔韧性

Figure 14. The synthesis and photograph of MXene/GO hybrid fiber ^[109]: (a) Schematic illustration of the spinning process for MXene/GO hybrid fibers. (b) Photograph of MXene/GO gel fiber states from the nozzle to the bath. (c) A bobbin of wound MXene/GO hybrid fibers over 1.2 m long. (d) The flexibility and bendability of MXene/GO fiber (40% MXene). Reprinted with permission.

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表 1 一些已报道的柔性应变传感器:材料、制备方法和性能

Table 1. Some of the reported flexible strain sensors: materials, production methods and performances.

Materials	Substrates	Production methods	Detection range(%)	Sensitive(GF)	Ref.
MXene/SWCNT	PI	Layer-by-layer spray	30~130	64.6~772.6	[74]
MXene/PANIF	Elastic rubber	Layer-by-layer spray	0~80	97.6~2369.1	[75]
SWCNT	PDMS	CVD	0~280	0.06~0.82	[76]
Graphene	Stretchable latex	CVD	0~70	0.76~2.55	[77]
Graphene	PDMS	CVD	0~30	35~10⁶	[78]
rGO	Elastic tape	Layer-by-layer adhere	0~82	16.2~150	[79]
CB/CMC	Paper	Dip-coating	0~0.6	4.3	[80]
AgNPs	XSBR	Mix to form film	0~100	0.0025~0.01	[81]
VN/CNT	\	In situ catalytic aerogel	0~10	135~386	[82]
ZnO Nanowire/Polystyrene	PDMS	Electrospinning	0~50	116	[83]

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表 2 一些已报道的柔性温度传感器:材料、制备方法和性能

Table 2. Some of the reported flexible temperature sensors: materials, production methods and performances.

Materials	Substrates	Production methods	Detection range(°C)	Sensitivity(%/°C)	Ref.
MXene	PDMS	Vacuum filtration	20~140	98600	[86]
MXene/graphene	PI	Ink jet printing	50~100	53.6 μV·°C⁻¹	[87]
PEDOT:PSS	PDMS	Drop-casting	30~55	4.2	[88]
Graphene nanowalls	PDMS	CVD	25~120	0.214	[89]
Graphene/P(VDF-TrFE)	\	Drop-casting	−20~300	2.5	[90]
CNT	PET	Screen printing/gravure printing	−40~100	−0.4	[91]
Nickel -CNT	Flax fabric	Dip-coating/electroless deposition	25~45	−2.96	[92]
FG/CNT/PDMS	PET	Screen printing	40~80	2.8	[93]
rGO	Parylene	Spray-coating	22~70	0.83%·K⁻¹	[94]
AgNPs	Paper	Ink jet printing	−20~60	0.11	[95]
AgNW	PI	spray-coating	25~60	0.332	[96]
NiO nanoparticles	PET	Drop-casting/laser-induced reductive sintering	25~70	−9.2	[97]

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表 3 一些已报道的柔性生物传感器:材料、制备方法和性能

Table 3. Some of the reported flexible biosensors: materials, production methods and performances.

Materials	Substrates	Production methods	Target substance	Sensitivity	Ref.
Enzyme/MXene/CNT/PB	CFM	Mix to vacuum filtration	Glucose/lactic acid/pH value	35.3 μA·mM⁻¹·cm⁻²(Glucose) 11.4 μA·mM⁻¹·cm⁻²(Lactic acid) −70 mV·pH⁻¹(pH value)	[100]
Enzyme/GO	PA	Vacuum assisted diffusion/ evaporation deposition	Lactic acid	71.3%(1~100 mM)	[101]
Enzyme/Pt-graphite/chitosan	PU	Screen printing	Glucose	105 μA·mM⁻¹·cm⁻²	[102]
Enzyme/SPP-PEDOT:PSS	PDMS	Spin-coating/ photolithography	Dopamine/ ascorbic acid/ glucose	113 nA·μM⁻¹·cm⁻²(Dopamine) 25 nA·μM⁻¹·cm⁻²(Ascorbic acid) 5.06 μA·mM⁻¹·cm⁻²(Glucose)	[103]
Antibody/PEDOT:PSS	Fibroin	Spin-coating/photolithography	Vascular endothelial growth factor	11.84%±4.44%(0.1~1 ng·ml⁻¹)	[104]
MoS₂	Al foil	Hydrothermal method	Uric Acid	98.1±1 μA·μM⁻¹	[105]
PtCo alloy nanoparticles/ nanoporous gold	Graphene paper	Electrodeposition	Glucose	7.84 μA·mM⁻¹·cm⁻²	[106]
Note: M—mol L⁻¹

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表 4 一些已报道的柔性气体传感器:材料、制备方法和性能

Table 4. Some of the reported flexible gas sensors: materials, production methods and performances.

Materials	Substrates	Production methods	Target gas	Detection range (×10⁻⁶)	Sensitivity	Ref.
MXene	PI	Drop-casting	H₂	2~100	0.2435(100×10⁻⁶, 23 °C)	[108]
MXene/rGO	\	Wet spinning	NH₃	10~50	0.0677(50×10⁻⁶,23 °C)	[109]
CNT	Paper	Ink jet printing	NO₂/Cl₂	10~100	0.35(10×10⁻⁶, NO₂) 0.16(10×10⁻⁶, Cl₂)	[110]
Graphene	PET	CVD	NO₂	\	0.2276(200×10⁻⁶, 23 °C)	[111]
MoS₂/Graphene	\	Wet spinning/ hydrothermal method	NO₂/NH₃	2~1000	\	[112]
Graphene/PEDOT:PSS	Flexible transparent film	Ink jet printing	NH₃	25~1000	0.096(500×10⁻⁶, 23 °C)	[113]
PANI	PET	In situ polymerization	NH₃	5~1000	0.3(200×10⁻⁶, 23 °C)	[114]
PANI/FWMCNT	PET	In situ polymerization/ deposition	NH₃	1~100	0.24(100×10⁻⁶, 23 °C)	[115]
Flower-like palladium nanoclusters/graphene	PEN	Electrodeposition	H₂	0.1~100	0.05(10×10⁻⁶, 23 °C)	[116]
SnO	PI	Ink jet printing	CO/CO₂	1~50(CO) 0.6~20(CO₂)	1.8(20×10⁻⁶, 300 °C) 35(20×10⁻⁶, 300 °C)	[117]
ZnO	PI	Themolysis assisted solution method	Ethanol	10~100	3.11(100×10⁻⁶, 300 °C)	[118]

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