基于激光诱导石墨烯复合材料的柔性传感器研究

在可穿戴设备领域，对应变、气体压力和气体成分等参数的监测至关重要。传统的传感器和材料通常具有刚性、体极大、便携性差等缺点，限制了它们在可穿戴领域的应用。目前，柔性传感器具有可拉伸、重量轻、便携的特点，在可穿戴设备和人机交互等领域得到广泛研究。然而，柔性传感器还存在以下问题，譬如在应变传感中仍存在较宽线性拉伸范围和高灵敏度难以兼得的问题，在气体传感中实现室温高灵敏度检测仍具有挑战，在柔性气体压力传感器中存在器件结构和测试系统复杂等问题。

本论文针对上述问题，通过理论预测与实验测试相结合的方法，深入研究了基于激光诱导石墨烯（LIG）复合材料的传感原理，并对传感器件结构和传感材料进行了优化，旨在解决传感器性能差的问题。本文的主要研究内容如下：

（1）在柔性气体压力传感器的研究中，构建了三维表面应变监测方法，对其气体压力传感性能进行表征，加速传感器设计的迭代效率。采用渗透法制备的聚二甲基硅氧烷/LIG复合薄膜成功组装了柔性气体压力传感器，性能测试结果表明，通过设计不同的激光参数和传感区域图案，可以有效调控传感器的灵敏度和检测范围。传感器的三维表面应变检测范围最宽可达40%，应变灵敏因子（GF）最大可达211.3。传感性能调控的主要机制在于调控裂纹导电网络的路径和密度。该研究有助于根据实际应用需求定制传感器的性能，为传感器的个性化设计提供了新的途径。该传感器可应用于微流控芯片内部气体压力监测，表明其在健康和医疗领域的潜在应用价值。

（2）在柔性应变传感器的研究中，采用密度泛函理论研究方法，研究了新型材料二硒化铪（HfSe2）和二硫化铪的应变效应，得出HfSe2对应变具有高灵敏响应。随后，采用原位激光法制备了HfSe2/LIG复合材料，并将其转移到具有高拉伸性能的Ecoflex柔性基底表面，构建了可拉伸应变传感器。HfSe2的复合使得GF提升了3倍以上，最低可测0.02%的应变，并且在0 ~ 30%应变范围内能够同时获得较高的灵敏度（GF = 46）和良好的线性度（R2 = 0.99），在人体运动监测和生理信号监测方面展示了潜在应用价值。

（3）在柔性气体传感器的研究中，通过在LIG表面复合HfSe2来提升其气体传感性能。采用密度泛函理论对本征HfSe2表面吸附氨气和臭氧分子的吸附能、转移电荷和电学性能，以及掺杂对吸附特性的影响进行了研究，结果表明HfSe2对氨气的吸附强度可以通过掺杂氧和硫原子来进行提高。其中，氧掺杂的二硒化铪（O-HfSe2）对氨气的吸附强度最大。基于理论研究结果，实验制得的O-HfSe2传感器对氨气的响应度较本征HfSe2提升了约12%。此外，成功制备了LIG柔性气体传感器和HfSe2/LIG气体传感器，检测氨气的浓度为100 ppm时，HfSe2/LIG气体传感器的响应度为86%，较单独LIG提升了约14%。

本论文最终构建了基于激光诱导石墨烯复合材料的柔性气体压力、应变和气体传感器，并深入研究了其传感性能，实现了对气体压力传感器性能的调控、对应变传感器线性拉伸范围和灵敏度的提升、对氨气的室温检测。该研究为高性能柔性传感器的研究和设计提供了新的策略和理论支撑，所制备的器件在健康监测等领域有着广阔的应用前景。

[1] Yang J C, Mun J, Kwon S Y, et al. Electronic skin: recent progress and futureprospects for skin-attachable devices for health monitoring, robotics, andprosthetics[J]. Advanced Materials, 2019, 31(48): 1904765.
[2] Wang L, Jiang K, Shen G. Wearable, implantable, and interventional medicaldevices based on smart electronic skins[J]. Advanced Materials Technologies,2021, 6(6): 2100107
[3] Kim H, Kwon Y T, Lim H R, et al. Recent advances in wearable sensors andintegrated functional devices for virtual and augmented reality applications[J].Advanced Functional Materials, 2020, 31(39): 2005692
[4] Pyo S, Lee J, Bae K, et al. Recent progress in flexible tactile sensors for humaninteractive systems: from sensors to advanced applications[J]. AdvancedMaterials, 2021, 33(47): 2005902
[5] Zhang S, Chhetry A, Zahed M A, et al. On-skin ultrathin and stretchablemultifunctional sensor for smart healthcare wearables[J]. npj Flexible Electronics,2022, 6(1): 1-12.
[6] Zhang H, He R, Niu Y, et al. Graphene-enabled wearable sensors for healthcaremonitoring[J]. Biosensors and Bioelectronics, 2022, 197: 113777.
[7] Shen Z, Liu F, Huang S, et al. Progress of flexible strain sensors for physiologicalsignal monitoring[J]. Biosensors and Bioelectronics, 2022, 211: 114298.
[8] Park C, Kim M S, Kim H H, et al. Stretchable conductive nanocomposites andtheir applications in wearable devices[J]. Applied Physics Reviews, 2022, 9(2):021312.
[9] Li S, Xiao X, Hu J, et al. Recent advances of carbon-based flexible strain sensorsin physiological signal monitoring[J]. ACS Applied Electronic Materials, 2020,2(8): 2282-2300.
[10] Amjadi M, Kyung K-U, Park I, et al. Stretchable, skin-mountable, and wearablestrain sensors and their potential applications: a review[J]. Advanced FunctionalMaterials, 2016, 26(11): 1678-1698.
[11] Liu H, Gao H, Hu G. Highly sensitive natural rubber/pristine graphene strainsensor prepared by a simple method[J]. Composites Part B: Engineering, 2019,171: 138-145.
[12] Luo Z, Li X, Li Q, et al. In situ dynamic manipulation of graphene strain sensorwith drastically sensing performance enhancement[J]. Advanced ElectronicMaterials, 2020, 6(6): 2000269.
[13] Chao M, Wang Y, Ma D, et al. Wearable MXene nanocomposites-based strainsensor with tile-like stacked hierarchical microstructure for broad-rangeultrasensitive sensing[J]. Nano Energy, 2020, 78: 105187.
[14] Chu Z, Jiao W, Huang Y, et al. Superhydrophobic gradient wrinkle strain sensorwith ultra-high sensitivity and broad strain range for motion monitoring[J].Journal of Materials Chemistry A, 2021, 9(15): 9634-9643.
[15] Amjadi M, Turan M, Clementson C P, et al. Parallel microcracks-basedultrasensitive and highly stretchable strain sensors[J]. ACS Applied Materials &Interfaces, 2016, 8(8): 5618-5626.
[16] Souri H, Bhattacharyya D. Highly sensitive, stretchable and wearable strainsensors using fragmented conductive cotton fabric[J]. Journal of MaterialsChemistry C, 2018, 6(39): 10524-10531.
[17] Zheng Q, Lee J, Shen X, et al. Graphene-based wearable piezoresistive physicalsensors[J]. Materials Today, 2020, 36: 158-179.
[18] Zhao J, Zhang G, Shi D. Review of graphene-based strain sensors[J]. ChinesePhysics B, 2013, 22(5): 057701.
[19] Ji J, Zhang C, Yang S, et al. High sensitivity and a wide sensing range flexiblestrain sensor based on the V-groove/wrinkles hierarchical array[J]. ACS AppliedMaterials & Interfaces, 2022, 14(20): 24059-24066.
[20] Amjadi M, Pichitpajongkit A, Lee S, et al. Highly stretchable and sensitive strainsensor based on silver nanowire-elastomer nanocomposite[J]. ACS Nano, 2014,8(5): 5154-5163.
[21] Xu S, Rezvanian O, Peters K, et al. The viability and limitations of percolationtheory in modeling the electrical behavior of carbon nanotube-polymercomposites[J]. Nanotechnology, 2013, 24(15): 155706.
[22] Lou Z, Wang L, Shen G. Recent advances in smart wearable sensing systems[J].Advanced Materials Technologies, 2018, 3(12): 1800444.
[23] Seyedin S, Zhang P, Naebe M, et al. Textile strain sensors: a review of thefabrication technologies, performance evaluation and applications[J]. MaterialsHorizons, 2018, 6(2): 219-249.
[24] Lu Y, Biswas M C, Guo Z, et al. Recent developments in bio-monitoring viaadvanced polymer nanocomposite-based wearable strain sensors[J]. Biosensorsand Bioelectronics, 2019, 123: 167-177.
[25] Chen J W, Yu Q L, Cui X H, et al. An overview of stretchable strain sensors fromconductive polymer nanocomposites[J]. Journal of Materials Chemistry C, 2019,7(38): 11710-11730.
[26] Liu C, Han S, Xu H, et al. Multifunctional highly sensitive multiscale stretchablestrain sensor based on a graphene/glycerol-KCl synergistic conductive network[J].ACS Applied Materials & Interfaces, 2018, 10(37): 31716-31724.
[27] He Y, Wu D, Zhou M, et al. Wearable strain sensors based on a porouspolydimethylsiloxane hybrid with carbon nanotubes and graphene[J]. ACSApplied Materials & Interfaces, 2021, 13(13): 15572-15583.
[28] Zhou J, Xu X, Xin Y, et al. Coaxial thermoplastic elastomer-wrapped carbonnanotube fibers for deformable and wearable strain sensors[J]. AdvancedFunctional Materials, 2018, 28(16): 1705591.
[29] Liang B, Lin Z, Chen W, et al. Ultra-stretchable and highly sensitive strain sensorbased on gradient structure carbon nanotubes[J]. Nanoscale, 2018, 10(28): 13599-13606.
[30] Wang Y, Hao J, Huang Z, et al. Flexible electrically resistive-type strain sensorsbased on reduced graphene oxide-decorated electrospun polymer fibrous mats forhuman motion monitoring[J]. Carbon, 2018, 126: 360-371.

[31] Qiao Y, Wang Y, Tian H, et al. Multilayer graphene epidermal electronic skin[J].ACS Nano, 2018, 12(9): 8839-8846.

[32] Chen Y, Liu S, Hong G, et al. Nano-optomechanical resonators for sensitivepressure sensing[J]. ACS Applied Materials & Interfaces, 2022, 14(34): 39211-39219

[33] Mohammad Haniff M A, Muhammad Hafiz S, Wahid K A, et al. Piezoresistiveeffects in controllable defective HFTCVD graphene-based flexible pressuresensor[J]. Scientific Reports, 2015, 5: 14751.

[34] Hassan J Z, Raza A, Din Babar Z U, et al. 2D material-based sensing devices: anupdate[J]. Journal of Materials Chemistry A, 2023, 11(12): 6016-6063.

[35] Li Z, Li H, Wu Z, et al. Advances in designs and mechanisms of semiconductingmetal oxide nanostructures for high-precision gas sensors operated at roomtemperature[J]. Materials Horizons, 2018, 6(3): 470-506.

[36] Kim H-J, Lee J-H. Highly sensitive and selective gas sensors using p-type oxidesemiconductors: Overview[J]. Sensors and Actuators B: Chemical, 2014, 192:607-627.

[37] Cho B, Hahm M G, Choi M, et al. Charge-transfer-based gas sensing usingatomic-layer MoS2[J]. Scientific Reports, 2015, 5: 8052.

[38] Rajapakse M, Anderson G, Zhang C, et al. Gas adsorption and light interactionmechanism in phosphorene-based field-effect transistors[J]. Physical ChemistryChemical Physics, 2020, 22(10): 5949-5958.

[39] Mathew M, Rout C S. Schottky diodes based on 2D materials for environmentalgas monitoring: a review on emerging trends, recent developments and futureperspectives[J]. Journal of Materials Chemistry C, 2021, 9(2): 395-416.

[40] Han Y, Huang D, Ma Y, et al. Design of hetero-nanostructures on MoS2 nanosheets to boost NO2 room-temperature sensing[J]. ACS Applied Materials &Interfaces, 2018, 10(26): 22640-22649.

[41] Yue Q, Shao Z, Chang S, et al. Adsorption of gas molecules on monolayer MoS2and effect of applied electric field[J]. Nanoscale Research Letters, 2013, 8(1):425.

[42] Shokri A, Salami N. Gas sensor based on MoS2 monolayer[J]. Sensors andActuators B: Chemical, 2016, 236: 378-385.

[43] Aftab S, Zahir Iqbal M, Hussain S, et al. New developments in gas sensing usingvarious two-dimensional architectural designs[J]. Chemical Engineering Journal,2023, 469: 144039.

[44] Jiang D, Liu Z, Xiao Z, et al. Flexible electronics based on 2D transition metal dichalcogenides[J]. Journal of Materials Chemistry A, 2022, 10(1): 89-121.

[45] Zhu M, Du X, Liu S, et al. A review of strain sensors based on two-dimensionalmolybdenum disulfide[J]. Journal of Materials Chemistry C, 2021, 9(29): 9083-9101.

[46] Zheng L, Wang X, Jiang H, et al. Recent progress of flexible electronics by 2Dtransition metal dichalcogenides[J]. Nano Research, 2021, 15(3): 2413-2432.

[47] Pi L, Li L, Liu K, et al. Recent progress on 2D noble-transition-metalsichalcogenides[J]. Advanced Functional Materials, 2019, 29(51): 1904932.

[48] Cai Y, Shen J, Ge G, et al. Stretchable Ti3C2Tx MXene/carbon nanotube composite based strain sensor with ultrahigh sensitivity and tunable sensing range[J].ACS Nano, 2018, 12(1): 56-62.

[49] Novoselov K S, Geim A K, Morozov S V, et al. Electric field effect in atomicallythin carbon films[J]. Science, 2004, 306(5696): 666-669.

[50] Bae S-H, Lee Y, Sharma B K, et al. Graphene-based transparent strain sensor[J].Carbon, 2013, 51: 236-242.

[51] Zhao J, Wang G, Yang R, et al. Tunable piezoresistivity of nanographene films forstrain sensing[J]. ACS Nano, 2015, 9(2): 1622-1629.

[52] Rinaldi A, Proietti A, Tamburrano A, et al. Graphene-based strain sensor array oncarbon fiber composite laminate[J]. IEEE Sensors Journal, 2015, 15(12): 7295-7303.

[53] Ye X, Yuan Z, Tai H, et al. A wearable and highly sensitive strain sensor based onpolyethylenimine-rGO layered nanocomposite thin film[J]. Journal of MaterialsChemistry C, 2017, 5(31): 7746-7752.

[54] Yan C, Wang J, Kang W, et al. Highly stretchable piezoresistive graphenenanocellulose nanopaper for strain sensors[J]. Advanced Materials, 2013, 26(13):2022-2027.

[55] Coskun M B, Akbari A, Lai D T H, et al. Ultrasensitive strain sensor produced bydirect patterning of liquid crystals of graphene oxide on a flexible substrate[J].ACS Applied Materials & Interfaces, 2016, 8(34): 22501-22505.

[56] Tao L, Wang D, Tian H, et al. Self-adapted and tunable graphene strain sensorsfor detecting both subtle and large human motions[J]. Nanoscale, 2017, 9(24): 8266-8273.

[57] Li X, Yang T, Yang Y, et al. Large-area ultrathin graphene films by single-stepmarangoni self-assembly for highly sensitive strain sensing application[J].Advanced Functional Materials, 2016, 26(9): 1322-1329.

[58] Wang D, Tao L, Liu Y, et al. High performance flexible strain sensor based onself-locked overlapping graphene sheets[J]. Nanoscale, 2016, 8(48): 20090-20095.

[59] Liu Y, Zhang D, Wang K, et al. A novel strain sensor based on graphene composite films with layered structure[J]. Composites Part A: Applied Science andManufacturing, 2015, 80: 95-103.

[60] Chen S, Wei Y, Wei S, et al. Ultrasensitive cracking-assisted strain sensors basedon silver nanowires/graphene hybrid particles[J]. ACS Applied Materials &Interfaces, 2016, 8(38): 25563-25570.

[61] Liu S, Lin Y, Wei Y, et al. A high performance self-healing strain sensor withsynergetic networks of poly(ɛ-caprolactone) microspheres, graphene and silvernanowires[J]. Composites Science and Technology, 2017, 146: 110-118.

[62] Luo S, Liu T. SWCNT/graphite nanoplatelet hybrid thin films for selftemperature-compensated, highly sensitive, and extensible piezoresistivesensors[J]. Advanced Materials, 2013, 25(39): 5650-5657.

[63] Shi J, Li X, Cheng H, et al. Graphene reinforced carbon nanotube networks forwearable strain sensors[J]. Advanced Functional Materials, 2016, 26(13): 2078-2084.

[64] Yang Z, Wang D Y, Pang Y, et al. Simultaneously detecting subtle and intensivehuman motions based on a silver nanoparticles bridged graphene strain sensor[J].ACS Applied Materials & Interfaces, 2018, 10(4): 3948-3954.

[65] Liu Q, Chen J, Li Y, et al. High-performance strain sensors with fish-scale-likegraphene-sensing layers for full-range detection of human motions[J]. ACS Nano,2016, 10(8): 7901-7906.

[66] Shi X, Liu S, Sun Y, et al. Lowering internal friction of 0D-1D-2D ternarynanocomposite-based strain sensor by fullerene to boost the sensingperformance[J]. Advanced Functional Materials, 2018, 28(22): 1800850.

[67] Inoue N, Onoe H. Graphene-based inline pressure sensor integrated with microfluidic elastic tube[J]. Journal of Micromechanics and Microengineering,2018, 28(1): 014001.

[68] Liu Y, Li C, Shi X, et al. High-sensitivity graphene MOEMS resonant pressuresensor[J]. ACS Applied Materials & Interfaces, 2023, 15(25): 30479-30485.

[69] Lee C, Ahn J, Lee K B, et al. Graphene-based flexible NO2 chemical sensors[J].Thin Solid Films, 2012, 520(16): 5459-5462.

[70] Yang G, Lee C, Kim J, et al. Flexible graphene-based chemical sensors on papersubstrates[J]. Physical Chemistry Chemical Physics, 2013, 15(6): 1798-1801.

[71] Dua V, Surwade S P, Ammu S, et al. All-organic vapor sensor using inkjet-printedreduced graphene oxide[J]. Angewandte Chemie International Edition, 2010,49(12): 2154-2157.

[72] Hassinen J, Kauppila J, Leiro J, et al. Low-cost reduced graphene oxide-basedconductometric nitrogen dioxide-sensitive sensor on paper[J]. Analytical andBioanalytical Chemistry, 2013, 405(11): 3611-3617.

[73] Chen Q, Liu D, Lin L, et al. Bridging interdigitated electrodes by electrochemicalassisted deposition of graphene oxide for constructing flexible gas sensor[J].Sensors and Actuators B: Chemical, 2019, 286: 591-599.

[74] Seekaew Y, Lokavee S, Phokharatkul D, et al. Low-cost and flexible printedgraphene-PEDOT:PSS gas sensor for ammonia detection[J]. Organic Electronics,2014, 15(11): 2971-2981.

[75] Guo Y, Wang T, Chen F, et al. Hierarchical graphene-polyaniline nanocompositefilms for high-performance flexible electronic gas sensors[J]. Nanoscale, 2016,8(23): 12073-12080.

[76] Chung M G, Kim D-H, Seo D K, et al. Flexible hydrogen sensors using graphenewith palladium nanoparticle decoration[J]. Sensors and Actuators B: Chemical,2012, 169: 387-392.

[77] Huang L, Wang Z, Zhang J, et al. Fully printed, rapid-response sensors based onchemically modified graphene for detecting NO2 at room temperature[J]. ACSApplied Materials & Interfaces, 2014, 6(10): 7426-7433.

[78] Kim Y, Choi Y S, Park S Y, et al. Au decoration of a graphene microchannel forself-activated chemoresistive flexible gas sensors with substantially enhanced参考文献- 117 -response to hydrogen[J]. Nanoscale, 2019, 11(6): 2966-2973.

[79] Naganaboina V R, Singh S G. Graphene-CeO2 based flexible gas sensor:monitoring of low ppm CO gas with high selectivity at room temperature[J].Applied Surface Science, 2021, 563: 150272.

[80] Yi J, Lee J M, Park W I. Vertically aligned ZnO nanorods and graphene hybridarchitectures for high-sensitive flexible gas sensors[J]. Sensors and Actuators B:Chemical, 2011, 155(1): 264-269.

[81] Jeong H Y, Lee D-S, Choi H K, et al. Flexible room-temperature NO2 gas sensorsbased on carbon nanotubes/reduced graphene hybrid films[J]. Applied PhysicsLetters, 2010, 96(21): 213105.

[82] Kim S J, Koh H J, Ren C E, et al. Metallic Ti3C2Tx MXene gas sensors withultrahigh signal-to-noise ratio[J]. ACS Nano, 2018, 12(2): 986-993.

[83] Ren Z, Shi Y, Song T, et al. Flexible low-temperature ammonia gas sensor basedon reduced graphene oxide and molybdenum disulfide[J]. Chemosensors, 2021,9(12): 345.

[84] Kang J Y, Koo W T, Jang J S, et al. 2D layer assembly of Pt-ZnO nanoparticles onreduced graphene oxide for flexible NO2 sensors[J]. Sensors and Actuators B:Chemical, 2021, 331: 129371.

[85] Wang J, Fatima-Ezzahra E, Dai J, et al. Ligand-assisted deposition of ultra-smallAu nanodots on Fe2O3/reduced graphene oxide for flexible gas sensors[J].Nanoscale Advances, 2022, 4(5): 1345-1350.

[86] Lin J, Peng Z, Liu Y, et al. Laser-induced porous graphene films from commercialpolymers[J]. Nature Communications, 2014, 5: 5714.

[87] Beckham J L, Li J T, Stanford M G, et al. High-resolution laser-induced graphenefrom photoresist[J]. ACS Nano, 2021, 15(5): 8976-8983.

[88] Ye R, Chyan Y, Zhang J, et al. Laser-induced graphene formation on wood[J].Advanced Materials, 2017, 29(37): 1702211.

[89] Le T S D, Phan H P, Kwon S, et al. Recent advances in laser-induced graphene:mechanism, fabrication, properties, and applications in flexible electronics[J].Advanced Functional Materials, 2022, 32(48): 2205158.

[90] Zhu J, Huang X, Song W. Physical and chemical sensors on the basis of laser induced graphene: mechanisms, applications, and perspectives[J]. ACS Nano,2021, 15(12): 18708-18741.

[91] Stanford M G, Li J T, Chyan Y, et al. Laser-induced graphene triboelectricnanogenerators[J]. ACS Nano, 2019, 13(6): 7166-7174.

[92] Kothuru A, Fernando P. Laser-induced graphene structures: from synthesis andapplications to future prospects[J]. Materials Today, 2023, 70: 104-136.

[93] Luo S D, Hoang P T, Liu T. Direct laser writing for creating porous graphiticstructures and their use for flexible and highly sensitive sensor and sensorarrays[J]. Carbon, 2016, 96: 522-531.

[94] Carvalho A F, Fernandes A J S, Leitão C, et al. Laser-induced graphene strainsensors produced by ultraviolet irradiation of polyimide[J]. Advanced FunctionalMaterials, 2018, 28(52): 1805271.

[95] Liu W, Huang Y, Peng Y, et al. Stable wearable strain sensors on textiles by directlaser writing of graphene[J]. ACS Applied Nano Materials, 2020, 3(1): 283-293.

[96] Kulyk B, Silva B F R, Carvalho A F, et al. Laser-induced graphene from paper formechanical sensing[J]. ACS Applied Materials & Interfaces, 2021, 13(8): 10210-10221.

[97] Rahimi R, Ochoa M, Yu W, et al. Highly stretchable and sensitive unidirectionalstrain sensor via laser carbonization[J]. ACS Applied Materials & Interfaces,2015, 7(8): 4463-4470.

[98] Dallinger A, Keller K, Fitzek H, et al. Stretchable and skin-conformableconductors based on polyurethane/laser-induced graphene[J]. ACS AppliedMaterials & Interfaces, 2020, 12(17): 19855-19865.

[99] Liu W, Chen Q, Huang Y, et al. In situ laser synthesis of Pt nanoparticlesembedded in graphene films for wearable strain sensors with ultra-highsensitivity and stability[J]. Carbon, 2022, 190: 245-254.

[100] Wang W, Lu L, Lu X, et al. Scorpion-inspired dual-bionic, microcrack-assistedwrinkle based laser induced graphene-silver strain sensor with high sensitivityand broad working range for wireless health monitoring system[J]. NanoResearch, 2022, 16(1): 1228-1241.

[101] Chhetry A, Sharifuzzaman M, Yoon H, et al. MoS2-decorated laser-induced graphene for a highly sensitive, hysteresis-free, and reliable piezoresistive strainsensor[J]. ACS Applied Materials & Interfaces, 2019, 11(25): 22531-22542.

[102] Stanford M G, Yang K C, Chyan Y, et al. Laser-induced graphene for flexible andembeddable gas sensors[J]. ACS Nano, 2019, 13(3): 3474-3482.

[103] Zhu J, Cho M, Li Y T, et al. Biomimetic turbinate-like artificial nose for hydrogendetection based on 3D porous laser-induced graphene[J]. ACS Applied Materials& Interfaces, 2019, 11(27): 24386-24394.

[104] Yan W H, Yan W R, Chen T D, et al. Size-tunable flowerlike MoS2 nanospherescombined with laser-induced graphene electrodes for NO2 sensing[J]. ACSApplied Nano Materials, 2020, 3(3): 2545-2553.

[105] Peng Z R, Tao L Q, Zou S M, et al. A multi-functional NO2 gas monitor and selfalarm based on laser-induced graphene[J]. Chemical Engineering Journal, 2022,428(5651): 131079.

[106] Faghihnasiri M, Ahmadi A, Golpayegan S A, et al. A first-principles study ofnonlinear elastic behavior and anisotropic wlectronic properties of twodimensional HfS2[J]. Nanomaterials, 2020, 10(3): 446.

[107] Ding G Q, Gao G Y, Huang Z S, et al. Thermoelectric properties of monolayerMSe2 (M = Zr, Hf): low lattice thermal conductivity and a promising figure ofmerit[J]. Nanotechnology, 2016, 27(37): 375703.

[108] Irelan R M, Henderson T M, Scuseria G E. Long-range-corrected hybrids using arange-separated Perdew-Burke-Ernzerhof functional and random phaseapproximation correlation[J]. Journal of Chemical Physics, 2011, 135(9): 094105.

[109] Perdew J P, Burke K, Ernzerhof M. Generalized gradient approximation madesimple[J]. Physical Review Letters, 1997, 78(7): 1396.

[110] Delley B. DMol, a standard tool for density functional calculations: Review andadvances[J]. Theoretical and Computational Chemistry, 1995, 2: 221-254.

[111] Grimme S. Semiempirical GGA-type density functional constructed with a longrange dispersion correction[J]. Journal of Computational Chemistry, 2006, 27(15):1787-1799.

[112] Behler J. Atom-centered symmetry functions for constructing high-dimensionalneural network potentials[J]. Journal of Chemical Physics, 2011, 134(7): 074106.

[113] Delley B. Hardness conserving semilocal pseudopotentials[J]. Physical Review B,2002, 66(15): 155125.

[114] Delley B. An all‐electron numerical method for solving the local densityfunctional for polyatomic molecules[J]. Journal of Chemical Physics, 1990, 92(1):508-517.

[115] Song H Y, Sun J J, Li M. Enhancement of monolayer HfSe2 thermoelectricperformance by strain engineering: a DFT calculation[J]. Chemical PhysicsLetters, 2021, 784(7345): 139109.

[116] Abbasi A, Sardroodi J J. Adsorption and dissociation of H2S on nitrogen-dopedTiO2 anatase nanoparticles: Insights from DFT computations[J]. Surfaces andInterfaces, 2017, 8: 15-27.

[117] Pei Z, Xiong X, He J, et al. Highly stretchable and durable conductive knittedfabrics for the skins of soft robots[J]. Soft Robot, 2019, 6(6): 687-700.

[118] Li Y, Miao X, Chen J Y, et al. Sensing performance of knitted strain sensor ontwo-dimensional and three-dimensional surfaces[J]. Materials & Design, 2021,197: 109273.

[119] Chen W, Yan X. Progress in achieving high-performance piezoresistive andcapacitive flexible pressure sensors: A review[J]. Journal of Materials Science &Technology, 2020, 43: 175-188.

[120] Nguyen T, Dinh T, Phan H-P, et al. Advances in ultrasensitive piezoresistivesensors: from conventional to flexible and stretchable applications[J]. MaterialsHorizons, 2021, 8(8): 2123-2150.

[121] Zhang J, Chen J, Li M, et al. Design, fabrication, and implementation of an arraytype MEMS piezoresistive intelligent pressure sensor system[J]. Micromachines,2018, 9(3): 104.

[122] Escudero P, Yeste J, Pascual-Izarra C, et al. Color tunable pressure sensors basedon polymer nanostructured membranes for optofluidic applications[J]. ScientificReports, 2019, 9(1): 3259.

[123] Lee C, Wei X, Kysar J W, et al. Measurement of the elastic properties andintrinsic strength of monolayer graphene[J]. Science, 2008, 321(5887): 385-388.

[124] Kim K S, Zhao Y, Jang H, et al. Large-scale pattern growth of graphene films for stretchable transparent electrodes[J]. Nature, 2009, 457(7230): 706-710.

[125] Cocco G, Cadelano E, Colombo L. Gap opening in graphene by shear strain[J].Physical Review B, 2010, 81(24): 241412.

[126] Bunch J S, Verbridge S S, Alden J S, et al. Impermeable atomic membranes fromgraphene sheets[J]. Nano Letters, 2008, 8(8): 2458-2462.

[127] Smith A D, Niklaus F, Paussa A, et al. Electromechanical piezoresistive sensing insuspended graphene membranes[J]. Nano Letters, 2013, 13(7): 3237-3242.

[128] Aguilera-Servin J, Miao T, Bockrath M. Nanoscale pressure sensors realized fromsuspended graphene membrane devices[J]. Applied Physics Letters, 2015, 106:083103.

[129] Milovanović S P, Tadić M Ž, Peeters F M. Graphene membrane as a pressuregauge[J]. Applied Physics Letters, 2017, 111(4): 043101.

[130] Faugeras C, Nerrière A, Potemski M, et al. Few-layer graphene on SiC, pyroliticgraphite, and graphene: A Raman scattering study[J]. Applied Physics Letters,2008, 92(1): 011914

[131] Reina A, Jia X, Ho J, et al. Large area, few-layer graphene films on arbitrarysubstrates by chemical vapor deposition[J]. Nano Letters, 2008, 9(1): 30-35.

[132] Tseng S F, Chen P S, Hsu S H, et al. Investigation of fiber laser-induced porousgraphene electrodes in controlled atmospheres for ZnO nanorod-based NO2 gassensors[J]. Applied Surface Science, 2023, 620(9): 156847.

[133] Kaidarova A, Khan M A, Marengo M, et al. Wearable multifunctional printedgraphene sensors[J]. npj Flexible Electronics, 2019, 3(1): 10.

[134] Lei T, Jingyu Z, Dawei Z, et al. Laser-induced graphene electrodes on poly(ether–ether–ketone)/PDMS composite films for flexible strain and humidity sensors[J].ACS Applied Nano Materials, 2023, 6(19): 17802-17813.

[135] Wang H, Zhao Z, Liu P, et al. A soft and stretchable electronics using laserinduced graphene on polyimide/PDMS composite substrate[J]. npj FlexibleElectronics, 2022, 6(1): 26.

[136] Parmeggiani M, Zaccagnini P, Stassi S, et al. PDMS/polyimide composite as anelastomeric substrate for multifunctional laser-induced graphene electrodes[J].ACS Applied Materials & Interfaces, 2019, 11(36): 33221-33230.

[137] Wang W, Lu L, Li Z, et al. Fingerprint-inspired strain sensor with balancedsensitivity and strain range using laser-induced graphene[J]. ACS AppliedMaterials & Interfaces, 2022, 14(1): 1315-1325.

[138] Xu K, Fujita Y, Lu Y, et al. A wearable body condition sensor system withwireless feedback alarm functions[J]. Advanced Materials, 2021, 33(18):e2008701.

[139] Wang W, Liu Y, Ding M, et al. From network to channel: crack-based strainsensors with high sensitivity, stretchability, and linearity via strain engineering[J].Nano Energy, 2023, 116: 108832.

[140] Song Z, Li W, Bao Y, et al. Breathable and skin-mountable strain sensor withtunable stretchability, sensitivity, and linearity via surface strain delocalization forversatile skin activities' recognition[J]. ACS Applied Materials & Interfaces, 2018,10(49): 42826-42836.

[141] Jing W, Ziyi H, Qiushui C, et al. Biochemical analysis on microfluidic chips[J].Trends in Analytical Chemistry, 2016, 80: 213-231.

[142] Jahn Y M, Ya'akobovitz A. Outstanding stretchability and thickness-dependentmechanical properties of 2D HfS2, HfSe2, and hafnium oxide[J]. Nanoscale, 2021,13(44): 18458-18466.

[143] Bertolazzi S, Brivio J, Kis A. Stretching and breaking of ultrathin MoS2[J]. ACSNano, 2011, 5(12): 9703-9709.

[144] Lin L, Ryan J, Tianyu M, et al. Work function: fundamentals, measurement,calculation, engineering, and applications[J]. Physical Review Applied, 2023,19(3): 037001.

[145] Ferrari A C, Meyer J C, Scardaci V, et al. Raman spectrum of graphene andgraphene layers[J]. Physical Review Letters, 2006, 97(18): 187401.

[146] Luong D X, Yang K, Yoon J, et al. Laser-induced graphene composites asmultifunctional surfaces[J]. ACS Nano, 2019, 13(2): 2579-2586.

[147] Yin L, Xu K, Wen Y, et al. Ultrafast and ultrasensitive phototransistors based onfew-layered HfSe2[J]. Applied Physics Letters, 2016, 109(21): 213105.

[148] Kang M, Rathi S, Lee I, et al. Electrical characterization of multilayer HfSe2 fieldeffect transistors on SiO2 substrate[J]. Applied Physics Letters, 2015, 106(14): 43108.

[149] Cruz A, Mutlu Z, Ozkan M, et al. Raman investigation of the air stability of 2Hpolytype HfSe2 thin films[J]. MRS Communications, 2018, 8(3): 1191-1196.

[150] Liu L, Li Y, Huang X, et al. Low-power memristive logic device enabled bycontrollable oxidation of 2D HfSe2 for in-memory computing[J]. AdvancedScience, 2021, 8(15): e2005038.

[151] Kang M, Rathi S, Lee I, et al. Tunable electrical properties of multilayer HfSe2field effect transistors by oxygen plasma treatment[J]. Nanoscale, 2017, 9(4):1645-1652.

[152] Mirabelli G, Mcgeough C, Schmidt M, et al. Air sensitivity of MoS2, MoSe2,MoTe2, HfS2, and HfSe2[J]. Journal of Applied Physics, 2016, 120(12): 125102.

[153] Chhetry A, Sharma S, Barman S C, et al. Black phosphorus@laser-engravedgraphene heterostructure-based temperature-strain hybridized sensor forelectronic-skin applications[J]. Advanced Functional Materials, 2020, 31(10):2007661.

[154] Cheng X, Cai J, Xu J, et al. High-performance strain sensors based onAu/graphene composite films with hierarchical cracks for wide linear-rangemotion monitoring[J]. ACS Applied Materials & Interfaces, 2022, 14(34): 39230-39239.

[155] Li Q, Wu T, Zhao W, et al. Laser-induced corrugated graphene films for integratedmultimodal sensors[J]. ACS Applied Materials & Interfaces, 2021, 13(31):37433-37444.

[156] Ma Y, Li Z, Han J, et al. Vertical graphene canal mesh for strain sensing with asupereminent resolution[J]. ACS Applied Materials & Interfaces, 2022, 14(28):32387-32394.

[157] Zhang J, Liu X, Neri G, et al. Nanostructured materials for room-temperature gassensors[J]. Advanced Materials, 2016, 28(5): 795-831.

[158] Jung H T. The present and future of gas sensors[J]. ACS Sensors, 2022, 7(4): 912-913.

[159] Li H, Yin Z, He Q, et al. Fabrication of single- and multilayer MoS2 film-basedfield-effect transistors for sensing NO at room temperature[J]. Small, 2012, 8(1): 63-67.

[160] Zhang D, Wang M, Zhang W, et al. Flexible humidity sensing and portableapplications based on MoSe2 nanoflowers/copper tungstate nanoparticles[J].Sensors and Actuators B: Chemical, 2020, 304: 127234.

[161] Ko K Y, Song J G, Kim Y, et al. Improvement of gas-sensing performance oflarge-area tungsten disulfide nanosheets by surface functionalization[J]. ACSNano, 2016, 10(10): 9287-9296.

[162] Guo H, Lan C, Zhou Z, et al. Transparent, flexible, and stretchable WS2 basedhumidity sensors for electronic skin[J]. Nanoscale, 2017, 9(19): 6246-6253.

[163] Eftekhari A. Tungsten dichalcogenides (WS2, WSe2, and WTe2): materialschemistry and applications[J]. Journal of Materials Chemistry A, 2017, 5(35):18299-18325.

[164] Guo S, Yang D, Zhang S, et al. Development of a cloud-based epidermal MoSe2device for hazardous gas sensing[J]. Advanced Functional Materials, 2019,29(18): 1900138.

[165] Kumar R, Zheng W, Liu X, et al. MoS2-based nanomaterials for roomtemperature gas sensors[J]. Advanced Materials Technologies, 2020, 5(5):1901062.

[166] Baek D-H, Kim J. MoS2 gas sensor functionalized by Pd for the detection ofhydrogen[J]. Sensors and Actuators B: Chemical, 2017, 250: 686-691.

[167] Ko K Y, Lee S, Park K, et al. High-performance gas sensor using a large-areaWS2xSe2-2x alloy for low-power operation wearable applications[J]. ACS AppliedMaterials & Interfaces, 2018, 10(40): 34163-34171.

[168] Lebègue S, Björkman T, Klintenberg M, et al. Two-dimensional materials fromdata filtering and ab initio calculations[J]. Physical Review X, 2013, 3(3): 031002.

[169] Gong C, Zhang H, Wang W, et al. Band alignment of two-dimensional transitionmetal dichalcogenides: Application in tunnel field effect transistors[J]. AppliedPhysics Letters, 2013, 103(5): 053513.

[170] Cui H, Jia P, Peng X. Adsorption of SO2 and NO2 molecule on intrinsic and Pddoped HfSe2 monolayer: A first-principles study[J]. Applied Surface Science,2020, 513: 145863.

[171] Cui H, Zhu H, Jia P. Adsorption and sensing of SO2 and SOF2 molecule by Ptdoped HfSe2 monolayer: a first-principles study[J]. Applied Surface Science,2020, 530: 147242.

[172] Timmer B, Olthuis W, Berg A V D. Ammonia sensors and their applications-areview[J]. Sensors and Actuators B: Chemical, 2005, 107(2): 666-677.

[173] Sui N, Zhang P, Zhou T, et al. Selective ppb-level ozone gas sensor based onhierarchical branch-like In2O3 nanostructure[J]. Sensors and Actuators B:Chemical, 2021, 336: 129612.

[174] Niu F, Tao L M, Deng Y C, et al. Phosphorus doped graphene nanosheets forroom temperature NH3 sensing[J]. New Journal of Chemistry, 2014, 38(6): 2269.

[175] Feng Q, Li X, Wang J, et al. Reduced graphene oxide (rGO) encapsulated Co3O4composite nanofibers for highly selective ammonia sensors[J]. Sensors andActuators B: Chemical, 2016, 222: 864-870.

[176] Feng Q, Li X, Wang J. Percolation effect of reduced graphene oxide (rGO) onammonia sensing of rGO-SnO2 composite based sensor[J]. Sensors and ActuatorsB: Chemical, 2017, 243: 1115-1126.

[177] Wang T, Sun Z, Huang D, et al. Studies on NH3 gas sensing by zinc oxidenanowire-reduced graphene oxide nanocomposites[J]. Sensors and Actuators B:Chemical, 2017, 252: 284-294.

[178] Lin Q, Li Y, Yang M. Tin oxide/graphene composite fabricated via a hydrothermalmethod for gas sensors working at room temperature[J]. Sensors and Actuators B:Chemical, 2012, 173: 139-147.

[179] Wang X, Gu D, Li X, et al. Reduced graphene oxide hybridized with WS2nanoflakes based heterojunctions for selective ammonia sensors at roomtemperature[J]. Sensors and Actuators B: Chemical, 2019, 282: 290-299.

[180] Haridas V, Sukhananazerin A, Mary Sneha J, et al. α-Fe2O3 loaded less-defectivegraphene sheets as chemiresistive gas sensor for selective sensing of NH3[J].Applied Surface Science, 2020, 517: 146158.

[181] Ye Z, Tai H, Guo R, et al. Excellent ammonia sensing performance of gas sensorbased on graphene/titanium dioxide hybrid with improved morphology[J].Applied Surface Science, 2017, 419: 84-90.

[182] Su P G, Yang L Y. NH3 gas sensor based on Pd/SnO2/rGO ternary compositeoperated at room-temperature[J]. Sensors and Actuators B: Chemical, 2016, 223:202-208.

[183] Schedin F, Geim A K, Morozov S V, et al. Detection of individual gas moleculesadsorbed on graphene[J]. Nature Materials, 2007, 6(9): 652-6555.

[184] Chen Y, Zhang W, Wu Q. A highly sensitive room-temperature sensing materialfor NH3: SnO2-nanorods coupled by rGO[J]. Sensors and Actuators B: Chemical,2017, 242: 1216-1226.

[185] Lu G, Ocola L E, Chen J. Reduced graphene oxide for room-temperature gassensors[J]. Nanotechnology, 2009, 20(44): 445502.

[186] Cho D Y, Min C H, Kim J, et al. Bond nature of oxygen-deficient HfO2/Si(100)film[J]. Applied Physics Letters, 2006, 89(25): 253510.

[187] Ye H, Liu L, Xu Y, et al. SnSe monolayer: a promising candidate of SO2 sensorwith high adsorption quantity[J]. Applied Surface Science, 2019, 484: 33-38.

[188] Liu L, Yang Q, Wang Z, et al. High selective gas detection for small moleculesbased on germanium selenide monolayer[J]. Applied Surface Science, 2018, 433:575-581