Comprehensive Investigation of the Temperature-Dependent Electromechanical Behaviors of Carbon Nanotube/Polymer Composites.

The performances of flexible piezoresistive sensors based on polymer nanocomposites are significantly affected by the environmental temperature; therefore, comprehensively investigating the temperature-dependent electromechanical response behaviors of conductive polymer nanocomposites is crucial for developing high-precision flexible piezoresistive sensors in a wide-temperature range. Herein, carbon nanotube (CNT)/polydimethylsiloxane (PDMS) composites widely used for flexible piezoresistive sensors were prepared, and then the temperature-dependent electrical, mechanical, and electromechanical properties of the optimized CNT/PDMS composite in the temperature range from -150 to 150 °C were systematically investigated. At a low temperature of -150 °C, the CNT/PDMS composite becomes brittle with a compressive modulus of ∼1.2 MPa and loses its elasticity and reversible sensing capability. At a high temperature (above 90 °C), the CNT/PDMS composite softens, shows a fluid-like mechanical property, and loses its reversible sensing capability. In the temperature range from -60 to 90 °C, the CNT/PDMS composite exhibits good elasticity and reversible sensing behaviors and its modulus, resistivity, and sensing sensitivity decrease with an increasing temperature. At room temperature (30 °C), the CNT/PDMS composite exhibits better mechanical and piezoresistive stability than those at low and high temperatures. Given that environmental temperature changes have significant effects on the sensing performances of conductive polymer composites, the effect of ambient temperature changes must be considered when flexible piezoresistive sensors are designed and fabricated.

Flexible Pressure Sensor with an Excellent Linear Response in a Broad Detection Range for Human Motion Monitoring.

Pressure sensing is highly demanding in wearable devices, robotics, and artificial intelligence, whereas it is still a big challenge to develop a pressure sensor with an excellent linear response in a broad detection range. Herein, a flexible and porous carbon nanotube (CNT)/carbon black (CB)/carbonyl iron powder (CIP)/silicone composite is proposed by a simple strategy of mixing, curing, and washing. Due to the porous structure induced by the sacrifice of sugar particles, an excellent linear response (R2 = 0.999) is achieved for the composite sensor by manipulating the contributions of contact resistance and tunnel resistance to the sensing performance via the alternation of CB and CNT contents. Moreover, the porous structure donates the composite sensor a low compressive modulus at a low pressure level, while the CIPs introduced lead to a high compressive modulus at a high pressure level with the assistance of an external magnetic field. As a result, the sensor produced has a wide linear response range of 80 Pa to 220 kPa, much wider than most of the linear response pressure sensors reported previously. The wide detection range is demonstrated by cyclic pressure tests in the frequency range of 0.1-5 Hz, durability tests, and monitoring human or robot motions including breathing, walking, lifting, and boxing, etc. Taking the advantages of low cost, high sensitivity, and excellent linear response in a wide pressure range, the current composite sensor is promising for precise monitoring of human motions and delicate controlling of robots.

Multiresponsive Ti3C2Tx MXene-Based Actuators Enabled by Dual-Mechanism Synergism for Soft Robotics.

Multiresponsive and high-performance flexible actuators with a simple configuration, high mechanical strength, and low-power consumption are highly desirable for soft robotics. Here, a novel mechanically robust and multiresponsive Ti3C2Tx MXene-based actuator with high actuation performance via dual-mechanism synergistic effect driven by the hygroexpansion of bacterial cellulose (BC) layer and the thermal expansion of biaxially oriented polypropylene (BOPP) layer is developed. The actuator is flexible and shows an ultrahigh tensile strength of 195 MPa. Unlike the conventional bimorph-structured actuators based on a single-mechanism, the actuator developed provides a favorable architecture for dual-mechanism synergism, resulting in exceptionally reversible actuation performance under electricity and near-infrared (NIR) light stimuli. Typically, the developed actuator can produce the largest bending angle (∼400°) at the lowest voltage (≤4 V) compared with that reported previously for single mechanism soft actuators. Furthermore, the actuator also can be driven by a NIR light at a 2 m distance, displaying an excellent long-distance photoresponsive property. Finally, various intriguing applications are demonstrated to show the great potential of the actuator for soft robotics.

Multifunctional Polyurethane Composite Foam with Outstanding Anti-impact Capacity for Soft Body Armors.

Herein, a multifunctional polyurethane (PU) composite foam with a hierarchical structure is fabricated by dip-coating a carbon nanotube/shear-thickening gel (CNT/STG) and spray-coating nano-SiO2/STG on PU foam. The prepared nano-SiO2/CNT/STG@PU (SCS@PU) composite foam is lightweight, highly compressive, electrically conductive, superhydrophobic, and impact-energy absorptive. As a result, it possesses an excellent sensing ability to compression with a stable response up to 80% strain, an outstanding linearity of R2 > 0.99, and a wide response frequency of 0.01 to 1 Hz; it can also be used for effectively detecting impact force and sensing various human motions. Moreover, the superhydrophobicity with a water contact angle up to 154° of SCS@PU composite foam endows it with an excellent resistance to hazardous liquids (strong acid and alkali) to ensure its service reliability under harsh circumstances. In particular, the SCS@PU exhibits an outstanding anti-impact capability with an impact force attenuation rate of SCS@PU as high as 81%. Finally, its applications as soft body armors are demonstrated in protecting a wearer wearing a helmet with the SCS@PU as liner and using the SCS@PU as a smart kneecap against impact. On consideration of its excellent strain-sensing ability, superhydrophobicity, and outstanding anti-impact capability, the multifunctional SCS@PU composite foam developed is promising for personal safety protection.

Superstrong, Lightweight, and Exceptional Environmentally Stable SiO2@GO/Bamboo Composites.

Development of lightweight structural materials from fast-growing bamboos is of great significance to building a sustainable society. However, previously developed structural bamboos by delignification combined with densification would easily fail under large external loading after exposure to water due to structure collapse, severely limiting their practical applications. Here, we demonstrate an ultrastrong and exceptional environmentally stable bamboo composite consisting of a graphene oxide (GO)/bamboo core and hierarchical SiO2 protection layer. The GO/bamboo composite exhibits ultrahigh tensile strength (641.6 MPa), superb flexural strength (428.4 MPa), and excellent toughness (17.5 MJ/m3), which are increased by about 480, 250, and 360% compared with natural bamboo, respectively. As a result, the specific tensile strength of the GO/bamboo composite is up to 513.3 MPa·cm3/g due to its low density (1.25 g/cm3), outperforming engineering structural materials such as aluminum alloys, steels, and titanium alloys. These large improvements benefit from the well-preserved bamboo scaffold and the strong hydrogen bonds between bamboo fibers and GO nanosheets. On the other hand, the SiO2@GO/bamboo composite shows superhydrophobicity due to the construction of hierarchical SiO2 layers, which endows it with outstanding water resistance. Moreover, the bamboo composite shows an ultralow coefficient of thermal expansion (≈2.3 × 10-6 K-1), indicating its excellent dimensional stability. Considering the ultrahigh mechanical performance and outstanding environmental stability, the developed lightweight SiO2@GO/bamboo composite is hopeful to be a green and sustainable structural material for practical engineering applications.

One-Step Synthesis of Microdome Patterns for Microstructured Pressure Sensors with Ultra-High Sensing Performance.

Pressure sensors usually suffer from a trade-off between sensitivity and the linear sensing range, which may be improved by manipulating the geometric microstructure of active sensing materials via the molding strategy, standard photolithography technique, and so on. However, these conventional microengineering techniques require specialized equipment, which are extremely complicated, high-cost, and time-consuming to manufacture. Herein, a mold-free, scalable, low-cost, and environment-friendly one-step thermofoaming strategy is proposed to fabricate surface morphology-tunable microdome-patterned composites (MPCs). The microstructured pressure sensor is then prepared by coating the MPCs with highly conductive graphene. Remarkably, the as-prepared pressure sensor presents a better overall sensing performance compared to the previous pressure sensors prepared using complicated microengineering methods. Moreover, an electromechanical response model and finite-element analysis are used to clarify the sensing mechanisms of the present microstructured pressure sensor. Furthermore, several successful application demonstrations are conducted under various pressure levels. Considering the advantages of the one-step fabrication strategy over conventional surface microengineering techniques and the high performance of the microstructured pressure sensor, the present pressure sensor has promising potential applications in health monitoring, tactile sensation, wearable devices, etc.

Polyacrylamide Hydrogel Composite E-skin Fully Mimicking Human Skin.

Transparent e-skin that can fully mimic human skin with J-shaped mechanical-behavior and tactile sensing attributes have not yet been reported. In this work, the skin-like hydrogel composite with J-shaped mechanical behavior and highly transparent, tactile, soft but strong, flexible, and stretchable attributes is developed as structural strain sensing element for e-skin. Piezo-resistive polyacrylamide (PAAm) hydrogel is used as supporting matrix to endow high transparency, softness, flexibility, stretch-ability and strain sensing capability desired for e-skin. Ultrahigh molecular weight polyethylene (UHMWPE) fiber with a wavy configuration is designed as reinforcement filler to provide the tunable strain-limiting effect. As a result, the as-prepared UHMWPE fiber/PAAm composite e-skin presents unique "J-shape" stress-strain behavior akin to human skin. And the PAAm composite can switch from supersoft to highly stiff in the designed strain range up to 100% with a prominent tensile strength of 48.3 MPa, which enables it to have the high stretch-ability and excellent load-bearing ability, simultaneously. Moreover, finite element model is developed to clarify the stress distribution and damage evolution for the UHMWPE fiber/PAAm composite during the tensile process. The PAAm composite exhibits not only an excellent strain sensing performance with a long-term reliability up to 5000 loading-unloading cycles but also an extraordinary softness and mechanical strength with a low initial modulus of 6.7 kPa, which is matchable with soft human epidermis. Finally, the e-skin is used for demonstrations in monitoring various human activities and protecting structural integrity in designed strain ranges. The strategy for reinforcing piezo-resistive hydrogel with wavy-shaped UHMWPE fibers proposed here is promising for the development of transparent, flexible, soft but strong e-skin with a tunable strain-limiting effect akin to human skin.

High-Performance Bamboo Steel Derived from Natural Bamboo.

It is highly desirable to develop green and renewable structural materials from biomaterials to replace synthetic materials involved from civil engineering to aerospace industries. Herein, we put forward a facile but effective top-down strategy to convert natural bamboo into bamboo steel. The fabrication process of bamboo steel involves the removal of lignin and hemicellulose, freeze-drying followed by epoxy infiltration, and densification combined with in situ solidification. The prepared bamboo steel is a super-strong composite material with a high specific tensile strength (302 MPa g-1 cm3), which is higher than that (227 MPa g-1 cm3) of conventional high specific strength steel. The bamboo steel demonstrates a high tensile strength of 407.6 MPa, a record flexural strength of 513.8 MPa, and a high toughness of 14.08 MJ/m3, which is improved by 360, 290, and 380% over those of natural bamboo, respectively. Particularly, the mechanical properties of the bamboo steel are the highest among the biofiber-reinforced polymer composites reported previously. The well-preserved bamboo scaffolds assure the integrity of bamboo fibers, while the densification under high pressure results in a high-fiber volume fraction with an improved hydrogen bonding among the adjacent bamboo fibers, and the epoxy resin impregnated enhances the stress transfer because of its chemical crosslinking with cellulose molecules. These endow the bamboo steel with superior mechanical performance. Furthermore, the bamboo steel demonstrates an excellent thermal insulating capability with a low thermal conductivity (about 0.29 W/mK). In addition, the bamboo steel shows a low coefficient of thermal expansion (about 6.3 × 10-6 K-1) and a very high-dimensional stability to moisture attack. The strategy of fabricating high-performance bamboo steel with green and abundant natural bamboo as raw materials is highly attractive for the sustainable development of structural engineering materials.

Bioinspired Color-Changeable Organogel Tactile Sensor with Excellent Overall Performance.

Inspired by chameleons' structural color regulation capability, a simple, but effective, swelling method is proposed for the first time to prepare an ionic polyacrylamide (PAAm) organogel for simultaneous tactile sensing and interactive color changing. The PAAm organogel obtained by swelling the PAAm scaffold in the dimethyl sulfoxide solution of organic electrochromic material (OECM) shows an extremely large stretchability with an elongation of 1600%, a supersoftness with a compressive modulus of 7.2 kPa, an excellent transmittance up to 90%, and a very fast response time of 0.5 s combined with the characteristic of interactive color changing. The PAAm organogel also suggests a universal design ability to tailor coloration spectra for tactile sensors via simply changing the type and content of OECM. The tactile sensor based on a PAAm organogel is capable of serving as a wearable device for precisely tracing human body motion performance and directly visualizing the stress distribution via interactive color changing capability. It is demonstrated that the swelling method proposed here is a simple and practical strategy to prepare ionic organogels with both piezo-resistive and electrochromic effects.

Spider-Inspired Ultrasensitive Flexible Vibration Sensor for Multifunctional Sensing.

Flexible vibration sensors can not only capture broad classes of physiologically relevant information, including mechano-vibration signatures of body processes and precision kinematics of core-body motions, but also detect environmental seismic waves, providing early warning to wearers in time. Spider is one of the most vibration-sensitive creatures because of its hairlike sensilla and lyriform slit structure. Here, a spider-inspired ultrasensitive flexible vibration sensor is designed and fabricated for multifunctional sensing. The vibration sensitivity of the flexible sensor is increased over 2 orders of magnitude from 0.006 to 0.5 mV/g, and the strain sensitivity is hugely enhanced from 0.08 to 150 compared to a plain sensor counterpart. It is shown that the synergistic effect of cilium arrays and cracks is the key for achieving the greatly enhanced vibration and strain sensitivity. The dynamic sensitivity of 0.5 mV/g outperforms the corresponding commercial vibration sensors. The flexible sensor is demonstrated to be generally feasible for detecting vibration signals caused by walk, tumble, and explosion as well as capturing human body motions, indicating its great potential for applications in human health-monitoring devices, posture control in robotics, early earthquake warning, and so forth.

Dual-Mode Carbon Aerogel/Iron Rubber Sensor.

Nowadays, the integration of easy production, simple structure, high sensitivity, and multifunctionality is the developing tendency for flexible sensors. Herein we report a facile manufacture of a highly flexible, sensitive, and multifunctional dual-mode sensor with an ultrasimple structure by directly attaching magnetic iron rubber (IR) onto the surface of carbon aerogel (CA) derived from melamine foam. The dual-mode CA/IR sensor exhibits high sensitivities of 5.6 kPa-1 and 1.6·10-3 Oe-1, respectively, toward pressure and magnetic field in a wide frequency ranging from 0.1 to 10 Hz, which are higher than those of the existing flexible pressure/magnetism sensors. The multifunctionality of the dual-mode CA/IR sensor is demonstrated by monitoring blood pulse, human breath, balloon volume, and thoracic volume via pressure and magnetism sensing or their combination. Due to its simple structure and high sensitivities, the dual-mode sensor is employed as the building block to create a direction-recognizable sensor for identifying the directions of pressure and magnetic field for the awareness of surrounding barriers that are of practical importance in sophisticated situations such as autonomous artificial intelligence, autodriving and robotics, and so on.

High-Performance Fiber-Film Hybrid-Structured Wearable Strain Sensor from a Highly Robust and Conductive Carbonized Bamboo Aerogel.

Bamboo, one of the most abundant biomaterials, has been used as a building material since ancient times; however, its application in functional materials has been rarely explored. Herein, a highly robust and conductive carbonized bamboo aerogel (CBA) is obtained from the natural bamboo through a simple three-step process of pulp oxidization, freeze-drying, and carbonization. The CBA obtained shows not only a low density of 0.02 g/cm3 but also a high conductivity of 6.42 S/m and remarkable elasticity with a maximum recoverable compressive strain of 60% due to its unique three-dimensional (3D) network randomly stacked with the hybrid structure of carbonized bamboo fibers and films. After encapsulation with silicone resin, the CBA/silicone composite prepared exhibits excellent flexibility and stretchability with a low Young's modulus (0.09 MPa) and a large failure strain (275%). Importantly, the CBA/silicone composite also offers remarkable strain-sensing performance with a maximum gauge factor of 30.6, a short responsive time of 50 ms, and a stable response to cyclic loading over 1000 cycles, which is comparable to those of the piezoresistive composites based on expensive nanomaterials. Moreover, the CBA/silicone composite demonstrates the capability as a wearable strain sensor for human motion recognition comprising finger bending, breathing, and throat movement. Considering the green and sustainable nature of bamboo as a raw material, combined with the excellent piezoresistive performance, low production cost, and simple preparation process, the flexible strain sensors with CBA/silicone composite as a sensing element are promising in wearable electronic devices, personalized healthcare, and artificial intelligence systems.

High-Performance Structural Flexible Strain Sensors Based on Graphene-Coated Glass Fabric/Silicone Composite.

Recently, various piezoresistive composites with good flexibility have been developed as sensing materials for flexible strain sensors (FSSs). External forces will be applied to strain sensors when they are used in some circumstances such as wrist bending, etc. However, conventional flexible composites may fail upon being subjected to external forces since they have low strength and are unable to protect the inner vulnerable structure of flexible sensors. In this work, the reduced graphene oxide-coated glass fabric (RGO@GF)/silicone composite is fabricated and used to make high-performance structural flexible strain sensors. The composite is not only flexible and sensitive to strain, but also exhibits the high tensile strength needed to maintain the structural integrity of the flexible strain sensor. Silicone resin and GF are employed to provide flexibility and high strength, respectively. By coating RGO on the surface of GF, the nonconductive GF becomes conductive, which renders the piezoresistive behavior and strain-sensing ability to the RGO@GF/silicone composite. The as-prepared structural flexible sensor not only possesses a good strain sensitivity with a gauge factor of around 113, which is much higher than that of typical strain sensors based on metals, but can also maintain its structural integrity until the applied external force is over 800 N, while the conventional flexible strain sensor fails upon being subjected to an external force of only 5 N. Moreover, the as-prepared structural FSS is applied to monitor wrist movement and breathing to demonstrate its applicability. Overall, the RGO@GF/silicone composite exhibits great potential as a sensing material for structural FSSs for wrist movement, etc.

Bioinspired Flexible and Highly Responsive Dual-Mode Strain/Magnetism Composite Sensor.

The mimicry of human skin to detect both oncoming and physical-contacting object is of great importance in the fields of manufacturing, artificial robots and vehicles, etc. Herein, a novel bioinspired flexible and highly responsive dual-mode strain/magnetism composite sensor, which works via both contact and contactless modes, is first fabricated by incorporating Fe3O4/silicone system into a carbon fiber aerogel (CFA). The distance dependence of magnetic field endorses the CFA/Fe3O4/silicone composite possible for spatial sensing due to the introduction of Fe3O4 magnetic nanoparticles. As a result, the as-prepared flexible sensor exhibits precise and real-time response not only to direct-contact compression as usual but also to contactless magnetic field in a wide frequency range from 0.1 to 10 Hz, achieving the maximum variance of 68% and 86% in relative electrical resistance, respectively. The contact and contactless sensing modes of the strain/magnetism sensor are clearly demonstrated by recording the speeds of bicycle riding and walking, respectively. Interestingly, this dual-mode composite sensor exhibits the capacity of identifying the contact and contactless state, which is the first report for flexible sensors. The current protocol is eco-friendly, facile, and thought-provoking for the fabrication of multifunctional sensors.

Bio-inspired highly flexible dual-mode electronic cilia.

Inspired by biological cilia, a highly flexible dual-mode electronic cilia (EC) sensor is fabricated from graphene-coated magnetic cilia arrays. Polydimethylsiloxane is used as a matrix to make the artificial cilia flexible while Co particles are used to endow the cilia with magnetic properties and graphene coating is employed to make the cilia conductive. The EC-based sensor shows a high sensitivity of 0.4% Pa-1 for a pressure of 0-100 Pa and a low detection limit of 0.9 Pa. The responsive behavior of the EC-based sensor is highly stable in a wide frequency range of 0.1-10 Hz up to 10 000 cycles. Meanwhile, the magnetic field sensitivity of the EC sensor is around 12.08 T-1 for a magnetic field intensity of 150-160 mT. Consequently, the EC sensor is successfully applied in blood pulse monitoring, pressure and magnetic field switching, and visualized pressure and magnetic field detection. Due to its high sensitivity, high durability and dual-mode responsiveness, the flexible EC sensor goes far beyond the capability of human skin, and is believed to have great potential in healthcare, robotics, e-skin and smart surgical tools, etc.

Laser-Printed In-Plane Micro-Supercapacitors: From Symmetric to Asymmetric Structure.

Here, we propose and demonstrate a complete solution for efficiently fabricating in-plane micro-supercapacitors (MSCs) from a symmetric to asymmetric structure. By using an original laser printing process, symmetric MSC with reduced graphene oxide (rGO)/silver nanowire (Ag-NW) hybrid electrodes was facilely fabricated and a high areal capacitance of 5.5 mF cm-2 was achieved, which reaches the best reports on graphene-based MSCs. More importantly, a "print-and-fold" method has been creatively proposed that enabled the rapid manufacturing of asymmetric in-plane MSCs beyond the traditional cumbersome technologies. α-Ni(OH)2 particles with high tapping density were successfully synthesized and employed as the pseudocapacitive material. Consequently, an improved supply voltage of 1.5 V was obtained and an areal capacitance as high as 8.6 mF cm-2 has been realized. Moreover, a demonstration of a miniaturized MSC pack was performed by multiply-folding the serial Ag-NW-connected MSC units. As a result, a compact MSC pack with a high supply voltage of 3 V was obtained, which can be utilized to power a light-emitting diode light. These presented technologies may pave the way for the efficiently producing high performance in-plane MSCs, meanwhile offering a solution for the achievement of practical power supply packs integrated in limited spaces.

A Novel Type of Battery-Supercapacitor Hybrid Device with Highly Switchable Dual Performances Based on a Carbon Skeleton/Mg2Ni Free-Standing Hydrogen Storage Electrode.

The sharp proliferation of high power electronics and electrical vehicles has promoted growing demands for power sources with both high energy and power densities. Under these circumstances, battery-supercapacitor hybrid devices are attracting considerable attention as they combine the advantages of both batteries and supercapacitors. Here, a novel type of hybrid device based on a carbon skeleton/Mg2Ni free-standing electrode without the traditional nickel foam current collector is reported, which has been designed and fabricated through a dispersing-freeze-drying method by employing reduced graphene oxide (rGO) and multiwalled carbon nanotubes (MWCNTs) as a hybrid skeleton. As a result, the Mg2Ni alloy is able to deliver a high discharge capacity of 644 mAh g-1 and, more importantly, a high cycling stability with a retention of over 78% after 50 charge/discharge cycles have been achieved, which exceeds almost all the results ever reported on the Mg2Ni alloy. Simultaneously, the electrode could also exhibit excellent supercapacitor performances including high specific capacities (296 F g-1) and outstanding cycling stability (100% retention after 100 cycles). Moreover, the hybrid device can switch between battery and supercapacitor modes immediately as needed during application. These features make the C skeleton/alloy electrode a highly promising candidate for battery-supercapacitor hybrid devices with high power/energy density and favorable cycling stability.

A paper-based touch sensor with an embedded micro-probe array fabricated by double-sided laser printing.

Touch sensor is one of the key components for human interfacing devices. However, although various touch sensors have been demonstrated, their sophisticated fabrication processes and complicated structures make them expensive and delicate, and thus they are not considered to be practical for wide application in daily life. Herein, we present a low-cost and scalable paper-based touch sensor suitable for practical applications. The sensor is based on the novel structure of embedded silver nanowire micro-probe arrays in a paper substrate, which exhibits high sensitivity to multiple touch inputs and compact structure with a total thickness of ca. 100 µm. Silver nanowire electrodes on two sides are manufactured at the same time via an original double-sided laser printing technique. Since this technique is mask-free, solvent-free and highly efficient, it is very suitable for paper substrates that cannot endure solvent processing. The sensing properties of the sensor in various extreme situations are examined and the spatial distributions of touch pressure are detected by arranging the sensing units in arrays. Demonstration examples of the touch sensor and pressure mapping are presented, and finally, the successful application of the sensor array in an electronic lock system is shown to further illustrate its applicability.

High performance surface-modified TiO2/silicone nanocomposite.

The mismatch of refractive index (RI) between light emitting diode (LED) chips and packaging resins severely lowers the lighting emitting efficacy of LED. The RI can be enhanced by the introduction of high RI nanoparticles but meanwhile it is a great challenge to maintain the high transparency for resins due to the agglomeration of nanoparticles. In this work, a facile strategy is proposed to fabricate silicone nanocomposites with a high transparency (>88%, less than 2% decrease relative to pure silicone resin), largely enhanced RI (an increase from 1.42 to 1.60) and improved thermal stability (73 °C increase in weight loss of 50%). Specifically, the ultra-fine monodispersed TiO2/silicone composites are prepared by direct solvent mixing of 1 wt% surface modified TiO2 nanoparticles (S-TiO2) into the silicone resin, in which S-TiO2 are prepared by direct introduction of titanate coupling agent in the process of TiO2 growth to induce the formation of protective layer on the surfaces of TiO2 nanoparticles. This methodology demonstrated is simple, cost-effective and versatile for the massive fabrication of highly transparent LED packaging materials with greatly enhanced refractive index and meanwhile enhanced thermal stability.