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Journal of Materials Chemistry A · 2022 ·Vol. 10 ·期 24 ·12921-12927 · IF 14.511

Direct ink writing of high-performance Bi2Te3-based thermoelectric materials using quasi-inorganic inks and interface engineering

Zhengshang Wang,Wen Cui,Hao Yuan,Xiaoli Kang,Zhou Zheng,Longqin Chen,Qiujun Hu,Wenbin Qiu,Jun Tang,Xudong Cui

Direct ink writing offers a unique solution for constructing shape-controllable devices. In this way, thermoelectric (TE) devices can optimize power generation from industrial waste heat by the design of structural parameters. Despite recent interest in the so-called all-inorganic inks with inorganic binders to engineer viscoelasticity, organic impurities may also be triggered by high portion of organic solvents, which hamper the electron and phonon transport. Herein, we report water-based inks to reduce organic residuals. The quasi-inorganic inks were synthesized by adding Bi2Te3-based particles to water solvent with a few organic binders, whose total organic content is less than that of all-inorganic inks. Moreover, an interface-solder approach is employed to fill the pores among grain particles with the liquefied phase. As a result, there is a tremendous enhancement of ZT values, reaching 0.71 and 0.59 for 3D-printed p- and n-type Bi2Te3-based TE materials, respectively. In particular, the flexible method promotes the realization of waste heat harvesting from an alumina pipe by fabricating a TE module integrated with printed half-annular legs. Our work demonstrates not only the effectiveness of quasi-inorganic inks and interface engineering as a means of increasing ZT values, but also the great potential of 3D-printed Bi2Te3-based TEGs for waste heat recovery.

研究领域: 材料科学 · 能源技术
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Flexible and Printed Electronics · 2024 ·Vol. 9 ·期 2 ·025009 · IF 2.8

A vibrating membrane ejector for direct ink writing of printed electronics

Shangjian Liu,Shuohao Hu,Song Lin,Jiakang Wu,Feng Shao,Junge Liang,Xi Wan,Xiaofeng Gu

Direct ink writing (DIW) represents a technical branch of additive manufacturing technology, particularly suitable for prototyping or small-batch printing production of printed electronic components. However, the existing print heads required for near or sub-100 μm line width are quite sophisticated, limiting the accessibility and application of the DIW method. This paper reports the use of the vibrating membrane ejector (VME) as a new option for the print head of DIW. The structure of the VME-based print head was specially designed for this purpose. Finite element modeling and analysis of the VME's vibration characteristics were performed to provide insights into the ejection conditions and behaviors. The factors influencing the size of printed structures were identified and analyzed through the printing of a metal–organic complex silver (Ag) ink. After optimizing several operational parameters to limit the spreading effects and suppress the satellite droplets, the DIW printed line width has reached about 100 μm. The effectiveness of the VME-based print head was further demonstrated through the DIW fabrication of interdigitated electrodes and microstrip transmission lines. This highlights the versatility of the VME-based print head as a practical tool for device prototyping and ink development in the field of printed electronics.

研究领域: 材料科学 · 印刷电子技术 · 制造工程
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ACS Nano · 2023 · IF 17.1

Multifunctional Microneedle Patches via Direct Ink Drawing of Nanocomposite Inks for Personalized Transdermal Drug Delivery

Yanyan Li,Kerong Chen,Yushuang Pang,Jiaxue Zhang,Ming Wu,Yurui Xu,Shitai Cao,Xinxin Zhang,Shaolei Wang,Yuping Sun,Xinghai Ning,Xiaoliang Wang,Desheng Kong

Additive manufacturing, commonly known as 3D printing, allows decentralized drug fabrication of orally administered tablets. Microneedles are comparatively favorable for self-administered transdermal drug delivery with improved absorption and bioavailability. Due to the cross-scale geometric characteristics, 3D-printed microneedles face a significant trade-off between the feature resolution and production speed in conventional layer-wise deposition sequences. In this study, we introduce an economical and scalable direct ink drawing strategy to create drug-loaded microneedles. A freestanding microneedle is efficiently generated upon each pneumatic extrusion and controlled drawing process. Sharp tips of ∼5 μm are formed with submillimeter nozzles, representing 2 orders of magnitude improved resolution. As the key enabler of this fabrication strategy, the yield-stress fluid inks are formulated by simply filling silica nanoparticles into regular polymer solutions. The approach is compatible with various microneedles based on dissolvable, biodegradable, and nondegradable polymers. Various matrices are readily adopted to adjust the release behaviors of the drug-loaded microneedles. Successful fabrication of multifunctional patches with heterogeneously integrated microneedles allows the treatment of melanoma via synergistic photothermal therapy and combination chemotherapy. The personalized patches are designed for cancer severity to achieve high therapeutic efficacy with minimal side effects. The direct ink drawing reported here provides a facile and low-cost fabrication strategy for multifunctional microneedle patches for self-administering transdermal drug delivery.

CAS / MDL: 9004-35-7
研究领域: 生物医学工程 · 制药科学 · 材料科学
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Micromachines · 2022 ·Vol. 13 ·期 6 ·880 · IF 3.523

A Novel Modification of Copper (II) Phthalocyanine Particles towards Electrophoretic Displays

Yao Wang,Zhi Zhang,Qun Chen,Caihong Ye,Jiahao Zhang,Qingguo Gao,Liming Liu,Jianjun Yang,Xinjian Pan,Yu Miao,Feng Chi,Mingliang Jin

Electrophoretic display (EPD) is a popular display technology in recent years. The core of the EPD is electrophoretic particles, and its Zeta potential has an important impact on EPDs. In this work, a method using pyrrolidine mono ionic liquid was proposed to improve the Zeta potential of electrophoretic particles: Copper (II) phthalocyanine pigment was modified with mono ionic liquid 1-Butyl-1-methylpyrrolidinium bromide. The characterization results show that the mono ionic liquid had been successfully coated on pigment particles. At the same time, the dispersion and stability of particles were improved. The modified Copper (II) phthalocyanine pigment could be stably dispersed in tetrachloroethylene for more than 20 days. The Zeta potential increased from 32.42 mV to 49.91 mV, increasing by 53.95%. Finally, the prepared blue electrophoretic particles were compounded with white titanium dioxide to prepare blue and white dual-color electrophoretic dispersion, and then an EPD cell was designed to test its performance. The results show that the prepared electrophoretic dispersion can realize reversible reciprocating motion. Therefore, because of the unique structure and properties of pyrrolidine mono ionic liquids, the blue nanoparticles prepared with pyrrolidine ionic liquids as charge control agents in this study can be used as excellent candidate materials for EPD.

研究领域: 材料科学 · 显示技术 · 纳米技术 · 化学
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Liquid crystal elastomer-based all-printed actuator and sensing array systems

Ke Zheng,Bin Tian,Panwang Guo,Haoye Zhan,Jing Liang,Youfusheng Wu,Wei Wu

Liquid crystal elastomers (LCEs) are valuable in soft actuators, sensors and other emerging fields. However, it is still a huge challenge to build high-performance LCE-based functional devices in a simple and fast way to achieve the orderly and patterned integration of multiple functional layers and LCE. Herein, screen-printing technology is used to realize the multi-layer pattern deposition of silver fractal dendrites conductive ink (with excellent Joule heating effect and strain-sensing function) and carbon black conductive ink (with photothermal conversion ability) on the surface of LCE. A series of LCE-based electronic devices are prepared through customized printing patterns. The as-obtained actuator possesses excellent electric actuating performance (bending angle of 102° at 200 mA) and self-sensing function (maximum relative resistance changes of −55.0%), and also exhibits NIR light-driven self-sensing bending actuation behavior (bending angle of 81° at 1.43 W/cm 2 ), which can be used to control the robotic arm. The as-printed NIR light sensing array system can accurately sense the intensity, spot size and position of NIR light, showing good application potential in the field of unmanned aerial vehicle flight safety. This work provides a new strategy for the efficient preparation of LCEs-based flexible electronics.

研究领域: 材料科学 · 柔性电子学 · 智能材料
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ACS Applied Materials & Interfaces · 2025 · IF 8.2

MXene/Carboxylated Cellulose Nanofiber Inks for Direct Ink Writing Electromagnetic Interference Shielding, Humidity Sensing, and Joule Heating

Li Xu,Sai Zhao,Peizhu Jiang,Zhiming Deng,Zijie Gao,Peng Min,Fuxin Liang,Zhong-Zhen Yu,Hao-Bin Zhang

Two-dimensional transition metal carbide/nitride (MXene)-based conductive inks are promising in the scalable production of printed electronics and wearable devices. Nevertheless, to realize desirable rheological properties of MXene-based inks and the multifunction of the resulting printed devices is still challenging. Herein, MXene inks with tunable rheological properties were developed by inducing carboxylated cellulose nanofibers (C–CNFs) modifier. The versatile rheological properties of MXene inks facilitate the preparation of MXene gratings by direct ink writing (DIW) and multifunctional devices integrated with electromagnetic interference (EMI) shielding, Joule heaters, and humidity sensors. The highest average EMI shielding effectiveness (SE) is 33.0 dB, with specific EMI SE up to 137481.5 dB cm2 g–1. Meanwhile, when functioning as a Joule heater, a low-voltage drive and excellent cyclic and long-term stability can be observed. In addition, the humidity-sensing function integrated with wireless transmission shows a maximum response value of 2768%. The MXene gratings fabricated by DIW are multifunctional and can be applied to the next generation of wearable devices.

研究领域: 材料科学 · 电子工程 · 纳米技术
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Carbon Letters · 2023 · IF 4.5

Synthesis of multicolor fluorescent CDs from natural plant kaempferide and their application in anti-counterfeiting inks

Ma Linping,Long Xiang,Ma Yanshun,Wu Shaogui

Carbon dots (CDs) are versatile nanomaterials with tunable luminescent properties. We used a natural plant kaempferol as a carbon source to synthesize multicolor CDs by reacting it with various nitrogen sources. Blue, green, and red CDs (B-CDs, G-CDs, and R-CDs) with emission wavelengths of 445 nm, 510 nm, and 600 nm respectively were successfully synthesized. Their photoluminescence quantum yields of are up to 37.4%, 20.1%, and 30.8%, respectively. Surface analysis revealed abundant nitrogen groups influencing luminescence. B-CDs and G-CDs show excitation-dependent emissions, indicating a potential correlation between their luminescence and particle sizes, while R-CDs exhibit excitation-independent emission, suggesting they belong to molecular state CDs. All three CDs exhibit stable luminescent performance, as well as good salt resistance and photobleaching resistance. The practical application of multicolored CDs in anti-counterfeiting fluorescent inks was further explored. This work offers a straightforward, eco-friendly route to synthesize multicolor CDs.

CAS / MDL: 95-54-5 6119-70-6
研究领域: 材料科学 · 化学 · 植物学
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ACS Applied Materials & Interfaces · 2023 · IF 9.5

Paintable Bioactive Extracellular Vesicle Ink for Wound Healing

Li Li,Zhiyu Wang,Kepeng Wang,Siyuan Fu,Dan Li,Mao Wang,Yi Cao,Houjuan Zhu,Ziyan Li,Lixing Weng,Zhiyang Li,Xianguang Ding,Lianhui Wang

The treatment of cutaneous wounds involving complex biological processes has become a significant public health concern worldwide. Here, we developed an efficient extracellular vesicle (EV) ink to regulate the inflammatory microenvironment and promote vascular regeneration for wound healing. The technology, termed portable bioactive ink for tissue healing (PAINT), leverages bioactive M2 macrophage-derived EVs (EVM2) and a sodium alginate precursor, forming a biocompatible EV-Gel within 3 min after mixing, enabling it to be smeared on wounds in situ to meet diverse morphologies. The bioactive EVM2 reprogram macrophage polarization and promote the proliferation and migration of endothelial cells, thereby effectively regulating inflammation and enhancing angiogenesis in wounds. Through integration with a 3D printing pen, the platform enables EV-Gel to be applied to wound sites having arbitrary shapes and sizes with geometric matches for tissue repairment. When evaluated using a mouse wound model, PAINT technology accelerates cutaneous wound healing by promoting the angiogenesis of endothelial cells and the polarization of macrophages to M2 phenotype in vivo, demonstrating the high potential of bioactive EV ink as a portable biomedical platform for healthcare.

CAS / MDL: 90-80-2
研究领域: 生物医学工程 · 组织工程 · 再生医学 · 药理学
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CRYSTAL RESEARCH AND TECHNOLOGY · 2021 ·Vol. 56 ·期 8 ·2100004 · IF 1.639

Crystallization Behavior and Luminescence of Inkjet Printing CH3NH3PbBr3

Rui Sun,Haixia Li,Yimin Guan,Yong Du,Hui Shen,Jiayue Xu

Lead halide perovskites display remarkable optoelectronic properties, like large absorption coefficients, high photoluminescence quantum efficiencies, and long lifetime and diffusion length of photocarriers. This system is easily fabricated using solution processes and inkjet printing is an effective way to prepare halide perovskite films and complex patterns. In this work, the crystallization behaviors of inkjet printing CH 3 NH 3 PbBr 3 crystals are systematically investigated with varied I − doping, printing times, and solvents. Using N , N -dimethylformamide (DMF) solvent, CH 3 NH 3 PbBr 3− x I x ( x = 0, 0.14, 0.29, 0.45, 0.59) are printed on the glass and the crystalline grains are developed from the (001) oriented tetragonal in side length of 10–50 µm to dendrite with increasing I − concentrations. The crystalline grains are kept tetragonal, while the average crystal size changes from 22 to 89 µm by increasing the number of printing from 10 to 1000 times. DMF and dimethyl sulfoxide (DMSO) are used as solvents for printing CH 3 NH 3 PbBr 3 , and more regular grains are obtained from DMF solvent. Several patterns are printed on glass and papers, and fluorescent two-dimensional (2D) patterns are observed under the 480 nm excitation. The as-printed patterns show excellent homogeneity and high reproducibility, indicating that the inkjet printing shows broad application prospects in flexible electronics.

研究领域: 材料科学 · 光学工程
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CARBOHYDRATE POLYMERS · 2022 · IF 10.723

3D printing of all-regenerated cellulose material with truly 3D configuration: The critical role of cellulose microfiber

Rui Yuan,Kai Wu,Qiang Fu

Direct ink writing, as a prospective three-dimensional (3D) printing technique, opens opportunities for offering high freedom to process cellulose into complex shapes. Current challenges are the accomplishment of dimensional accuracy of printed object and its truly 3D configuration, which put stringent requirements to the ink rheology that should be easily flowable under a suitable shear force while can rapidly recover to solid state after the force is removed. In this study, benefiting from the exquisite regulation of residual cellulose microfiber in a dissolved cellulose solution, a remarkable ink with excellent thixotropic property is prepared, which elaborately balance the traditional rheology tradeoff (extrudability and self-supporting) upon the formation of interconnected microfiber network. As a result, the optimized cellulose ink allows the printed object to successfully display arbitrary and truly 3D configurations, such as anatomical heart, ear, rabbit, lamp, and cup, and exhibit fine microstructure with a resolution of 250 μm.

研究领域: 材料科学 · 生物材料
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LANGMUIR · 2019 · IF 3.683

Facile and High-Yield Replacement Reaction-Assisted Synthesis of Silver Dendrites by Jet for Conductive Ink

Muhammad Murtaza,Naveed Hussain,Junchen Liu,Hui Wu

Metallic dendrites with uniform morphology, high purity, and large yield remain challenging to synthesize. In this work, single-crystalline silver (Ag) dendrites with uniform morphology, high purity, and large yield are successfully synthesized by employing single replacement reaction between aqueous silver nitrate (AgNO3) and solid copper (Cu) by jet. The combined effect of diffusion-limited aggregation and the locally oriented attachment of Ag particles is responsible for the formation of silver dendrites under nonequilibrium conditions. Finally, the potential applications of as-synthesized silver dendrites are demonstrated by successfully preparing silver-based conductive ink for flexible electronics and wearable equipment. The conductive pattern exhibits resistivity of 7.2 μΩ·cm, showing good conductivity of the prepared conductive material. This facile and time-efficient synthetic route can be extended to synthesize other noble metal nanostructures with desired morphologies by adopting selective precursor salt concentrations and substrate metals with proper redox potentials.

CAS / MDL: 7761-88-8
研究领域: 材料科学 · 化学合成
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2021 · IF 6.953

Tendon-inspired fibers from liquid crystalline collagen as the pre-oriented bioink

Feng Deng,Yuan Dang,Lele Tang,Tianshuo Hu,Cuicui Ding,Xiaoqing Hu,Hui Wu,Lihui Chen,Liulian Huang,Yonghao Ni,Min Zhang

Nature provides rich bionic resources for the construction of advanced materials with excellent mechanical properties. In this work, inspired by animal tendons, a bionic collagen fiber was developed using collagen liquid crystals as the pre-oriented bioink. The texture of liquid crystalline collagen observed from polarized optical microscopy (POM) showed the specific molecular pre-orientation. Meanwhile, the collagen spinning liquids exhibited a minimal rise in viscosity upon increasing concentration from 60 to 120 mg/mL, indicating the feasible processability . The collagen fiber, which was prepared via wet spinning without being denatured, exhibited the favorable orientation of fibrils along its axis as observed with FESEM and AFM . Thanks to the synergistic effects between pre-orientation and shearing orientation, the maximum tensile strength and Young's modulus of collagen fibers reached 9.98 cN/tex (219.29 ± 22.92 MPa) and 43.95 ± 1.11 cN/tex (966.20 ± 24.30 MPa), respectively, which were also analogous to those of tendon. In addition, the collagen fiber possessed a desirable wet strength . Benefiting from the natural tissue affinity of collagen, the as-prepared bionic collagen fiber possessed excellent wound suture performance and biodegradability in vivo , which offers a new perspective for the potential of widespread applications of collagen fibers in biomedical fields .

研究领域: 生物材料学 · 医学工程
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