Additive manufacturing of wet-spun polymeric scaffolds forbone tissue engineering

聚己内酯药物控释材料的研究进展鲁手涛;徐海荣;刘黎明;曹文瑞;张海军【摘要】综述了聚ε-己内酯(PCL)药物控释材料的研究进展,以及PCL微球、PCL 纳米微粒、PCL纤维、PCL薄膜、PCL胶束、PCL水凝胶的制备方法及应用.PCL 在药物控释领域研究中,可通过与其他聚合物共混或共聚来改善亲水性和控释行为.PCL共聚物也可应用到靶向给药系统中,靶向给药系统不仅能够将药物输送至病灶部位,还能实现定向释放.随着新材料的不断研发,构建新型智能药物控释系统的前景将更加广阔.【期刊名称】《合成树脂及塑料》【年(卷),期】2018(035)004【总页数】5页(P94-98)【关键词】可降解高分子;药物控释;药物载体;聚ε-己内酯;靶向给药【作者】鲁手涛;徐海荣;刘黎明;曹文瑞;张海军【作者单位】生物医用材料改性技术国家地方联合工程实验室,山东省德州市251100;生物医用材料改性技术国家地方联合工程实验室,山东省德州市251100;生物医用材料改性技术国家地方联合工程实验室,山东省德州市251100;生物医用材料改性技术国家地方联合工程实验室,山东省德州市251100;生物医用材料改性技术国家地方联合工程实验室,山东省德州市251100;同济大学介入血管研究所,上海市200072【正文语种】中文【中图分类】TQ323.8药物控释是一种新兴的交叉学科，它可以控制药物在人体内的释放、吸收过程，使药物按照预定的剂量，以一定的模式在体内释放或使药物在指定部位释放。

与传统给药模式相比，控释系统不仅能够减少给药次数，维持血药浓度，提高药物浓度稳定性，还降低了药物的不良反应，提高了药物治疗的有效性［1-2］。

药物载体是控释技术的支撑点，不同性质的载体具有不同的药物释放参数。

可降解高分子药物控释载体具有良好的生物相容性和较高的载药量，而且人体的代谢可以清除它们的降解产物，使可降解高分子成为首选的药物控释载体之一。

可降解高分子载体（如微米和纳米微粒、纤维等），可用于药物运输和靶向药物输送系统［3-5］。

DOI: 10.29026/oea.2018.170004Additive manufacturing frontier: 3D printing electronicsBingheng Lu1, Hongbo Lan2,3* and Hongzhong Liu13D printing is disrupting the design and manufacture of electronic products. 3D printing electronics offers great potential to build complex object with multiple functionalities. Particularly, it has shown the unique ability to make embedded elec-tronics, 3D structural electronics, conformal electronics, stretchable electronics, etc. 3D printing electronics has been considered as the next frontier in additive manufacturing and printed electronics. Over the past five years, a large num-ber of studies and efforts regarding 3D printing electronics have been carried out by both academia and industries. In this paper, a comprehensive review of recent advances and significant achievements in 3D printing electronics is provided. Furthermore, the prospects, challenges and trends of 3D printing electronics are discussed. Finally, some promising so-lutions for producing electronics with 3D printing are presented.Keywords: 3D printed electronics; embedded electronics; 3D structural electronics; additive manufacturingLu B H, Lan H B, Liu H Z. Additive manufacturing frontier: 3D printing electronics. Opto-Electronic Advances1, 170004 (2018).Introduction3D printing (also known as additive manufacturing, AM) is a breakthrough technology that has been developing for more than 30 years, but has attracted more and more attentions in recent years. The American Society for Testing and Materials (ASTM) International defines AM as “A process of joining materials to make objects from 3D model data, usually layer upon layer, as opposed to subtractive manufacturing methodologies”. The seven major additive manufacturing processes as classified per ISO (ASTM F42) are: material jetting, binder jetting, material extrusion, vat polymerization, powder bed fu-sion, direct energy deposition, sheet lamination. With the development of 3D printing (3DP) from rapid prototyp-ing to the end-of-use product manufacturing process, manufacturing constraints have been greatly relieved and the design freedom has been significantly expanded, in-cluding shape complexity, material complexity, hierar-chical complexity, and functional complexity1. In partic-ular, 3D printing has the unique capability to control the point-line-area in geometry and material of each layer for an object at full scale length ranging from micro to mac-ro-scale. The emerging multi-scale and multi-material 3D printing technique possesses great potential to im-plement the simultaneous and full control of fabricated object which involves the external geometry, internal architecture, functional surface, material composition and ratio as well as gradient distribution, feature size ranging from nano, micro, to macro-scale, embedded components and electro-circuit, etc. Therefore, it is able to construct the heterogeneous and hierarchical struc-tured object with tailored properties and multiple func-tionalities which cannot be achieved through the existing technologies. Such technology has been considered as a revolutionary technology and next-generation manufac-turing tool which can really fulfill the “creating material” and “creating life”, especially subvert traditional product design and manufacturing scheme. 3D printing paves the pathway and will result in great breakthrough in various applications for example functional tissue and organ, functionally graded material/structure, lattice materi-al/structure, metamaterial, smart material, functionally embedded electronic component, bio-inspired material/1State Key Laboratory for Manufacturing System Engineering, Xi’an Jiao Tong University, Xi’an 710049, China; 2Qingdao Engineering Research Center for 3D Printing, Qingdao University of Technology, Qingdao 266033, China; 3Nanomanufacturing and Nano-Optoelectronics Lab, Qingdao University of Technology, Qingdao 266033, China* Correspondence: H B Lan, E-mail: hblan99@Received 31 December 2017; accepted 21 January 2018; accepted article preview online 9 February 2018structure, multi-functionality product, soft robot, etc. Furthermore, it may promote the tremendous progress in many subjects involving material, bio-medical, elec-tronics, mechanics, bionics, aerospace, etc 2–8.In last few years, 3D printing has been utilized to fab-ricate electronics and structural electronics. More specif-ically, electronic/electrical components can be deposited and embedded in a 3D structure to form a mul-ti-functionality product by interrupting the 3D printing process. 3D printing promotes the integrated assemblage and embedded other components as results of layer-by- layer or point-by-point characteristics. Functional ele-ments such as sensors, circuits, and embedded compo-nents are now being integrated into 3D-printed products or structures, paving the way for exciting new markets, applications and opportunities. Furthermore, 3D print-ing can be harnessed to print electronics on stretchable and flexible bio-compatible “skins” with integrated cir-cuitry that can conform to irregularly-shaped mounting surfaces. Therefore, 3D printing electronics can offer great potential and unique capabilities to build complex object with multiple functionalities. Particularly, it has shown the unique ability to produce the embedded elec-tronics, 3D structural electronics, conformal electronics, stretchable electronics, OLED, etc 9–16. 3D printing appli-cations have been significantly expanded. 3D printing electronics has been considered as the next frontier in AM. Harrop J , the director of technology research firm IDTechEx, thinks the most promising use of multi mate-rial 3D printing will come in the electronics space. A large number of studies and efforts regarding 3D print-ing electronics have been carried out by both academia and industries. Great progresses in 3D printing electron-ics have been achieved in recent years. This paper mainly presents a comprehensive review of recent progresses in 3D printing electronics. Furthermore, the challenges and prospects of 3D printing electronics are discussed. This paper may provide a reference and direction for the fur-ther explorations and studies of 3D printing electronics.Recent progresses in 3D printing electronicEmbedded electronicsMany researchers have been conducted to add electronic functionality into the 3D printed structures by embed-ding electronic/electrical components and fully encapsu-lating interconnect conductive tracks. The ability of starting or stopping the build at any given layer enables the embedding of electronic components for manufac-turing conformal embedded 3D electronic systems. Tak-ing advantage of the layer-based additive manufacturing method and access to individual layers during fabrication, a single object with multiple materials and embedded components can be built now.Embedded electronics can greatly reduce the mass and assembly complexity due to the elimination of cabled interconnects and redundant electronics packaging. The ability to embed complex functioning components and electronics into 3D printed structures is very crucial for the small-satellite users who are looking to exploit 3DP in a limited space. NASA/GRC (National Aeronautics and Space Administration/Glenn Research Center) and America Makes have performed AM techniques to de-velop the embedded electronics used in the structures of spacecraft. A manufacturing platform, the multi 3D system which integrates two FDM (fused deposition modeling) systems, a CNC (computer numerical control) router for micromachining and a precision dispenser for depositing conductive inks (as shown in Fig. 1), has been developed to produce 3D, multi-material, multifunctional devices (3D-printed CubeSat module) for addressing the re-quirements of aerospace applications. The system can embed wires and components on a multi-material sub-strate to provide mechanical, electronic, thermal and electromagnetic functionality, and making conformal structures with integrated electronics. Figure 2 illustrates the process flow of the multi 3D system and fabricated parts using the platform. A CubeSat Trailblazer inte-grated a 3D-printed structure and the embeddedFig. 1 | (a ,b ) Photograph of the multi 3D system. (c ) Schematic of a fabrication example. Figure reproduced from: (a ) ref. 9, Springer International Publishing AG; (b ) ref. 14, Elsevier Ltd; (c ) ref. 9, Springer International Publishing AG.FDM1FDM2Pneumatic slideBuild platform aStrengthFlame retardancebcelectronics has been successfully launched in 20139,14,17–20. Figure 3 demonstrated the fabrication procedure of a fully encapsulated capacitive sensor. This study provides a proof of concept for advanced fully encapsulated 3D printable devices. It also verified the utility of fully em-bedded bulk conductors interconnect 21.A shoe insole with embedded pressure and tempera-ture sensing circuitry, with wireless communications chip for data transmission was fabricated by mul-ti-material 3D printing, shown in Fig. 4. Using a hybrid 3D printing process, multi-layer tactile sensors including insulating layers and sensing elements have been built. This process enables building a sensor body layer by lay-er, prints sensing elements onto the surface of the body, and builds additional layers. With the combination of ink jet, aerosol jet and extrusion print heads, the depositedmaterial can ranges from one to tens of thousands cps with a wide range of solvents. The case demonstrated the feasibility of fabricating an electronically functional ob-ject through 3D printing 22.Figure 5 shows a 3D “smart cap” with an embedded inductor–a wireless passive sensor, which has beenFig. 2 | (a ) Process flow of the multi 3D system. (b ) Fabricated parts. Figure adapted from ref. 9, Springer International Publishing AG.Build substrate with FDMabMachine channels and cavities for circuitryDispense conductive inkPlace electronic components Join traces and electronic componentsCure conductive inksabdFig. 3 | Fabrication procedure of fully encapsulated capacitive sensor with 3D printing . (a ) Polycarbonate (PC) substrate with recesses designed for all electronic components. (b ) Components arranged in in the PC substrate. (c) Electrical components with corresponding embedded wiring. (d ) Completed capacitive sensor with fully embedded wiring, diodes, LEDs, resistors, and a microcontroller. Figure reproduced from ref. 21, IEEE.cFig. 4 | (a ) Printed wireless pressure and temperature sensor within a shoe's insole. (b ) Pressure and temperature data obtained through wireless communication from the printed insole 22. Figure reproduced from ref. 22, Society for Imaging Science and Technology.Pressure 1 Pressure 2Temperature1200011000100009000T e m p e r a t u r e (d i g i t a l v a l u e )17000 16000 15000 1400013000 12000P r e s s u r e (d i g i t a l v a l u e )0 100200300400 500 600 Time (s)abdemonstrated to monitor the quality of liquid food wire-lessly. The 3D structures including both supporting and sacrificial structures are constructed with a resolution of 30 μm using the FDM technology equipped with a multi-ple-nozzle system. After removing the sacrificial materi-als, silver particles suspensions are injected subsequently and solidified as the metallic elements/interconnects. This may be the first demonstration of a comprehensive manufacture process for printing 3D additive polymer with liquid metal paste filling for the use of potential ap-plications 12.A commercial 3Dn-300 multi-material printer from nScrypt Inc. has been utilized to fabricate a fully embed-ded low-profile antenna. The 3D printer includes dual deposition heads allowing two different kinds of materi-als to be dispensed. The thermoplastic stock is dispensed from one head through a filament extrusion process to print the dielectric components. While the other head prints the ink/paste is printed from the other head with feature sizes of as small as 20 μm to build the conductive elements 23.A hybrid 3D printing process integrating stereolitho-graphy (SL) and direct print (DP) was adopted to pro-duce functional, monolithic 3D structures with embed-ded electronics. The hybrid SL/DP system (as shown in Fig. 6) consists of a 3D Systems SL 250/50 machine and an nScrypt micro-dispensing pump integrated within the SL machine through orthogonally-aligned linear transla-tion stages. The substrate/mechanical structure was fab-ricated by SL while interconnections were made by DP conductive inks. A process was developed to fabricate a 3D electronic device using the hybrid SL/DP machine with the requirement of multiple starts and stops of the SL process, removing the uncured resin from the SL sub-strate, inserting active and passive electronic components, and DP and laser curing of the conductive traces. By curing the conductive traces in situ, the construction of monolithic 3D structural electronic devices can be per-formed without removal of the device from the machine during fabrication. Functional 2D and 3D 555 timer cir-cuits have been fabricated by the hybrid 3D printing sys-tem combined with the proposed process 24. J ang et al. also presented a 3D circuit device fabrication by the hy-brid process of SL and DW technologies. A custom-made SL system was adopted instead of a commercial SL ma-chine 25.Fig. 5 | Fabrication process of 3D “smart cap” with an embedded inductor–a wireless passive sensor . (a ) 3D fabrication process with embedded and electrically conductive structures. (b ) 3D microelectronics components, including parallel-plate capacitors, solenoid-type inductors, and meandering-shape resistors. (c ) A 3D LC tank, which is formed by combining a solenoid-type inductor and a parallel-plate capacitor. (d ) A wireless passive sensor demonstration of a “smart cap”, containing the 3D-printed LC-resonant circuit. (e ) A smart cap with a half-gallon milk package, and the cross-sectional schematic diagram. (f) Sensing principle with the equivalent circuit diagram. Figure reproduced from ref. 12, Macmillan Publishers Limited.aDual 3D printing nozzlesInjection holeLiquid metalInjectionG-S-G padsCapacitorsInductorsResistorsLC tankViaSpiral inductorTop electrodeBottom electrode z yx bcd ReaderSmart capFrequency responseM a g n i t u d e o f S 11f res f res fEnergy RF coilInformationLiquid food qualityR CLfSpiral inductorSmart capViaTop electrodeBottom electrode BottleLiquid foode3D structural electronicsA hybrid technology combined with direct-write/cure (DWC) and projection microstereolithography (PμSL) has been utilized to make 3D structural electronics. A PμSL process was applied to build the 3D structures, and the conductive tracks was produced by the combination of DWC with CNT/polymer nanocomposites, which may capacitate a new generation of inexpensive 3D structural electronics in the field of consumer, defense, and medicalelectronics. The technology of hybrid manufacturing combined with AM technologies will offer capabilities of fully 3D, high-resolution, multimaterial and large-area fabrication as well as requiring only ambient processing conditions (no clean room, vacuum or high temperature environment required). Figure 7 demonstrated the hy-brid 3D printing process and the fabricated 3D structural electronics 10.Disadvantages in the manufacturing process of printedFig. 6 | (a ) Schematic of the hybrid SL/DP system. (b –d ) Fabricated 3D 555 timer circuits packaged within SL substrates. Figure reproduced from: (b –d ) ref. 24, Emerald Publishing Limited. SLA-250Z -axisnScrypt headnScrypt controller PLC controllerY -axisX -axisOptical tableDP computerScanning mirrorSL computer355 nm DPSSlaserLaser beamSL partPlatform SL resin SL vataLEDs bMicrochip Resistor Vertical interconnects Power supplyEmbedded capacitor cdThermistorFig. 7 | The hybrid 3D printing process and fabricated 3D structural electronics . (a ) Bottom insulating structure. (b ) “U” shape wire. (c ) Top insulating layer. (d ) Wires on top surface. (e ) P μSL of the bottom insulating structure. (f ) DWC of the “U” shape wire. (g ) P μSL of the topinsulating structure. (h ) DWC of wires on the top surface. (i ) Fabricated 3D structural electronics with embedded wires. Figure reproduced from ref. 10, Springer International Publishing AG.Projector lens Projected beamDispensing head Conductive material Photocurable materialPhotocurable materialConductive materialf be a cdg hicircuit board include complexity, time consuming, high-er cost, and limited product formation as the printed circuit board must be included. In order to get over these disadvantages, Jiang et al. reported a hybrid process us-ing stereolithography and direct writing (DW) to fabri-cate 3D circuit devices. The insulated structures of circuit boards having high precision were fabricated using SL. Furthermore, the circuits were made on the several layers using DW 25. Lopes et al. also presented a similar manu-facturing system using SL and DW technologies for the fabrication of 3D structural electronics 24.The integration of SL in combination with both microdispensing (nozzle deposition) and pick-and-place technology (component insertion) can produce dielectric substrates of intricately-detailed, complex shape where miniature cavities are used for the integration of press-fit electronic components. Printed conductive traces serve as electrical connections deposited by an integrated mi-cro-dispensing system within the SL system and this combination of fabrication technologies stands to revo-lutionize the integration of electronics within mechanical structures as ‘‘3D structural electronics’’. Wicker and MacDonald demonstrated the development of multiple material and multiple technology SL systems capable of manufacturing multiple material structures with me-chanical, electrical, and biochemical functionality. Some functional objects including multi-material tissue engi-neered implants, multi-material micro-scale parts, 3D structural electronics, have been successfully fabricated.Contamination issues associated with using multiple viscous materials in a single build, throughput, and lim-ited materials as well as conductive inks with low-temperature curing capabilities remain still a chal-lenging. Figure 8 shows some examples of printed 3D structural electronics 18,24.Stretchable electronicsWith the development of electronics, progresses in man-ufacturing techniques have promoted the development in the aspects of smaller, faster, more efficient. So far, the main focus has been on rigid electronics. However, re-cent interest in devices such as wearable electronics and soft robotics has led to an whole new set of electronic devices–stretchable electronics. These new devices re-quire new manufacturing solutions to integrate hetero-geneous soft functional materials. 3D printing can be harnessed to print electronics on stretchable and flexible bio-compatible “skins” with integrated circuitry that can conform to irregularly-shaped mounting surfaces.Muth et al. reported a method of embedded 3D print-ing (e-3DP) for the fabrication of strain sensors, as shown in Fig. 9. In this method, a viscoelastic ink is ex-truded into an elastomeric reservoir via a deposition nozzle. The ink is used as a resistive sensing element, while the reservoir form the matrix material. A capping (filler fluid) layer is used to fill the void space formed in the process of the nozzle translating through the reser-voir. Finally, a monolithic part was formed by theFig. 8 | Examples of printed 3D structural electronics . (a ) A gaming die which includes a microcontroller and accelerometer. (b , c ) A magnetometer system with microprocessor and orthogonal Hall Effect sensors. Figure reproduced from ref. 18, Taylor & Francis.5 mma5 mm5 mmb cFig. 9 | Schematic illustration of the embedded 3D printing (e-3DP) process and printed stretchable electronics . (a ) Schematicillustration of the e-3DP process. (b ) Photograph of a glove with embedded strain sensors produced by e-3DP. (c ) Photograph of a three-layer strain and pressure sensor in the stretched state. Figure reproduced from ref. 11, WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.Printing directionabcFiller fluidco-cure of both the reservoir and filler fluid, which cov-ered and keep the embedded conductive ink fluid. The e-3DP can create soft sensors in a highly programmable and seamless manner. In order to enable e-3DP, a multi-component materials system composed of an ink, reser-voir, and filler fluid was developed. The above method that for building highly stretchable sensors by e-3DP opens new approaches for manufacturing soft functional devices for wearable electronics, human/machine inter-faces, soft robotics, and so on 11.The ability of printing integrated circuits on the flexi-ble substrate enables the electronic devices with con-formity, lightweight structure and shock-resistant con-struction, which are challenging to be achieved by using rigid substrates such as semiconductor wafers and glass plates. Bijadi et al. have successfully tested the feasibility of a syringe extrusion-based 3D printing process to print stretchable embedded electronics through the use of SS-26S conductive silicone on flexible non-conductive silicone substrates. Instead of merely using the conduc-tive silicone traces as flexible interconnects, this method used the conductive material for creating complete cir-cuitry with SMT components and embedded microcon-trollers 26. Vatani et al. presented a hybrid manufacturing process including direct print/cure (DPC) and projec-tion-based stereolithography for stretchable tactile sen-sors. The fabrication process of the tactile sensor (shown in Fig. 10) includes building the sensor body, printing sensing elements on the body surface, and building some additional layers to cover the cured sensing elements 27. The developed 3D printable stretchable sensing material is a photocurable and stretchable liquid resin filled with multi-walled carbon nanotubes (MWNTs).Other electronic/electrical products and related technologies3D printing possesses the ability of creating complex and conformal electronics integrated within a manufactured product. The Aerosol J et printing from Optomec has been demonstrated the ability of building the functional antennae on the conformal 3D printing substrates. The whole printing process accurately controls the location, geometry and thickness of the deposit and produces a smooth mirror-like surface finish to insure optimumFig. 10 | Fabricated stretchable tactile sensor using integrated PSL and DP processes . (a ) An example (partial sphere) of 3D structure built in the PSL system. (b ) Printed sensing elements using the DP process on the insulating layers built in the PSL system. (c ) Final sensor with two sensing layers. (d ) Deformed sensor. Figure reproduced from ref. 27, Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.abcdFig. 11 | 3D printed electronics using Aerosol Jet printing from Optomec . (a ) 3D MID demonstrator. (b ) 3D MID with integrated sensor. (c ) Printed conformal electronics (curve). (d ) Printed conformal electronics (dome). (e ) Printed conformal electronics (dome). (f) Sub-mm lengthscale, custom made 3D metal-dielectric. Figure reproduced from (a –c ) ref. 28, Neotech; (d –f ) ref. 29, Optomec.d e a b cfantenna performance. Some kinds of mobile device an-tennas, such as the LTE, NFC, GPS, Wifi, WLAN, and BT, have been printed through the Aerosol J et process. And the performance of such antennas tested by a cell phone component supplier is in the same level with other production methods. For now, the Aerosol Jet technolo-gy has been using for the mass production of printed 3D conformal electronics in the application of antenna and sensor. As can been seen that a hybridized DW/AM pro-cess presents great potential for creating antennas with 3-dimensional structure. Figure 11 demonstrated 3D printed electronics using Aerosol Jet printing process 28–29. Aerosol J et printing process has the ability to print conformal interconnects on 3D surfaces eliminating the need for wire bonding – for example printing electrical connections on 3D stacked die or for LED chip fabrica-tion. Runge showed Leg prosthesis part produced from PLA (Polylactic Acid) via FDM showing complexnon-planar surfaces, with surface-integrated strain gauge sensors produced by Aerosol J et TM printing and con-ductive paths deposited via micro-dispensing, both using the modular manufacturing platform. The structural elements of this leg prosthesis shaft were produced via the FDM process from PLA, a thermoplastic polymer. Its functionalization relies on a surface-integrated strain gauge realized via Aerosol J et printing. The conductive paths that lead across the part as well as the contact pads at their end were deposited through micro-dispensing. The material of the resistive sensor is a silver based ink, while interconnects and contact pads are made from sil-ver particle-filled epoxy, as shown in Fig. 12 31.The first multi-material 3D electronics printer in the world, named as Voxel8, provides an all-in-one, desktop solution for designing and prototyping next generation 3D electronic devices. Therefore, it has been regarded as a disruptive manufacture platform with the capabilities of printing embedded electronics. It enables prototyping of 3D electronic devices by the method of co-printing both thermoplastics and a highly conductive silver ink, which can be printed and cured at ambient temperature without the need for thermal annealing. Figure 13 demonstrates Voxel8 and some printed products 32.Prospect, challenges and future trends3D printing is disrupting the design and manufacture of electronic products. Functionalities of the devic-es/products fabricated by 3D printing can be significantly expanded by incorporating electronic components, such as sensors and circuits, in predetermined cavities within fabricated structures. 3D printed objects include not only traditional mechanical characteristics, but also embedded optical and electrical functions, such as sensor; all com-plex structures are difficult to produce with existingFig. 13 | Voxel8 and some printed products . (a , b ) Photograph of Voxel8 3D printer. (c ) Printed unmanned aerial vehicle. (d ) Printed antenna (dome). (e ) Printed wearable device. Figure reproduced from ref. 32, Voxel8.bac d eFig. 12 | Leg prosthesis part produced by FDM and Aerosol Jet printing . Figure reproduced from ref. 31, University of Applied Science Bremerhaven.manufacturing methods. Many emerging and innovative products, such as embedded electronics, 3D structural electronics, conformal electronics, stretchable electronics, etc., have been fabricated using the technologies. 3D printing electronics has been considered as the next fron-tier in AM. Optomec has developed a high volume printing solution for the production of 3D antenna and 3D sensors that are tightly integrated with an underlying product ranging from smartphones to industrial com-ponents. It can be utilized for high volume printing of conformal sensors and antennas directly onto preformed 3D structures. Complex electronics can be 3D printed at micron resolution which will enable cheaper smartphones and medical gadgets. Aerosol J et 3D mi-cro-structure printing is capable of ultra-high resolutions with lateral features sizes of 10 μm and aspect ratios of more than 100:1 33–37.The conductivity is still one of the major difficulties in both 3D printed electronics and general 2D printed elec-tronics because of the poor conductivity of ink caused by the low curing temperature due to the limitation of sub-strate material such as cardboard, polymers. More and more challenges in the fields of material types and pro-cessing challenges in the process of printing from 2D electronics to 3D integrated objects. Therefore, the com-patible material sets should be explored and created to provide the adequate functionality and manufacturability for the product invention by designers. Besides, the ad-hesion between the materials is also a big issue, because the conductive materials would be stripped from the substrate with a poor adhesion. This is especially im-portant case for traces that are embedded within a print and not on the surface because repair is impossible after a circuit is embedded.In order to make electronics with 3D printing, new processes should be developed to possess the ability of depositing broader types of materials. To date, there are several solutions which have the ability to fabricate mul-tifunctional 3D structures or products with embedded functional systems. Compared to other methods, the hybrid process combining FDM and direct print/writing shows higher applied potential, more flexibility. Material jetting systems seem currently to be the most successful multi-material 3D printing process among AM technol-ogies. To date, fabrication of true 3D multiple material polymeric components using material jetting processes has been demonstrated. Currently, material jetting of polymers appears to be the nearest approximation to this vision that is currently available: The combination of high resolution, controlled material deposition with the possibility of photo polymerization, which allows imme-diate solidification of the material after printing and thus facilitates deposition of materials with different func-tional or structural roles directly besides each other, pro-vides the foundation for effectively printing a structural electronics system directly. Multi-material and mul-ti-scale 3D printing will be the most promising solutions. More and more 3D printed functional electronics and products with electronics will be fabricated. 3D printing electronic technology provides a powerful tool for inno-vative product development, and extends 3D printing multiple functionalities. Significant advances in 3D printing electronics have been accomplished in the re-cent years. 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温敏水凝胶的英语The English Composition on Thermo-Sensitive HydrogelsThermo-sensitive hydrogels have gained significant attention in the field of biomedicine due to their unique properties and potential applications. These intelligent materials possess the ability to undergo reversible phase transitions in response to changes in temperature, making them particularly useful in various biomedical applications.Hydrogels are a class of hydrophilic polymeric networks that can absorb and retain large amounts of water or biological fluids within their three-dimensional structure. Thermo-sensitive hydrogels, specifically, exhibit a temperature-dependent phase transition, which means they can undergo a sol-gel transition as the temperature changes. This property is often referred to as the lower critical solution temperature (LCST) or upper critical solution temperature (UCST), depending on the specific polymer system.One of the most well-known thermo-sensitive hydrogels is poly(N-isopropylacrylamide) (PNIPAAm), wh ich has an LCST around 32°C, close to the human body temperature. Below the LCST, PNIPAAmhydrogels are in a swollen, hydrophilic state, allowing for the incorporation and release of various therapeutic agents. However, as the temperature increases above the LCST, the polymer chains undergo a conformational change, leading to the collapse of the hydrogel structure and the expulsion of water. This temperature-induced phase transition makes PNIPAAm-based hydrogels particularly useful for controlled drug delivery applications.The mechanism behind the temperature-responsive behavior of thermo-sensitive hydrogels, such as PNIPAAm, is related to the delicate balance between hydrophobic and hydrophilic interactions within the polymer network. At temperatures below the LCST, the polymer chains are hydrated, and the hydrogen bonding between water molecules and the polymer's amide groups dominates, leading to a swollen, hydrophilic state. As the temperature increases above the LCST, the hydrogen bonding between water and the polymer becomes weaker, and the hydrophobic interactions between the isopropyl groups of the polymer become more prominent. This results in the collapse of the polymer chains, causing the expulsion of water and the formation of a more compact, hydrophobic structure.The unique temperature-responsive behavior of thermo-sensitive hydrogels has led to their widespread application in various biomedical fields. One of the primary applications is in controlleddrug delivery systems. Thermo-sensitive hydrogels can be used as carriers for therapeutic agents, such as small-molecule drugs, proteins, or even cells. These hydrogels can be designed to release the encapsulated drugs in a controlled manner by responding to the temperature changes in the body. For example, a PNIPAAm-based hydrogel loaded with a drug can be administered in a liquid state at room temperature and then undergo a phase transition to a gel state upon reaching body temperature, effectively trapping the drug within the hydrogel matrix. As the temperature increases further, the hydrogel can undergo a volume phase transition, leading to the release of the drug in a controlled manner.Another important application of thermo-sensitive hydrogels is in tissue engineering and regenerative medicine. These hydrogels can be used as scaffolds for cell growth and tissue regeneration. The temperature-responsive nature of the hydrogels allows for easy administration and in situ gelation, which can facilitate the encapsulation of cells or the delivery of growth factors directly to the site of injury or disease. The hydrogel scaffold can then provide a suitable microenvironment for cell proliferation, differentiation, and tissue formation.Thermo-sensitive hydrogels have also found applications in wound healing and burn treatment. The ability of these hydrogels to undergo a sol-gel transition in response to temperature changes canbe exploited to create wound dressings that can be easily applied in a liquid form and then transition to a gel state upon contact with the body. This can help maintain a moist environment, promote wound healing, and prevent infection.Furthermore, thermo-sensitive hydrogels have been investigated for use in various diagnostic and sensing applications. For instance, they can be designed to incorporate responsive elements, such as enzyme-substrate pairs or antibody-antigen interactions, which can trigger a detectable change in the hydrogel's physical properties in response to the presence of specific analytes or biomarkers.The development of thermo-sensitive hydrogels has also led to advancements in the field of injectable biomaterials. These hydrogels can be designed to be injected in a liquid form and then undergo in situ gelation at the target site, allowing for minimally invasive procedures and the delivery of therapeutic agents or cells directly to the site of interest.Despite the numerous promising applications of thermo-sensitive hydrogels, there are still several challenges that need to be addressed. One of the key challenges is the optimization of the LCST or UCST to match the specific requirements of the target application. Researchers are exploring ways to fine-tune the polymer composition and structure to achieve the desired temperature-responsive behavior. Additionally, the long-term biocompatibility and biodegradability of these hydrogels need to be thoroughly investigated to ensure their safe and effective use in biomedical applications.In conclusion, thermo-sensitive hydrogels have emerged as a versatile class of biomaterials with tremendous potential in the field of biomedical engineering. Their temperature-responsive behavior, coupled with their ability to encapsulate and deliver therapeutic agents, make them a promising platform for a wide range of applications, from controlled drug delivery to tissue engineering and regenerative medicine. As research in this field continues to advance, we can expect to see even more innovative and impactful applications of thermo-sensitive hydrogels in the years to come.。

Vol. 35 No. 1功 能 高 分 子 学 报2022 年 2 月Journal of Functional Polymers93文章编号： 1008-9357(2022)01-0093-08DOI: 10.14133/ki.1008-9357.20210322002温度响应型酰腙可逆共价键水凝胶的制备及性能何 元1， 罗媛媛2， 刘 通1， 张银山1， 郭赞如1， 章家立1（1. 华东交通大学材料科学与工程学院，高分子材料与工程系，南昌 330013；2. 重庆市计量质量检测研究院，重庆 401120）摘 要： 首先，通过可逆加成-断裂转移（RAFT）聚合制备了丙烯酰胺（AM）、双丙酮丙烯酰胺（DAAM）和N-异丙基丙烯酰胺（NIPAM）的共聚物（PAM-co-PDAAM-co-PNIPAM）；然后，使PAM-co-PDAAM-co-PNIPAM与己二酸二酰肼（ADH）反应后，得到了具有温度和pH双重响应性的水凝胶。

通过核磁共振氢谱（1H-NMR）和凝胶渗透色谱（GPC）、流变仪、扫描电镜（SEM）以及傅里叶变换红外光谱（FT-IR）对共聚物和水凝胶的结构和组成，以及水凝胶的温度和pH双重响应行为进行了研究。

研究表明，该水凝胶具有温度调控的自愈合性，对药物阿霉素（Dox）表现出pH和温度双重响应的可控释放行为。

关键词： 智能水凝胶；酰腙可逆共价键；自愈合；温度响应中图分类号： O633 文献标志码： APreparation and Properties of Temperature-Responsive HydrogelsBased on Acylhydrazone Reversible Covalent BondsAll Rights Reserved.HE Yuan1, LUO Yuanyuan2, LIU Tong1, ZHANG Yinshan1, GUO Zanru1, ZHANG Jiali1（1. Department of Polymer Materials and Engineering, School of Materials Science and Engineering, East China JiaotongUniversity, Nanchang 330013, China; 2. Chongqing Academy of Metrology andQuality Inspection, Chongqing 401120, China）Abstract: A series of PAM-co-PDAAM-co-PNIPAM copolymers were synthesized by reversible addition fracture transfer(RAFT) polymerization from acrylamide (AM), diacetone acrylamide (DAAM) and N-isopropylacrylamide (NIPAM). Theirstructure and composition were characterized by Nuclear Magnetic Resonance (NMR) and Gel Permeation Chromatography(GPC). Hydrogel with pH and temperature dual-response formed by the acyl hydrazone dynamic bonds between ketocarbonylin polymer and hydrazide in adipic dihydrazide (ADH). The dual-responsive behavior of hydrogels to temperature and pHwas researched by rheological measurement, Scanning Electron Microscope (SEM) and Fourier Transform Infrared (FT-IR)spectroscopy. At the same time, the hydrogel demonstrated temperature controlled self-healing properties. Besides, thehydrogels showed pH-and temperature-responsive controlled release behaviors for doxorubicin(Dox).Key words: smart gel； acylhydrazone dynamic covalent bond； self-healing； temperature response收稿日期： 2021-03-22基金项目： 国家自然科学基金（21802041，51563009，21865009）；江西省杰出青年基金（20202ACBL214001）作者简介： 何 元（1994—），男，硕士，主要研究方向为功能高分子材料。