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ACS Sustainable Chemistry & Engineering · 2019 · IF 6.97

Intelligent Icephobic Surface toward Self-Deicing Capability

Fatang Liu,Zhikui Wang,Qinmin Pan

Superhydrophobic surfaces show attractive anti-icing properties. However, it remains a challenge for them to achieve icephobicity and ultralow ice adhesion in a humid environment, which is fundamentally attributed to the icing behavior on their hierarchical textures. Here, we address the issue by integrating a superhydrophobic copper mesh with an intelligent organogel that can secrete antifreezing agent autonomously in response to temperature. The antifreezing agent is composed of ethylene glycol and water. By autonomously secreting the antifreezing agent at subzero temperatures, the hybrid surface effectively inhibits the frosting process on the hierarchical texture of the superhydrophobic mesh. Consequently, the surface not only exhibits excellent antifrosting properties in a humid atmosphere but also repeatedly removes the ice deposited spontaneously due to ultralow ice adhesion (8 Pa). This integration of intelligent organogel paves a new and promising avenue to design superhydrophobic surfaces with excellent icephobic properties.

研究领域: 材料科学 · 表面工程 · 化学工程
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2020 · IF 7.489

Environmentally stable, photochromic and thermotropic organohydrogels for low cost on-demand optical devices

Zhuo Zhang,Luxuan Guo,Xiaolai Zhang,Jingcheng Hao

Hypothesis The color-changing ability of creatures widely existed in nature has inspired the development of adaptive allochroic materials, which can respond to various external stimuli. Integrating multi-stimuli responsiveness and long-term stability in allochroic system are urgent for practical applications under complex circumstances. Experiments The photochromic/thermotropic organohydrogels (PTOs) comprised polyacrylamide and cationic cellulose (JR400) were prepared by facile free-radical polymerization and glycerol displacement. The coexisting covalent bonds and noncovalent interactions collaboratively reinforce the networks, endowing the PTOs with boosted stretchability and toughness. Findings The photochromic ammonium molybdate (Mo 7 ) and thermo-sensitive poly(ethylene oxide)-poly(propylene oxide)-poly(ethylene oxide) (EPE) were made into networks. In these cooperative networks, each constituent performed their own function without disruption, including fast photochromism (10 s) and durable thermo-responsiveness. Importantly, the glycerol-water solvent bestowed the distinct anti-freezing (-30 °C) and anti-dehydration performances on the PTOs. Accordingly, the materials could serve as promising rewritable devices for high-resolution and long-term data storage/encryption. Moreover, on-demand PTO windows integrating UV-prevention and solar energy regulation with T lum (92.96%) and ΔT sol (46.02%) could create comfortable and healthy environments for occupants. This work offers a new design strategy for low-cost, environmentally stable smart optical devices .

研究领域: 材料科学 · 环境科学
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CHEMICAL ENGINEERING JOURNAL · 2019 · IF 8.355

Biocompatible, self-wrinkled, antifreezing and stretchable hydrogel-based wearable sensor with PEDOT:sulfonated lignin as conductive materials

Qinhua Wang,Xiaofeng Pan,Changmei Lin,Dezhi Lin,Yonghao Ni,Lihui Chen,Liulian Huang,Shilin Cao,Xiaojuan Ma

Gel-based strain sensors have great potential in the fields of motion detection and real-time healthcare. Nevertheless, the relatively low strain sensitivity and inferior anti-freezing property limit the utilization of these sensors. In this work, a novel multifunctional organohydrogel sensor was developed based on a poly (acrylic acid) (PAA) skeleton with poly (3,4-ethylenedioxythiophene): sulfonated lignin (PEDOT:SL) as the conductive material and a water/glycerol binary solvent as the dispersion medium. The conductive, self-wrinkled, soft and elastic properties endue the organohydrogel sensor with a superior gauge factor (GF) of up to 7 (strain: 100%), while the freezing tolerance of the water/glycerol solvent endows the organohydrogel with an excellent anti-freezing property. The organohydrogel sensor senses not only the movement of limbs, but also a weak pulse and throat vibrations. Moreover, physiological signals such as those used for electrocardiography (ECG) and electromyography (EMG) can be readily detected. In addition, the cell culture test shows that the organohydrogel is nontoxic, and the animal experiments demonstrate that the organohydrogel can protect skin from frostbite. Overall, this work presents a new concept to use lignin for conductive PEDOT polymerization and integrates the fabrication of conductive organohydrogel materials for precise strain sensing.

研究领域: 生物医学工程 · 材料科学
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2021 · IF 6.953

Preparation of stretchable and self-healable dual ionically cross-linked hydrogel based on chitosan/polyacrylic acid with anti-freezing property for multi-model flexible sensing and detection

Yongzhi Liang,Yuexin Shen,Xingyue Sun,Haiyi Liang

As a kind of promising material for flexible wearable electronics, conductive hydrogels have attracted extensive interests of researchers for their inherent merits such as superior mechanical properties, biocompatibility, and permeability. Herein, we constructed a new type of highly stretchable, anti-freezing, self-healable, and conductive hydrogel based on chitosan/polyacrylic acid. The large amount of ions inside the network had five functions for the proposed hydrogel, including excellent mechanical behaviors, high conductivity, self-recovery, self-healing and anti-freezing capability. Consequently, the proposed hydrogel possessed tunable stretchability (1190–1550%), tensile strength (0.96–2.56 MPa), toughness (5.7–14.7 MJ/m 3 ), superior self-healing property (self-healing efficiency up to 83.7%), high conductivity (4.58–5.76 S/m), and excellent anti-freezing capability. To our knowledge, the self-healable hydrogel with balanced tensile strength, toughness, conductivity, and low-temperature tolerance can hardly be achieved till now. Furthermore, the conductive hydrogels exhibited high sensitivity (gauge factor up to 10.8) in a broad strain window (0–1000%) and could detect the conventional motion signals of human body such as bending of a knuckle, swallowing, and pressure signal at both room temperature and −20 °C. Moreover, the hydrogels could also be fabricated as flexible detectors to identify different temperatures, different kinds of solutions, and different concentrations of the solution.

CAS / MDL: 7783-20-2 13520-92-8
研究领域: 材料科学 · 生物医学工程
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BIOMACROMOLECULES · 2022 · IF 6.978

Gelatin-Reinforced Zwitterionic Organohydrogel with Tough, Self-Adhesive, Long-Term Moisturizing and Antifreezing Properties for Wearable Electronics

Lilong Cao,Zhijie Zhao,Junjie Li,Yunfeng Yi,Yuping Wei

Strong mechanical performance, appropriate adhesion capacity, and excellent biocompatibility of conductive hydrogel-based sensors are of great significance for their application. However, conventional conductive hydrogels usually exhibit insufficient mechanical strength and adhesion. In addition, they will lose flexibility and conductivity under subzero temperature and a dry environment owing to inevitable freezing and evaporation of water. In this study, a tough, flexible, self-adhesive, long-term moisturizing, and antifreezing organohydrogel was prepared, which was composed of gelatin, zwitterionic poly [2-(methacryloyloxy) ethyl] dimethyl-(3-sulfopropyl) (PSBMA), MXene nanosheets, and glycerol. Natural gelatin was incorporated to enhance mechanical performance via the entanglement of a physical cross-linked network and a PSBMA network, which was also used as a stabilizer to disperse MXene into the organohydrogel. Zwitterionic PSBMA endowed the organohydrogel with good adhesion and self-healing properties. Long-term moisturizing properties and antifreeze tolerance could be achieved owing to the synergistic water retention capacity of PSBMA and glycerol. The resulting PSBMA–gelatin–MXene–glycerol (PGMG) organohydrogel exhibited high mechanical fracture strength (0.65 MPa) and stretchability (over 1000%), excellent toughness (3.87 MJ/m3), strong and repeated adhesion to diverse substrates (e.g., paper, glass, silicon rubber, iron, and pig skin), good fatigue resistance (under the cyclic stretching–releasing process), and rapid recovery capacity. Moreover, the PGMG organohydrogel showed good stability under −40 °C. The sensor based on PGMG organohydrogel could tightly attach to the human skin and real-time-monitor the motions of joints (e.g., bending of the finger, wrist, elbow, and knee) and the change in mood such as smiling and frowning. Therefore, PGMG organohydrogels have a huge potential for wearable sensors under room temperature or extreme environments.

研究领域: 材料科学 · 生物医学工程
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ACS Applied Materials & Interfaces · 2022 · IF 10.383

Highly Sensitive Zwitterionic Hydrogel Sensor for Motion and Pulse Detection with Water Retention, Adhesive, Antifreezing, and Self-Healing Properties

Yanqing Wang,Picheng Chen,Xinjie Zhou,Yuetao Liu,Ning Wang,Chuanhui Gao

The design and synthesis of conductive hydrogels with antifreezing, long-term stable, highly sensitive, self-healing, and reusable is a critical procedure to enable applications in flexible electronics, medical monitoring, soft robotics, etc. Herein, a novel zwitterionic composite hydrogel possessing antifreezing, fast self-healing performance, water retention, and adhesion was synthesized via a simple one-pot method. LiCl, as an electrolyte and antifreeze, was promoted to dissociate under the electrostatic interaction with zwitterions, resulting in the composite hydrogels with high electrical conductivity (7.95 S/m) and excellent antifreeze ability (−45.3 °C). Meanwhile, the composite hydrogels could maintain 97% of the initial water content after exposed to air (25 °C, 55% RH) for 1 week due to the presence of salt ions. Moreover, the active groups of zwitterions could form conformal adhesion between the composite hydrogels and skin, which was particularly crucial for the stable signal output of the sensor. The dynamic borate ester bonds, active group of zwitterions, and the hydrogen bond between different components could achieve rapid self-healing (2 h, self-healing efficiency to 97%) without any external intervention. Notably, the developed PBAS-Li (poly(vinyl alcohol) Borax/acrylamide/zwitterionic-LiCl) hydrogel not only succeeded in sensitively detecting human motions but also could precisely captured handwritings signals and subtle pulse waves on the neck and wrist. The above findings demonstrated the great potential of PBAS-Li hydrogels in the field of flexible electronic devices.

研究领域: 材料科学 · 生物医学工程 · 柔性电子
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ACS Applied Polymer Materials · 2023 · IF 5

High Adhesive Force, Wide Temperature Adaptability Thermochromic Ionogel Smart Window

Shengping Dai,Xu Dong,Yaoyao Jiang,Jun Ge,Jianning Ding,Ningyi Yuan

Traditional thermochromic hydrogels have attracted much attention in the field of smart windows, but they still have some problems of temperature adaptability, such as easy freezing, water evaporation, etc. Here, a dynamic physically cross-linking network structure ionogel was constructed by an ionic liquid ([BMIm]+[BF4]−) with low vapor pressure, which has outstanding mechanical properties (670%, 89.5 kPa), antifreezing properties, and strong adhesion properties (under water and at high and low temperatures). Due to the repositionable phase separation caused by the internal hydrogen bonds, the ionogel exhibited transmittance changes of up to 72% in the range of 0 °C ∼ 60 °C, excellent optical stability, and thermochromic ability during the heating–cooling cycles. Furthermore, the ionogel was used as the active layer of the smart window, which could change the light transmittance of the window in real-time according to the outdoor temperature and then realize the indoor temperature adjustment to achieve the energy saving and emission reduction. This study provides a promising strategy for developing an ionogel smart window with wide temperature adaptability.

CAS / MDL: 141-32-2 9003-49-0
研究领域: 材料科学 · 能源与环境科学
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ACS Applied Materials & Interfaces · 2023 · IF 9.5

Highly Sensitive Temperature Detection Based on a Frost- and Dehydration-Resistive Ion-Doped Hydrogel-MXene Composite

Zeyi Wang,Xuejie Zou,Zhiwei Yang,Jian Wang,Qian Chen,Chengjie Pei,Zhiwei Wang,Mengwei Dong,Jian Zhang,Hai Li,Xiao Huang

Wearable temperature sensors with high sensitivity and stability hold great potential for human health monitoring. However, hydrogels, which are commonly used for wearable devices, often show poor thermal and electrical conductivity and are susceptible to dehydration and freezing. Herein, we developed a frost- and dehydration-resistive temperature sensor based on Fe2+/Ti2CTx/κ-carrageenan (CA)-polyacrylamide (PAM) hydrogel. The Fe2+ ions within the hydrogel existed in two forms: as free ions and bonded ions. The free Fe2+ ions could complex with water molecules, resulting in the improved resistance to dehydration and freezing, as well as enhanced ionic conductivity in the hydrogel. On the other hand, the remaining Fe2+ ions acted as linkers to form coordination bonds with the sulfate groups of CA chains, resulting in the greatly enhanced mechanical strength of the hydrogel. In addition, the Ti2CTx nanosheet-based fillers formed a well-defined porous laminar structure, which reduced the phonon scattering and improved the phonon adsorption within the hydrogel. The Fe2+/Ti2CTx/CA-PAM hydrogel sensor exhibited excellent temperature sensing performance including a good linearity (R2 = 0.998) within a broad working range (−10 to 60 °C), high resolution (0.1 °C), and good repeatability. Furthermore, the sensor was integrated into a wireless system for continuous monitoring of body temperature, demonstrating its potential in healthcare monitoring, electronic skins, and intelligent robots.

研究领域: 材料科学 · 生物医学工程 · 电子皮肤
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2023 · IF 8.2

Tremella polysaccharide-based conductive hydrogel with anti-freezing and self-healing ability for motion monitoring and intelligent interaction

Xiaokun Han,Tianyun Lu,Zuocai Zhang,He Wang,Shaorong Lu

The application of conductive hydrogels in flexible wearable devices has garnered significant attention. In this study, a self-healing, anti-freezing, and fire-resistant hydrogel strain sensor is successfully synthesized by incorporating sustainable natural biological materials, viz. Tremella polysaccharide and silk fiber, into a polyvinyl alcohol matrix with borax cross-linking. The resulting hydrogel exhibits excellent transparency, thermoplasticity, and remarkable mechanical properties, including a notable elongation (1107.3 %) and high self-healing rate (91.11 %) within 5 min, attributed to the dynamic cross-linking effect of hydrogen bonds and borax. A strain sensor based on the prepared hydrogel sensor can be used to accurately monitor diverse human movements, while maintaining exceptional sensing stability and durability under repeated strain cycles. Additionally, a hydrogel touch component is designed that can successfully interact with intelligent electronic devices, encompassing functions like clicking, writing, and drawing. These inherent advantages make the prepared hydrogel a promising candidate for applications in human health monitoring and intelligent electronic device interaction.

CAS / MDL: 9002-89-5
研究领域: 材料科学 · 生物医学工程
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FOOD AND CHEMICAL TOXICOLOGY · 2019 · IF 3.775

Effects of gelatin-based antifreeze peptides on cell viability and oxidant stress of Streptococcus thermophilus during cold stage

Xu Chen,Ling Li,Fujia Yang,Jinhong Wu,Shaoyun Wang

Cold stage adversely affects cell proliferation and cell viability of probiotics such as Streptococcus thermophilus in food industry, new type of cryoprotectants continues to be needed. Gelatin-based antifreeze peptide becomes a popular topic because of its cryoprotective effects on cold-stressed probiotics. In this study the effects of tilapia scales antifreeze peptides (TSAPP) on cell viability and oxidant stress of S. thermophilus during cold stage were investigated. The results showed that the percentage of viable cells was increased 10.85 folds compared with control groups. Addition of TSAPP activated the activities of ATPases, relieved the hyperpolarization of cell membrane potential and regulated the intracellular Ca 2+ concentration. Furthermore, TSAPP significantly inhibited reactive oxygen species level and malonaldehyde content in cells. Under cryopreservation with TSAPP, cells of S. thermophilus maintained higher activities of antioxidant enzymes including catalase , peroxidase and total antioxidant capacity . These findings indicate that TSAPP likely offered its cellular protection by maintaining membrane integrity and alleviation of oxidative stress .

研究领域: 食品科学 · 微生物学 · 生物技术
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Self-adhesive frost-resistant conductive hydrogel electrolytes based on TA@WSCA-Zn autocatalytic system for flexible and foldable solid-state capacitors

Yanjun Pang,Xinxin Luan,Kefeng Zhang,Yuxiang Liu,Lu Li,Congxia Xie,Jinhui Pang

In this study, we have successfully prepared a freeze-resistant conductive hydrogel with a fast polymerization rate and excellent mechanical and adhesive properties. In this paper, hydrogels capable of rapid polymerization in a short time were prepared based on the TA@WSCA-Zn (WSCA, water-soluble cellulose acetate; TA@WSCA, tannic acid-coated WSCA suspension; TA@WSCA-Zn, a certain amount of zinc chloride (ZnCl 2 ) was added to TA@WSCA suspension;) autocatalytic system at room temperature or low temperature. TA@WSCA-Zn forms a stable reversible quinone-catechol redox reaction to activate the decomposition of ammonium persulfate (APS, initiator) to produce SO 4 −· radicals, which triggers the ultra-fast polymerization of amphoteric ([2-(methacryloyloxy) ethyl] dimethyl-(3-sulfopropyl), SBMA) and acrylic monomers (AA). To improve the frost resistance and electrical conductivity of the hydrogels, we also introduced amphoteric ions, which can provide migration channels for Zn 2+ and greatly increase the migration rate. The TA@WSCA-7.5/PSA hydrogel (PSA, hydrogel prepared by polymerization of acrylic acid and SBMA as monomers;) can achieve tensile strength and toughness of 1.33 MPa and 4.89 MJ m −3 . It can provide excellent electrical conductivity and interfacial adhesion over a temperature range of 25 to −60 °C. In addition, the supercapacitor assembled from the TA@WSCA-7.5/PSA hydrogel electrolyte still has good capacitance characteristics after folding and 10,000 charge/discharge cycles, with a capacitance retention of 93.33 % and an excellent cycle life. This autocatalytic system provides a new strategy and approach for the preparation of freeze-resistant conductive hydrogel electrolytes.

CAS / MDL: 7727-54-0 110-26-9
研究领域: 材料科学 · 电化学 · 聚合物化学 · 能源存储
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Green Chemical Engineering · 2023 · IF 0

Bioinspired anti-freezing 3D-printable conductive hydrogel microfibers for highly-sensitive and wide-range detection of ultralow and high strains

Yi-Min Yang,Ting-Yuan Hu,Haidong Fan,Lu Shi,Shi-Yuan Zhang,Zhuang Liu,Xiao-Jie Ju,Rui Xie,Wei Wang,Liang-Yin Chu

Soft strain sensors that can transduce stretch stimuli into electrical readouts are promising as sustainable wearable electronics. However, most strain sensors cannot achieve highly-sensitive and wide-range detection of ultralow and high strains. Inspired by bamboo structures, anti-freezing microfibers made of conductive poly(vinyl alcohol) hydrogel with poly(3,4-ethylenedioxythiphene)-poly(styrenesulfonate) are developed via continuous microfluidic spinning. The microfibers provide unique bamboo-like structures with enhanced local stress to improve both their length change and resistance change upon stretching for efficient signal conversion. The microfibers allow highly-sensitive (detection limit: 0.05% strain) and wide-range (0%–400% strain) detection of ultralow and high strains, as well as features of good stretchability (485% strain) and anti-freezing property (freezing temperature: −41.1 °C), fast response (200 ms), and good repeatability. The experimental results, together with theoretical foundation analysis and finite element analysis, prove their enhanced length and resistance changes upon stretching for efficient signal conversion. By integrating microfluidic spinning with 3D-printing technique, the textiles of the microfibers can be flexibly constructed. The microfibers and their 3D-printed textiles enable high-performance monitoring of human motions including finger bending and throat vibrating during phonation. This work provides an efficient and general strategy for developing advanced conductive hydrogel microfibers as high-performance wearable strain sensors.

研究领域: 材料科学 · 生物医学工程
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