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CARBON · 2022 · IF 11.307

High strength and ultralight lignin-mediated fire-resistant aerogel for repeated oil/water separation

Yiying Yue,Yu Wang,Junyao Li,Wanli Cheng,Guangping Han,Tao Lu,Chaobo Huang,Qinglin Wu,Jianchun Jiang

Oil spillage accidents have caused serious environmental issues, and resulted in oil-cleaning materials receiving widespread attention. In this study, lignin, a crucial recalcitrant component in biomass utilization , was employed to mediate the preparation of graphene aerogel for oil/water separation and rapid regeneration through combustion. The resultant aerogel exhibits ultralight weight (14.22 mg/cm 3 ), high porosity (99.01%), good mechanical properties (1.361 ± 0.04 MPa), super-hydrophobicity (Water Contact Angle = 154.9°), excellent oil and water separation performance (adsorption capacity of chloroform = 102 g/g), and rapid regeneration via direct ignition within 1 min. In addition, the obtained aerogel not only maintained high oil absorption rates in harsh environments (strong acid, strong alkali, high salinity, and high temperature) and facilitated continuous separation of oil and water through pumping but also retained approximately about 90% of the initial absorption capacity after at least 20 combustion cycles. Therefore, based on these extraordinary properties, the obtained aerogel demonstrates great potential for the treatment of marine oil spills. Furthermore, this work may provide a new approach for realizing the high-value utilization of lignin.

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JOURNAL OF BIOMATERIALS APPLICATIONS · 2022 · IF 2.712

Conductive, self-healing, and antibacterial Ag/MXene-PVA hydrogel as wearable skin-like sensors

Lumin Li,Xiaofeng Ji,Kai Chen

The rapid development of flexible electronic technology has led to the in-depth study of flexible wearable sensors to achieve accurate sensing under different external stimuli. However, it is still a huge challenge to develop hydrogel-based wearable skin-like sensors with super ductility, high sensitivity, and self-healing properties. Herein, the Ti3C2 type of MXene was synthesized, and the Ag/MXene nanocomplexes were incorporated into polyvinyl alcohol-borax matrix to construct a novel composite hydrogel as the multifunctional nanofillers, which could bring both improved properties and novel functionalities. The Ag/MXene-Poly (vinyl alcohol) (PVA) hydrogel displayed integrated merits of highly strain sensitive (GF = 3.26), self-healing (within 10 min, 91% healing efficiency), and excellent antibacterial activity. The hydrogel could be assembled into a wearable skin-like sensor to monitor human movement, including large deformations (finger, elbow, wrist, and knee bending) and tiny deformations (mouth’s movement and throat vocalization) in real time. Therefore, this work shed a new light on the development of flexible wearable skin-like sensors for the personalized healthcare monitoring, human–machine interfaces, and artificial intelligence.

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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.

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ACS Applied Energy Materials · 2022 · IF 6.959

Boron Nitride-Doped Inorganic Hydrated Salt Gels Demonstrating Superior Thermal Energy Storage and Wearability Toward High-Performance Personal Thermal Management

Yingying Luo,Liqing Zou,Junpeng Qiao,Jiaming Zhang,Kai Liu,Hongjiao Wu,Pengcheng Lin,Ying Chen

Realizing the person thermal management (PTM) toward human body and its local environment is emerging as a research hotspot. Sodium sulfate decahydrate (SSD) possessing reversible thermal energy absorption, storage, and release around the human body temperature provides a promising solution for PTM and thermal comfort. However, developing SSD-based functional materials with superior thermophysical properties and wearability to enable efficient PTM still remains a huge challenge. Herein, a strategy of ionic cross-linking, chemical cross-linking, and boron nitride (BN) doping is developed to manufacture the high-performance hybrid SSD gels. The supercooling degree of the BN@SSD gels can be reduced to 0 °C. The thermal conductivity (1.2668 W m–1 K–1) of the BN@SSD gels can be increased by 63.14%. The BN@SSD gels present a large thermal energy storage capacity of 132.52 J g–1. The BN@SSD gels demonstrate excellent form stability to confine the liquid SSD and high cyclic stability of 200 cycles. Furthermore, The BN@SSD gels also possess superior wearability in terms of high flexibility, high self-repairing efficiency, and high cost effectiveness (5.53 × 10–3 ¥ g–1). Owing to the various merits of the synergistic enhancement effect, the BN@SSD gels are effectively utilized in wearable PTM to generate thermal comfort for the human body. The multifunctional thermal energy storage gels offer a promising route to the highly efficient application of PCMs in next-generation PTM.

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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS · 2022 · IF 5.518

A freestanding dual-cross-linked membrane with robust anti-crude oil-fouling performance for highly efficient crude oil-in-water emulsion separation

Yuqi Wang,Yi He,Jing Yu,Hongjie Li,Shuangshuang Li,Shuting Tian

Hydrogel membranes generally possess weak mechanical properties , and the membrane surface is susceptible to abrasion, which results in the loss of superwetting properties and oil/water separation ability. Therefore, we prepared a flexible freestanding membrane using a dual-cross-linking approach. A mixed solution of sodium alginate (SA) and polyvinyl alcohol (PVA) was covalently and ionically cross-linked with borax and calcium chloride (CaCl 2 ) to form a hydrogel, and sodium carbonate (Na 2 CO 3 ) solution was then added to synthesize calcium carbonate (CaCO 3 ) in situ. The combination of covalent and ionic cross-linking improves the tensile strength . The prepared SA/PVA/borax/CaCO 3 (SPBC) membrane maintained excellent superwetting properties and oil/water separation ability, even after abrasion. The SPBC membranes have broad application prospects in the oily wastewater purification owing to their numerous advantages, such as cost effectiveness, high separation efficiency, and improved mechanical strength .

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COMPOSITES PART A-APPLIED SCIENCE AND MANUFACTURING · 2022 · IF 9.463

An anti-freezing wearable strain sensor based on nanoarchitectonics with a highly stretchable, tough, anti-fatigue and fast self-healing composite hydrogel

Yanqing Wang,Bo Pang,Rixuan Wang,Yiliang Gao,Yuetao Liu,Chuanhui Gao

The application of conductive hydrogel sensors in wearable devices and electronic skin has aroused great research interest. However, hydrogel sensor cannot simultaneously have good self-healing properties, anti-freezing properties and excellent anti-fatigue properties, which results in poor reusability and unstable sensing performance. A composite hydrogel was synthesized by one-pot method using polyvinyl alcohol, acrylamide, sodium alginate and glycerol as raw materials. The obtained hydrogel has excellent mechanical properties (0.51 MPa stress, 1500% elongation at break and tensile toughness of 3.6 MJ/m 3 ) and fast self-healing performance with healing efficiency (HE) as high as 92% without any external stimulus. At the same time, glycerol has strong freeze resistance for hydrogels. The hydrogel can stably transmit electrical signals at subzero temperature (−20 °C). In addition, we also verified that the hydrogel could self-recover in a short time through cyclic stretching, indicating the fatigue resistance and rapid recovery of the material.

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POLYMERS FOR ADVANCED TECHNOLOGIES · 2022 ·Vol. 33 ·期 8 ·2528-2541 · IF 3.348

Double dynamic bonds tough hydrogel with high self-healing properties based on acylhydrazone bonds and borate bonds

Lijun Chen,Sui Wang,Zhiyong Guo,Yufang Hu

Hydrogels with excellent self-healing properties have specific applications in smart polymer materials, but they often do not have excellent mechanical properties, or the preparation process of hydrogels is too complicated. Here, we prepared a multi-functional intelligent hydrogel using a simple water bath one-pot method through the synergistic effect of dual dynamic cross-linked agents, including acylhydrazone bonds (the first cross-linked agent) and borate ester bonds (the second cross-linked agent), at the same time hydrogen bonds provided physical interaction. The hydrogel exhibited excellent self-healing ability (up to 91%) and extraordinary mechanical strength (tensile stress 173.1405 kPa and hysteresis energy of 1.8659 MJ m −3 ). The research used chemical cross-linked (acylhydrazone bonds and borate ester bonds) and physical cross-linked (hydrogen bonds). The prepared hydrogel had the dual advantages of excellent self-healing performance and high mechanical strength. The hydrogel can be used in smart materials, such as working pressure tissues and sensing materials that require a certain degree of mechanical strength and self-healing properties, and also provides a design strategy for preparing hydrogels with high mechanical strength and excellent self-healing properties.

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COLLOIDS AND SURFACES B-BIOINTERFACES · 2022 · IF 5.999

High efficiency of in-situ cross-linking and acid triggered drug delivery by introducing tobramycin into injectable and biodegradable hydrogels

Ke Xu,Wangjie Shan,Neng Hu,Jiping Wang,Wenlong Zhou,Peter Müller-Buschbaum,Qi Zhong

High efficiency of in-situ cross-linking and acid triggered drug delivery is realized by introducing tobramycin into the hydrogels. Injectable and biodegradable hydrogels are prepared through two steps: First generation of reactive aldehyde groups in the sodium alginate (A-Alg) and then introduction of antibiotic tobramycin as cross-linker. Due to the formation of dynamic Schiff base bonds between the amino groups in tobramycin and aldehyde groups in A-Alg, the gelation of hydrogels can be realized immediately. Thus, tobramycin acts well as the first role cross-linker and the hydrogels containing tobramycin can be injected into the wound during the treatment. In addition, the acid from the decomposition of organic compounds by the bacteria can break the cross-linking points previously formed by tobramycin in the hydrogels. Therefore, tobramycin can be released and act as the second role model drug to kill the bacteria. Because the hydrogels network is broken, the release of tobramycin is more efficient than the traditional drug delivery from hydrogels by diffusion . Based on these unique properties, the present hydrogels containing tobramycin exhibit a good injectable and biodegradable capability. In addition, due to the existence of the reversible acid-labile linkages in the hydrogels, the hydrogels containing tobramycin are also self-healing, which additionally is favorable for the application of wound dressing. More importantly, the antibacterial hydrogels also demonstrate good biocompatibility in vitro and significantly therapeutic effects on an infected mice model in vivo. Based on the above special properties, the hydrogels cross-linked by tobramycin indicate a new approach to prepare hydrogel dressings with low-cost, non-toxicity and good anti-bacterial performance in the treatment of infectious wounds.

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CARBOHYDRATE POLYMERS · 2022 · IF 10.723

Tunable mechanical, self-healing hydrogels driven by sodium alginate and modified carbon nanotubes for health monitoring

Wen Li,Lu-Qi Tao,Mei-Cun Kang,Chang-Heng Li,Ci-Yong Luo,Gang He,Tian-Yi Sang,Ping Wang

Conductive hydrogels featuring a modulus similar to the skin have flourished in health monitoring and human-machine interface systems. However, developing conductive hydrogels with self-healing and tunable force-electrical performance remains a problem. Herein, a hydrogen bonding cross-linking strategy was utilized by incorporating silk sericin-modified carbon nanotubes (SS@CNTs) into sodium alginate (SA) and polyvinyl alcohol (PVA). Hydrogels synthesized with desirable tensile strength and self-healing ability (67.2 % self-healing efficiency in fracture strength) assembled into strain sensors with a low detection limit of 0.5 % and a gauge factor (GF) of 4.75 (0–17 %). Additionally, as-prepared hydrogels exhibit high sensitivity to tiny pressure changes, allowing recognition of complex handwriting. Notably, resulting hydrogels possess self-powered property, generating up to 215 V and illuminating 100 commercial green LEDs. This work stems from the pressing need for multifunctional hydrogels with prospective applications in human motion sensing and energy harvesting.

CAS / MDL: 9005-38-3 1303-96-4
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APPLIED SURFACE SCIENCE · 2022 · IF 7.392

N, O co-doped carbon aerogel derived from sodium alginate/melamine composite for all-solid-state supercapacitor

Jinqiang Sun,Jing Zhang,Mengge Shang,Minna Zhang,Xinfu Zhao,Sijia Liu,Xiaochan Liu,Shuo Liu,Xibin Yi

Hierarchical porous carbon shows great potential in the field of energy storage due to high porosity, large surface area, and excellent electrical conductivity. Here, we successfully fabricated carbon aerogel derived from sodium alginate/melamine composite (SAM) by directional freeze-drying combined with simple carbonization and activation process. The optimal SAM-700-4 possesses a high nitrogen (5.67 at.%) and oxygen (8.98 at.%) contents along with high specific surface area of 2577.62 m 2 /g and unique directional channel structure. Due to their synergistic effect, the SAM-700-4 electrode exhibits a high specific capacitance of 441.80   F/g at a current density of 0.5 A/g. Interestingly, the all-solid-state symmetric supercapacitor based on SAM-700-4//SAM-700-4 in PVA/SA/KOH gel electrolyte has a large energy density of 20.87 Wh/kg at a power density of 4000 W/kg and exhibits excellent cycling stability. It is believed that this N, O co-doped directional hierarchical porous carbon aerogel may show promising prospects as advanced energy storage materials.

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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2022 · IF 8.025

Polyvinyl alcohol/carboxymethyl chitosan hydrogel loaded with silver nanoparticles exhibited antibacterial and self-healing properties

Yalei Liu,Jie Mao,Zhiyong Guo,Yufang Hu,Sui Wang

Hydrogel materials are gradually increasing research in biological aspects due to their unique properties. In order to prepare hydrogels with the potential to be used in clinical wound therapy, the authors prepared a bifunctional hydrogel with antibacterial and self-healing properties. The hydrogel was composed of borax cross-linked polyvinyl alcohol (PVA) and carboxymethyl chitosan (CMCS), which realizes self-healing between polymers through hydrogen bonds and borate ester bonds. The double cross-linking of hydrogen bonds and borate ester bonds also endows the hydrogel with better mechanical properties (toughness and tensile stress can reach 22.30 MJ/m 3 and 70.35 KPa, respectively). On this basis, adding highly stable silver nanoparticles (AgNPs) to the hydrogel can effectively inhibit the growth of E. coli and S. aureus . This idea provides the possibility for the application of hydrogels in the process of biological wound healing.

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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

Injectable Tumor Microenvironment-Modulated Hydrogels with Enhanced Chemosensitivity and Osteogenesis for Tumor-Associated Bone Defects Closed-Loop Management

Min Cai,Xiaojun Li,Meng Xu,Shiqi Zhou,Lei Fan,Jingyan Huang,Cairong Xiao,Yichen Lee,Bo Yang,Le Wang,Ross William Crawford,Yin Xiao,Lei Zhou,Chengyun Ning,Yan Wang

Patients with postoperative tumor-associated bone defects need both chemotherapy and bone repair in the shifted disease states, but chemotherapy resistance, severe side-effects, and poor bone regeneration result in tumor recurrence and therapy failure. Herein, we develop an injectable and tumor microenvironment (TME)-modulated hydrogel composed of bio-responsive drug-loaded mesoporous bioactive glass nanoparticles (MBGN), gelatin (Gel), and oxidized chondroitin sulfate (OCS) for tumor-associated bone defects closed-loop management. The TME-modulated hydrogels can deplete protons and glutathione (GSH) within residual tumor tissues with sustained drug responsive-release capability, therefore interfering TME and overcoming cancer resistance, and also reducing off-target effects. Mechanistically, in the early state of treatment, acidic environment of TME will break the Schiff’s base bond network of hydrogels, thus deliver drug-loaded nanoparticles into tumor cells. Subsequently, the pH-responsive amide bonds, GSH-responsive disulfide bonds and acidity-degradable nanocarriers of drug-loaded nanoparticles can induce ROS stress and mitochondrial-related damage, activating the p16-CYLD tumor suppressor pathway to induce apoptosis and inhibit metastasis. In the late state of treatment, the hydrogels shifted into regenerative scaffolds to exert long-lasting osteogenesis effects. Overall, the TME-modulated hydrogels can orchestrate steady bone repair and avoid tumor recurrence, achieving closed-loop management of postoperative tumor-associated bone defects.

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