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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2024 · IF 7.7

Fe3+-induced coordination cross-linking gallic acid-carboxymethyl cellulose self-healing hydrogel

Yongyan Yang,Ying Ma,Meiliang Wu,Xueping Wang,Yuan Zhao,Shuangling Zhong,Yan Gao,Xuejun Cui

Self-healing hydrogel is a promising soft material for applications in wound dressings, drug delivery, tissue engineering, biomimetic electronic skin, and wearable electronic devices. However, it is a challenge to fabricate the self-healing hydrogels without external stimuli. Inspired by mussel, the metal-catechol complexes were introduced into the hydrogel systems to prepare the mussel-inspired hydrogels by regulating the gelation kinetics of Fe 3+ crosslinkers with gallic acid (GA) in this research. The amine-functionalized carboxymethyl cellulose (CMC) was grafted with GA and then chelated with Fe 3+ to form a multi-response system. The crosslinking of carboxymethyl cellulose-ethylenediamine-gallic acid (CEG) hydrogel was controlled by adjusting the pH to affect the iron coordination chemistry, which could enhance the self-healing properties and mechanical strength of hydrogels. In addition, the CEG hydrogel exhibited great antibacterial and antioxidant properties. And the CEG hydrogel could strongly adhere to the skin tissue. The adhesion strength of CEG hydrogel on pigskin was 11.44 kPa, which is higher than that of commercial wound dressings (∼5 kPa). Moreover, the thixotropy of the CEG hydrogel was confirmed with rheological test. In summary, it has great potential in the application field of wound dressing.

研究领域: 材料科学 · 生物医学工程 · 化学 · 生物材料
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Small · 2024 · IF 13

3D-Printed Hydrogels with High-Strength and Anisotropy Mediated by Chain Rigidity

Deshuai Kong,Yunmeng Li,Biao Yang,Yaokun Pang,Hua Yuan,Cong Du,Yeqiang Tan

Extrusion-based 3D printing is a facile technology to construct complex structures of hydrogels, especially for tough hydrogels that have shown demonstrated potential in load-bearing materials and tissue engineering. However, 3D-printed hydrogels often possess mechanical properties that do not guarantee their usage in tissue-mimicking, load-bearing components, and motion sensors. This study proposes a novel strategy to construct high-strength and anisotropic Fe 3+ cross-linked poly(acrylamide- co -acrylic acid)/sodium alginate double network hydrogels. The semi-flexible sodium alginate chains act as a “conformation regulator” to promote the formation of strong intermolecular interactions between polymer chains and lock the more extended conformation exerted by the pre-stretch, enabling the construction of 3D-printed hydrogel structures with high orientation. The equilibrated anisotropic hydrogel filaments with a water content of 50–60 wt.% exhibit outstanding mechanical properties (tensile strength: 9–44 MPa; elongation at break: 120–668%; Young's modulus: 7–62 MPa; toughness: 26–52 MJ m − 3 ). 3D-printed anisotropic hydrogel structures with high mechanical performance show demonstrated potential as loading-bearing structures and electrodes of flexible triboelectric nanogenerators for versatile human motion sensing.

研究领域: 材料科学 · 生物医学工程 · 组织工程 · 纳米技术 · 3D打印
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Journal of Water Process Engineering · 2024 · IF 6.3

Highly efficient photocatalysis-Fenton degradation of antibiotics and phenol over sulfidated FeOCl under natural sunlight illumination

Jiayang Huang,Yunchang Xie,Chunhui Dai,Hao Cui,Chao Zeng

Sulfidated FeOCl is prepared as a heterogeneous photo-Fenton catalyst. And the surface sulfidation of FeOCl can remarkably accelerate the photoinduced charge separation and transfer, while also increase Fe 2+ /Fe 3+ atomic ratio, leading to the boosted photo-Fenton activity in the presence of H 2 O 2 . Under irradiation of natural sunlight (light intensity: ∼80 mW·cm −2 ), over 10 mg sulfidated FeOCl catalyst with using 20 μL 15 % H 2 O 2 , 91.2 % of ofloxacin solution (50 mg·L −1 ) and 97.5 % of sulfisoxazole solution (60 mg·L −1 ) can be degraded in 80 min, and 99.6 % of phenol solution (625 mg·L −1 ) is decomposed in 4 h. Under irradiation of a white Light-Emitting Diode (LED) lamp (light intensity: 5 mW·cm −2 ), 99.8 % of ofloxacin solution is decomposed after treatment for 4 h. Moreover, this photo-Fenton degradation system displays a stable activity in a wide range of pH (1−10), diverse water bodies, and various coexisting ions with concertation from 1 mM to 500 mM. Moreover, sulfidated FeOCl catalyst coated on a frosted glass sheet exhibits excellent stability for degrading ofloxacin even in seven continuous cycles. Particularly, the non-toxicity of the treated ofloxacin, sulfisoxazole, and phenol solution, have been proven by testing their toxic effects on cabbage seed, bacteria, and human embryonic kidney cell, respectively.

研究领域: 环境科学 · 催化 · 光化学 · 水处理 · 材料科学
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Harnessing bimetallic iMWA nanosensitizer to unleash ferroptosis and calcium overload: Unlocking tumor vulnerability for potentiated iMWA therapy against hepatocellular carcinoma

Guanhua Qiu,Duo Wang,Peihan Xie,Zelun Li,Niqiang Zhou,Xiaoqian Zhang,Xiaobo Wang,Jiali Tang,Jun Cao,Junjie Liu,Danke Su

Microwave ablation (MWA) holds promise as a tumor treatment modality, yet incomplete ablation with low-frequency MWA (iMWA) remains a significant obstacle to survival, while the high-frequency MWA poses safety concerns. To address these challenges, we introduce a novel bimetallic iMWA nanosensitizer, CFT-NPs, constructed via metal-coordination interactions between tannic acid (TA) and iron/calcium dual metal ions (Fe 3+ /Ca 2+ ). The Fe 3+ /Ca 2+ in CFT-NPs work in harmony to convert electromagnetic energy into heat, thereby bolstering the effectiveness of iMWA while maintaining good biosafety. Furthermore, the pH-triggered rupture of CFT-NPs release TA, Fe 3+ , and Ca 2+ . The liberated Fe 3+ undergoes reduction by TA, and when combined with Ca 2+ , they trigger ferroptosis and Ca 2+ overload respectively, significantly amplifying the therapeutic effects of iMWA. Utilization iMWA with CFT-NPs results in lipid oxidation, mitochondrial dysfunction, and disruption of redox balance, both in vitro and in vivo . Notably, this nanosensitizer exerts a robust antitumor effect, effectively inhibiting tumor growth and downregulating the expression of matrix metalloproteinases, which is associated with tumor metastasis. Collectively, this innovative study offers a promising approach to overcome the challenges of incomplete ablation and biological safety, enhancing the antitumor efficacy of iMWA..

CAS / MDL: 10043-52-4 1401-55-4
研究领域: 肿瘤学 · 生物医学工程 · 材料科学 · 癌症治疗
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

A gelatin-based ionic conductor with a dense/loose alternating network enabled by surface active cellulose

Haocheng Fu,Bin Wang,Jinpeng Li,Li Zhang,Jun Xu,Jinsong Zeng,Wenhua Gao,Kefu Chen

Although conductive and stretchable ionic conductors are increasingly prepared for flexible sensing applications, such as health monitoring, tissue engineering, and electronic skin, achieving a balance between remarkable mechanical properties and high sensing sensitivity remains a significant challenge. In this work, a dense/loose alternating network was meticulously constructed through a pre-assembly process in sodium citrate solution and a subsequent re-assembly in FeCl 3 solution. This approach ensured the robustness of the network structure and facilitated ion migration. Within the network, a gelatin network cross-linked via covalently and hydrogen bonds was significantly enhanced by a synergy of micro-enhancement and dynamic bidirectional crosslinking containing hydrogen bonds, imine bonds, and Fe coordinate bonds enabled by surface active cellulose. Benefiting from the dense network, the obtained composite hydrogels delivered a strong tensile strength (496.3 kPa), outstanding elastic modulus (917.6 kPa), and an excellent energy dissipation rate (55.6 %) at 80 % of strain. The loose polymer network can also endow Fe 3+ /Cl − ions with sensitive mobility, leading to an ultra-high sensing sensitivity (maximum GF: 20.06). These exceptional properties enable the ionic conductor to accurately detect a wide range of motions and pressures without being affected by environmental noise. With attributes such as reusability, biodegradability, strength, and sensitivity, this ionic conductor emerges as a reliable soft material with promising applications in the field of healthcare monitoring, wearable strain sensor sensors, and writing anti-counterfeiting materials.

CAS / MDL: 7473-98-5 9002-89-5
研究领域: 材料科学 · 生物医学工程 · 传感器与执行器 · 柔性电子 · 健康监测
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2021 · IF 8.128

Multi-functionalized carbon aerogels derived from chitosan

Lu Wang,Qiong Wu,Baozheng Zhao,Zelin Li,Yuehong Zhang,Lang Huang,Shitao Yu

Carbon aerogels are prepared by a thermal treating-freeze drying approach from chitosan, with glycine hydrochloride ionic liquid (IL) acting as solvent and nitrogen source. Different post-treatments such as ball milling and high temperature carbonization are employed to functionalize the obtained carbon aerogels with tuned properties, making it promising candidates as fluorescence material (NACs-Q), electrode material (FDC-800) and catalyst support (NAC Pd -C). NACs-Q is water-soluble quantum dot with average particle sizes of 3.8 nm, presenting excitation-/emission-independent and pH-sensitive properties, which could be used as sensor for testing acetone vapor or an “on-off-on” sensor for detections of Fe 3+ and vitamin C in fruits. FDC-800 exhibits fluffy lamellar structure with developed micro-mesopores and nitrogen-containing groups on their surfaces, which is beneficial for building flexible solid-state supercapacitor with excellent performance, delivering a capacitance of 208F/g at 0.5 A/g, and achieving an energy density of 7.2 W h/kg at a power density of 50 W/kg. Moreover, NAC Pd -C can be used as catalyst for phenol hydrogenation, and phenol conversion of 100% with cyclohexanone selectivity of 98.3% is achieved, due to the synergetic effects of the Pd active-site, the N -containing groups, and the Lewis acid sites on the support.

研究领域: 材料科学 · 化学工程 · 纳米技术 · 环境科学 · 分析化学 · 催化
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2023 · IF 8.2

Alginate based photothermal cryogels boost ferrous-supply for enhanced antibacterial chemodynamic therapy and accelerated wound healing

Jia Chen,Yu Xia,Qian Lan,Min Hu,Yueying Xu,Quanxin Wu,Xinguang Liu,Yun Liu

Uncontrolled hemorrhage is a main cause of pre-hospital death. Given the importance of hemostatic wound dressings in pre-hospital emergency treatment, novel composite materials are required for fast hemostasis, synergistic bacterial ablation with negligible resistance and wound healing acceleration. Herein, multifunctional SCTF cryogels were fabricated by the simultaneous cross-linking of sodium alginate (SA) and tannic acid (TA) with Fe 3+ ions. As a result, the prepared SCTF cryogels consisted of Fe 3+ /TA-based metal phenolic networks (MPNs) and Fe 3+ /SA-based 3D skeleton for collagen (CA). MPNs endowed the cryogels with photothermal effect, photothermal-enhanced Fenton activity and pH/photothermal dual-responsive release property of TA and Fe 2+ , which were beneficial for the antibacterial capacity. Due to the intrinsic high porosity, in vitro and in vivo assays demonstrated that SCTF cryogels possessed good hemostatic capacity. Moreover, the synergistic photothermal therapy (PTT), chemodynamic therapy (CDT) and pH/photothermal responsive chemo-therapy dramatically enhanced the bactericidal efficacy of SCTF cryogels both in vitro and in vivo . Eventually, their outstanding healing-accelerating effects were confirmed via animal experiments, which were attributed to the presence of CA and TA. Therefore, the developed composite materials could offer new strategy on exploiting multifunctional wound dressing for clinical applications in the future.

CAS / MDL: 50-81-7 1401-55-4
研究领域: 材料科学 · 生物材料 · 生物医学工程 · 伤口愈合 · 抗菌治疗
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2018 · IF 5.091

A one-pot strategy for preparation of high-strength carboxymethyl xylan-g-poly(acrylic acid) hydrogels with shape memory property

Xinxin Liu,Minmin Chang,Bei He,Ling Meng,Xiaohui Wang,Runcang Sun,Junli Ren,Fangong Kong

High strength hydrogels open new possibilities in the fields of bioengineering and biomedical. In this paper, a highly efficient one-pot strategy was developed to prepare carboxymethyl xylan-g-poly (acrylic acid) (CMX-g-PAA) hydrogels with high compression strength, high elongation and high elasticity by using the metal coordination and the reinforcement of hydroxylate multi-walled carbon nanotubes (HCNTs). Prepared hydrogels were characterized by means of FTIR, XRD, SEM, rheological measurements as well as their swelling and mechanical properties. Results showed that the Fe 3+ -carboxyl coordination and HCNTs imparted hydrogels with high strength and good rapid recovery properties, in which the maximum high compressive strength and elongation at break were achieved to 10.4 MPa and 1032%, and the shape of hydrogels almost returned to the original shape after the external force was removed after 30 cycles of compression. These hydrogels also exhibited Fe 3+ -triggered shape memory properties. Therefore, as-prepared hydrogels possessing high strength, rapid recovery and shape memory properties, could broaden access for application in intelligent toys, electronic skin, biosensing, and tissue engineering.

CAS / MDL: 110-26-9
研究领域: 材料科学 · 生物医学工程 · 生物工程
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Advanced Healthcare Materials · 2022 ·Vol. 11 ·期 15 ·2200559 · IF 11.092

Coordination-Driven Metal-Polyphenolic Nanoparticles toward Effective Anticancer Therapy

Di Wu,Bin Zhou,Jing Li,Xinyi Wang,Bin Li,Hongshan Liang

Stabilization of bioactive components, especially for hydrophobic functional factors, is a promising approach for improving their biological activity. Here, a metal-phenolic coordination chemistry that synthesizes biocompatible and biodegradable thin film based on tannic acid and trivalent metal ion (Fe 3+ or Al 3+ ) is addressed, and the results also demonstrate its use for encapsulating a hydrophobic drug (nobiletin) and triggering drug release for cancer treatment both in vitro and in vivo. This assembled system provides drug-loaded nanoparticles (NPs) with small, but uniform, size (≈200 nm). It displays beneficial potential in enhancing colloidal stability and preventing premature drug leakage. Moreover, the metal-phenolic coating is found to possess high cell biocompatibility as a delivery vector for controlled drug delivery, while the final fabricated drug NPs have effective anti-tumor activity by both inducing higher tumor apoptosis and inhibiting tumor metastasis, which is superior to naked drug formulations. Overall, these findings propose an effective and straightforward way for coating hydrophobic drugs employing interfacial adhesion and assembly, which can be a highly promising vehicle for controlled-release biomedical applications for cancer therapy.

CAS / MDL: 1401-55-4
研究领域: 纳米技术 · 药学 · 生物医学工程 · 癌症研究 · 材料科学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2023 · IF 9.9

Coenzyme-depleting nanocarriers for enhanced redox cancer therapy under hypoxia

Yao Li,Mengying Liu,Yan Zheng,Zheng Wang,Yanjun Zhao

Cancer cells show unique redox homeostasis . Glutathione (GSH) and reduced nicotinamide adenine dinucleotide phosphate (NADPH) play essential roles as coenzymes of multiple key antioxidant enzymes. Coenzyme depletion offers a unique opportunity for cancer treatment by inducing oxidative stress . Here, we report an innovative hybrid nanocarrier for cancer redox therapy via selective depletion of GSH and NADPH. The nanocarrier core is a sorafenib-loaded porous zeolitic imidazole framework (ZIF-65), and the shell is epigallocatechin gallate (EGCG)-Fe 3+ complex (EF). The nitroimidazole ligand in ZIF-65 could selectively deplete NADPH under hypoxia . Sorafenib diminished GSH by inhibiting cystine import and GSH biosynthesis. EGCG can reduce Fe 3+ to Fe 2+ , which aids the generation of hydroxyl radicals via the Fenton reaction . The reversible coordination between nitroimidazole and Zn 2+ , EGCG, and Fe 3+ enables triggered cargo release in acidic lysosomes . Tailored nanocarriers induced the depletion of both coenzymes (GSH and NADPH) and boosted reactive oxygen species in a 4T1 murine cancer cell line. The altered redox balance eventually resulted in efficient apoptotic cell death. The current work offers a novel means of redox cancer therapy via the selective depletion of key antioxidant enzymes in hypoxic cells.

研究领域: 癌症治疗 · 纳米技术 · 氧化还原生物学 · 药学
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Confined conductive and light-adsorbed network in metal organic frameworks (MIL-88B(Fe)) with enhanced photo-Fenton catalytic activity for sulfamethoxazole degradation

Hui He,Yuexin Wang,Juan Li,Shanliang Jiang,Subhan Sidra,Wenxue Gong,Ying Tang,Yang Hu,Rule Wei,Dongxiao Yang,Xuesheng Li,Zhongxing Zhao

High light adsorption and fast charge separation are crucial for photo-Fenton catalytic activity of MOFs. Herein, bottom-up design was proposed to fabricate polypyrrole (PPy C ) nanowires in MIL-88B(Fe) cages as photo-Fenton catalyst for Sulfamethoxazole (SMX) efficient degradation. Pyrrole was prior anchored into MIL-88B(Fe) cluster via Fe-N coordination, and then the additional monomer pyrrole was further triggered bottom-up polymerization in confined cages of MIL-88B(Fe) and formed PPy C @Py-MIL(Fe) composite. These PPy C nanowires were dispersed in Py-MIL(Fe) cages and tightly connected with MOFs clusters via Fe-N bonding. Characterization proved that: (1) Interfacial Fe-N can significantly promote the efficient electron transport from PPy C nanowires to Py-MIL(Fe), enhance optical absorption property, and construct strong Lewis acidic sites and ligand vacancies in PPy C @Py-MIL(Fe). (2) The confined PPy C nanowire via Fe-N connection remarkably promote photo-generated electron-hole separation, Fe 2+ |Fe 3+ redox ability of MOF, and improved photo-electric corrosion ability. As a result, it significantly enhanced the photo-Fenton catalytic performance for SMX degradation. Catalytic oxidation was attributed to the generation of ‧OH species that oxidized 93% SMX in 60 min, showing ultra-rapid degradation and TOC removal rates of 33.7 min −1 ·mg·g −1 and 8.68 min −1 ·mg·g −1 respectively, which was about 4–220 times higher than those reported state-of-the-art catalysts. Additionally, the PPy C @Py-MIL(Fe) catalyst showed minimal loss in catalytic activity even after recycling for 10 times, exhibiting good recycling stability compared to many MOFs. Systematic analysis shown that in-situ anchored growth of polypyrrole in confined porous cages of MOF can effectively enhance the catalytic activity and stability of MIL-88B(Fe), and has great development potential applications for photo-Fenton catalytic degradation of organic pollutants.

研究领域: 环境科学 · 材料科学 · 催化 · 水处理
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Nano Energy · 2022 · IF 19.069

Extreme environment-adaptable and fast self-healable eutectogel triboelectric nanogenerator for energy harvesting and self-powered sensing

Yufan Feng,Jie Yu,Dan Sun,Chao Dang,Wenfeng Ren,Changyou Shao,Runcang Sun

Hydrogel-based triboelectric nanogenerators (H-TENGs) are emerging as an appealing platform for the wearable electronics owing to their attractive mechanical flexibilities and conductive properties. However, time- and energy-consuming polymerization process of hydrogel and inevitable freezing of water within hydrogel networks at sub-zero temperature severely limit the practical applications of H-TENGs. To address the issues, we herein report a transparent, stretchable, anti-freezing, and self-healable TENG based on the ultrafast fabricated eutectogels for energy harvesting and self-powered sensors. The eutectogel electrode is initially constructed by a dynamic oxidation and coordination system composed of sulfonated lignin (SL) and Fe 3+ . After immersed in deep eutectic solvent (DES), the obtained eutectogels with high stretchability (~450%), transparency (93.5%) and ionic conductivity (8.70 mS cm −1 ) can be retained even in extreme temperature as low as − 80 °C. Notably, the eutectogel assembled TENGs (E-TENGs) show high and stable electrical output performances including open-circuit voltage of 105 V, short-circuit current of 0.5 µA, short-circuit charge of 10 nC, and power density up to 53 mW m −2 . The E-TENG with a self-charging system can easily light up 20 light-emitting diodes (LEDs) and charge up capacitors to drive commercial electronics by harvesting energy. Moreover, as a proof of concept , the flexible E-TENG can serve as a self-powered biomechanical sensor to realize the real-time monitoring of various human motions, which provide a promising and versatile platform for environment adaptable hydrogel-based TENG with reliable output performance and self-healing ability.

CAS / MDL: 10025-77-1
研究领域: 材料科学 · 纳米技术 · 能量收集 · 可穿戴电子 · 传感器
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