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DALTON TRANSACTIONS · 2023 ·Vol. 52 ·期 32 ·11076-11084 · IF 4

Highly dispersed Co anchored on Ce-doped hydroxyapatite as a dual-functional catalyst for selective hydrogenolysis of 5-hydroxymethylfurfural

Zhuoyou Gao,Mengying Wang,Ningzhao Shang,Wei Gao,Xiang Cheng,Shutao Gao,Yongjun Gao,Chun Wang

Hydrodeoxygenation (HDO) is an indispensable approach to produce renewable biofuels and value-added chemicals using natural biomass and its derivatives. 2,5-Dimethylfuran (DMF) is considered to be a very promising liquid biofuel, and it can be fabricated by HDO of the biomass derivative 5-hydroxymethylfurfural (HMF). Herein, a highly efficient bifunctional catalyst, Co/HAP(Ce), was fabricated by anchoring highly dispersed Co on Ce-doped hydroxyapatite (HAP(Ce)). Co/HAP(Ce) displayed excellent HDO catalytic activity to convert HMF to DMF, and 99% HMF conversion and 96% DMF selectivity can be obtained under 150 °C, 2 MPa H2 conditions for 5 h. Density functional theory calculations revealed that H2 can be more easily activated by Co/HAP(Ce). Systematic studies confirmed that the high activity of Co/HAP(Ce) can be ascribed to the desired acid–alkali properties, highly dispersed cobalt species and strong metal–support interactions. This research provides a cost effective approach for designing efficient catalysts for HDO of biomass and its derivatives.

研究领域: 催化 · 化学工程 · 可再生能源 · 材料科学
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ADVANCED FUNCTIONAL MATERIALS · 2024 · IF 18.5

Continuous-Gradient Mineralized Hydrogel Synthesized via Gravitational Osmosis for Osteochondral Defect Repair

Rongtai Sun,Qiang Zhang,Congcong Yu,Yiwei Zhu,Yang Zheng,Tianyuan Gu,Lin Ye,Wentao Yang,Xiaozhang Ying,Yiyang Xu,Shunwu Fan,Ruikang Tang,Weiming Qi,Shasha Yao

The repair of hierarchical osteochondral defects requires complex gradient reconstruction at different levels, with continuous-gradient mineralization being crucial. Strategies for achieving continuous-gradient mineralization have rarely been reported. Here, a continuous-gradient mineralized hydrogel is prepared using simple gravitational osmosis of a ≈2 nm amorphous calcium phosphate nanocluster (ACPC) suspension into composite organic frameworks for osteochondral regeneration. During gravitational infiltration, ACPC underwent gradual mineralization, resulting in the spontaneous formation of hydroxyapatite (HAP). The continuous-gradient mineralized hydrogel aligned closely with the normal osteochondral structure, thereby effectively promoting repair of the cartilage and subchondral bone. In the cartilage layer, organic compounds improved the oxidative stress environment induced by injury and complemented the extracellular matrix of the cartilage. In the subchondral bone layer, HAP from the continuously mineralized hydrogel induced intracellular calcium accumulation in mesenchymal stem cells (MSCs), activating calcium/calmodulin-dependent protein kinase 2 (CaMK2) and promoting osteogenic differentiation of MSCs through the calcium signaling pathway. Ultimately, compared with the nongradient hydrogel, this innovative gradient mineralization method exhibited significantly enhanced regeneration capabilities for osteochondral defects, as evidenced by metrics, such as bone volume/tissue volume (BV/TV), trabecular thickness (Tb.Th), and trabecular number (Tb.N). This holistic strategy provides hope in the field of osteochondral repair.

研究领域: 生物医学工程 · 组织工程 · 骨科 · 再生医学
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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

A novel dual-signal molecularly imprinted electrochemical sensor based on NiFe prussian blue analogue and SnS2 for detection of p-Hydroxyacetophenone

Yan Huang,Daixin Ye,Jing Yang,Huan Lu,Li Li,Yaping Ding

Herein, based on the dual-signal strategy, an electrochemical sensor with molecularly imprinted polymer (MIP) was designed for the analysis of p-Hydroxyacetophenone (p-HAP) for the first time. The sensor was fabricated by modifying the electrode with NiFe prussian blue analogue (NiFe-PBA) and followed by SnS 2 , obtaining the dual-signal from [Fe(CN) 6 ] 3−/4− at 0.20 V and NiFe-PBA at 0.52 V. In the electropolymerization of the MIP film, o-phenylenediamine was used as functional monomer and p-HAP acted as template molecule. After the adsorption of p-HAP, the two above oxidation peak currents decreased simultaneously compared with the elution, achieving the dual-signal analysis. Under the optimal conditions, the sensor exhibited a wide linear range of 10 −13 M to 10 −7 M and a low detection limit of 3.52 × 10 −14 M (3σ). Moreover, it was successfully applied to the p-HAP detection in human serum and environment water samples with satisfactory recovery.

研究领域: 分析化学 · 电化学 · 环境科学 · 材料科学
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Acta Biomaterialia · 2024 · IF 9.4

A Bifunctional Lactoferrin-Derived Amyloid Coating Prevents Bacterial Adhesion and Occludes Dentinal Tubules via Deep Remineralization

Bing Sun,Jiao Sun,Kai Zhang,Yanyun Pang,Cheng Zhi,Fan Li,Yangyang Ye,Jinglin Wang,Yongchun Liu,Jiayin Deng,Peng Yang,Xu Zhang

Dentin hypersensitivity (DH) manifests as sharp and uncomfortable pain due to the exposure of dentinal tubules (DTs) following the erosion of tooth enamel. Desensitizing agents commonly used in clinical practice have limitations such as limited depth of penetration, slow remineralization and no antimicrobial properties. To alleviate these challenges, our study designed a lactoferrin-derived amyloid nanofilm (PTLF nanofilm) inspired by the saliva-acquired membrane (SAP). The nanofilm utilises Tris(2-carboxyethyl)phosphine (TCEP) to disrupt the disulfide bonds of lactoferrin (LF) under physiological conditions. The PTLF nanofilm modifies surfaces across various substrates and effectively prevents the early and stable adhesion of cariogenic bacteria, such as Streptococcus mutans and Lactobacillus acidophilus . Simultaneously, it adheres rapidly and securely to demineralized dentin surfaces, facilitating in-situ remineralization of HAP through a simple immersion process. This leads to the formation of a remineralized layer resembling natural dentin, with an occlusion depth of dentinal tubules exceeding 80 µm after three days. The in vivo and vitro results confirm that the PTLF nanofilm possesses good biocompatibility and its ability to exert simultaneous antimicrobial effects and dentin remineralization. Accordingly, this innovative bifunctional PTLF amyloid coating offers promising prospects for the management of DH-related conditions. Statement of Significance We design a simple, fast, inexpensive, and easy-to-process PTLF nanofilm for nearly any material surface or shape. The PTLF nanofilm modifies surfaces across various substrates and effectively prevents the adhesion of cariogenic bacteria, such as Streptococcus mutans and Lactobacillus acidophilus. The abundant functional groups on the surface of PTLF nanofilm facilitate bioactive hydroxyapatite (HAP) formation and maintain stability at the HAP remineralization interface

研究领域: 牙科材料 · 口腔生物学 · 材料科学 · 纳米技术 · 生物医学工程
✓ 已验证 DOI PubMed 高影响因子
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POLYMER · 2019 · IF 3.771

Direct bromination of nano hydroxyapatite strategy towards particle brushes via surface-initiated ATRP for highly efficient heavy metal removal

Miaomiao Wang,Xiao Wang,Kangmin Zhang,Mingyuan Wu,Qingyun Wu,Jiuyi Liu,Jianjun Yang,Jianan Zhang

Aminated n-HAP-g-polyacrylonitrile (n-HAP-g-APAN) particle brushes were developed for highly efficient heavy metal removal based on surface-initiated ATRP (SI-ATRP) and subsequent amination. An efficient one-step method for morphology controlled synthesis of ATRP initiator immobilized n-HAP (n-HAP-Br) was realized by using 2-bromoisobutyric acid as tetherable initiator. Uniform and individually dispersed n-HAP-Br NCs were obtained with controlled morphology and particle size by adding portion of water miscible organic solvents to rational adjusting aqueous dispersion medium. Aminated n-HAP-g-APAN displayed record-high adsorption capacity of heavy meatal ions due to the combined contributions of grafted APAN providing pendent amino diethylenepentamine as chelating groups and n-HAP core towards heavy metal ions (pure n-HAP of q e  = 284.4 mg/g vs n-HAP-g-APAN of q e  = 944.4 mg/g). The proposed one-step direct bromination of n-HAP strategy provides the preparation of uniform n-HAP NCs ready for polymer grafting and further fabrication of n-HAP-g-polymers via SI-ATRP for various applications depending on the characteristic of grafted polymers.

研究领域: 材料科学 · 环境科学 · 化学工程
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Materials Futures · 2024 ·Vol. 3 ·期 3 ·035403 · IF 12

rADSC-loaded tubular units composed of multilayer electrospun membranes promoted bone regeneration of critical-sized skull defects

Huamin Jiang,Zhaoyi Lin,Jinze Li,Ting Song,Hongyun Zang,Pengwen Li,Jiarun Li,Wenyi Hou,Jianhua Zhou,Yan Li

Adipose-derived stem cells (ADSCs) have considerable potential for bone regeneration. However, their performance is limited by a lack of scaffolds that adequately mimic the hierarchical structure of bone to promote proliferation and osteogenic differentiation of ADSCs. In this study, nanofiber membranes composed of polycaprolactone, poly(lactide-co-glycolide), and hydroxyapatite (HAp) were prepared via electrospinning, and the membranes curled after responding to temperature stimuli in an aqueous solution. Transmission electron microscopy and scanning electron microscopy observations indicated that needle-like HAp nanoparticles with an average diameter of 57 ± 39 nm and a length–diameter ratio of 7.4 ± 1.56 were entrapped in the nanofiber matrix and did not affect the surface morphology of fibers. After cutting and deformation, the nanofibers changed from straight to bent, and the diameters increased; they were 1105 ± 200 nm for BPLG85-H and 1120 ± 199 nm for BPLG80-H. Additionally, tubular units with a single layer (BPLG-H(1.5)) or multiple layers (BPLG-H(3.5)) were obtained by controlling the initial shape and size of the membranes. rADSCs on the concave surface of BPLG-H(3.5) proliferated faster and exhibited better osteogenic activity than those on the convex side of BPLG-H(3.5) and both surfaces of BPLG-H(1.5), which was correlated with the higher expressions of vascular endothelial growth factor and bone morphogenetic protein 2. Additionally, rADSCs on both units maintained osteogenic activity after storage at -80 °C for 20 d. In rat skull defect (diameter of 8 mm) models, rADSC-loaded BPLG-H(3.5) units fixed using gelatin hydrogel (ADSC@BHM) exhibited 84.1 ± 6.6% BV/TV after implantation for 12 weeks, which was 155.6% higher than that of the Blank group. H&E and Masson's staining results demonstrated that there was more bone regeneration at the defect center of ADSC@BHM than in the BHM and Blank groups. In conclusion, rADSC-loaded BPLG-H(3.5) with an osteon-mimic structure provides a potential strategy to repair bone defects.

CAS / MDL: 920-66-1
研究领域: 组织工程 · 再生医学 · 生物材料科学 · 生物医学工程
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Journal of Extracellular Vesicles · 2025 ·Vol. 14 ·期 9 ·e70162 · IF 14.5

Targeted Blockage of Pathological Extracellular Vesicles and Particles From Fibroblast-Like Synoviocytes for Osteoarthritis Relief: Proteomic Analysis and Cellular Effect

Bin Liu,Yansi Xian,Tao Shen,Yu Ben,Wenshu Wu,Yong Shi,Xueying An,Rui Peng,Wentian Gao,Wang Gong,Xiang Chen,Baosheng Guo,Qing Jiang

Osteoarthritis (OA), the prevalent debilitating joint disorder, is accelerated by dysregulated intercellular crosstalk, yet the role of fibroblast-like synoviocyte (FLS)-derived extracellular vesicles and particles (EVPs) in disease progression remains to be elucidated. Here, integrative analysis of clinical specimens, animal models, and publicly available datasets revealed significant alterations in exosomal pathways within OA synovium. Proteomic profiling revealed distinct molecular signatures in EVPs derived from inflammatory and senescent FLSs, reflecting the pathophysiological status of their parent cells. We demonstrated that FLSs under inflammatory and senescent states in OA secreted pathogenic EVPs that propagated joint degeneration by disrupting chondrocyte homeostasis, polarizing macrophages towards a pro-inflammatory phenotype, and impairing chondrogenesis of mesenchymal stem cells. To therapeutically target these pathogenic EVPs, we engineered an adeno-associated virus 9 (AAV9) vector fused with a synovium-affinity peptide (HAP-1) to deliver shRNA against Rab27a , a key regulator of EVP secretion. Intra-articular administration of the engineered AAV9 in a murine OA model induced by destabilization of the medical meniscus significantly reduced synovial hyperplasia, cartilage degradation and inflammatory responses, while demonstrating satisfactory systemic biosafety. Our findings establish FLS-derived EVPs as critical mediators of OA pathogenesis and propose a targeted strategy to block their secretion, offering a promising disease-modifying therapeutic avenue for OA. Graphical Osteoarthritis (OA) progression involves pathogenic extracellular vesicles and particles (EVPs) from inflamed/senescent fibroblast-like synoviocytes (FLSs). Proteomic profiling revealed that pathogenic EVPs contribute to OA progression by disrupting the homeostasis of macrophages, chondrocytes and mesenchymal stem cells. Targeted inhibition of FLS-derived exosomes effectively alleviated OA progression with good biosafety.

CAS / MDL: 8002-74-2
研究领域: 分子生物学 · 生物化学 · 细胞生物学 · 蛋白质组学 · 基因治疗 · 病毒学 · 免疫学 · 风湿病学 · 生物医学工程
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY · 2017 · IF 2.764

Bilayered HA/CS/PEGDA hydrogel with good biocompatibility and self-healing property for potential application in osteochondral defect repair

Baihao You,Qingtao Li,Hua Dong,Tao Huang,Xiaodong Cao,Hua Liao

The fabrication of osteochondral tissue engineering scaffolds comprised of different layers is a big challenge. Herein, bilayers comprised of double network hydrogels with or without nano hydroxyapatite (HAp) were developed by exploiting the radical reaction of poly(ethylene glycol) diacrylate (PEGDA) and the Schiff-base reaction of N-carboxyethyl chitosan (CEC) and oxidized hyaluronic acid sodium (OHA) for osteochondral tissue engineering. The bilayered osteochondral scaffold was successfully fabricated based on the superior self-healing property of both hydrogels and evaluated by scanning electron microscopy, macroscopic observation and mechanical measurements. In addition, the hydrogels exhibited good biocompatibility as demonstrated by the in vitro cytotoxicity and in vivo implantation tests. The results indicated that the bilayered hydrogel had great potential for application in osteochondral tissue engineering.

CAS / MDL: 1306-06-5 12167-74-7
研究领域: 材料科学 · 生物医学工程 · 组织工程 · 生物材料
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Acta Biomaterialia · 2024 · IF 9.4

Bioinspired Janus Mesh with Mechanical Support and Side-specific Biofunctions for Hernia Repair

Xiaoli Han,Zhenliang Liu,Liwei Sun,Zexiang Li,Yanhong Dong,Lu Zhou,Lingwan Hao,Jie Zhao,Rujian Jiang

Postoperative adhesion (PA) caused by the combination of proteins, inflammatory response and bacterial infection poses substantial challenges for polypropylene meshes (PPMs) based hernioplasty. Herein, inspired by the peritoneum, a Janus PPMs with side-specific functions was developed via a surface-initiated photoiniferter-mediated polymerization technology. A physical barrier composed of zwitterionic polymer brushes (PS) was firstly constructed on the one side of the PPMs, while the polymethacrylic acid (PMAA) brushes acting as the linker for bioactive nanoparticles (HAP) were precisely situated on the opposite surface subsequently. Our findings reveal that the mesh surface modified with PS demonstrated significant antifouling property that more than 99% of protein adhesion could be inhibited even after the co-incubation for 72 h in the crucial test. Meanwhile, on the other surface of the PPMs modified with HAP achieved satisfactory ROS-scavenging, inflammation-inhibiting and cell adhesion-promoting properties as well as good bactericidal performance (killing rate > 99.9%). Furthermore, the Janus PPMs could maintain comparable mechanical property with pristine meshes. Equipped with the above multiple merits and asymmetric property, the constructed Janus PPMs demonstrated effective treatment for abdominal hernia defects in vivo without any PA formation. Overall, this study duplicates the unique characteristics of peritoneum onto PPMs to successfully address postoperative complications of the hernioplasty and also offers a versatile and innovative idea to construct asymmetrical functions on the one implant. Statement of Significance The implantation of surgical meshes in the hernia defect provides additional firm support to reinforce the abdomen fascia in tension-free way. However, multiple post-surgery complications induced tissue adhesions is of great challenges for commercial mesh-based hernioplasty. Although material designing and surface modification might circumvent these limitations partly, the construction of side-specific biofunctions on the commercial mesh surfaces is very challenging because of its porous structure. Herein, we demonstrate a feasible and promising approach to construct asymmetric biofunctions on the opposite sides of network structured polypropylene mesh, which is rarely achieved previously. The fabricated Janus PPMs maintains the inherent long-term mechanical support; meanwhile, the opposite sides of PPMs could perform multiple biofunctions independently.

CAS / MDL: 1898-66-4
研究领域: 生物材料 · 组织工程 · 外科植入物 · 聚合物化学 · 生物医学工程
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Applied Materials Today · 2024 · IF 7.2

Injectable foam-like scaffolds release glucose oxidase-integrated metal–organic framework hybrids for diabetic bone defects

Yan Gong,Yuci Gan,Pei Wang,Chuchen Gong,Bing Han,Peizhe Li,Enze Liu,Ziyou Yu,Lingling Sheng,Xiansong Wang

Diabetic bone defect repair remains a significant clinical challenge due to the impact of glucose fluctuations, reactive oxygen species (ROS) damage, and the inflammatory microenvironment, all of which impede the normal bone repair process. In this study, we have developed a biological scaffold material aimed at localized regulation of the diabetic microenvironment within bone defect sites. Our approach involves the creation of an injectable, UV-curable, gas-foamed multifunctional hydrogel, incorporating methacrylic anhydride gelatine (GelMA) and hydroxyapatite nanowires (HAP NWs). This hydrogel is further enhanced with Gallic acid and magnesium ion (Mg²⁺) metal-organic frameworks (MOF) loaded with glucose oxidase (GOx), forming the GOx-MOF/HAP-GelMA composite. It can be injected and immediately cured to assume various customized shapes, while maintaining desirable hardness. It's noteworthy that the controlled release of Gallic acid within GOx-MOF actively engages in a cascade reaction, efficiently eliminating the H 2 O 2 generated by GOx-catalyzed glucose decomposition, thus optimizing the benefits of GOx while minimizing potential harm. The developed composite demonstrates remarkable capabilities in blood sugar regulation, ROS elimination, inflammation modulation, and the facilitation of osteogenesis and angiogenesis. This study represents a major step in precisely controlling the microenvironment for diabetic bone regeneration and provides a minimally invasive solution for addressing bone defects.

研究领域: 生物医学工程 · 材料科学 · 再生医学 · 组织工程 · 糖尿病研究
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