Journal of Functional Biomaterials
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2022
·Vol. 13
·期 4
·220
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IF 4.901
Wenhsuan Lu,Conglei Li,Jian Wu,Zhongshi Ma,Yadong Zhang,Tianyi Xin,Xiaomo Liu,Si Chen
Here, we developed a new synthetic method for the production of a new class of polymeric inorganic hybrid biomaterial that has potential for dental implant applications and, in general, other orthopedic applications owing to its excellent mechanical properties and biomechanical compatibility. The new hybrid biomaterial is a composite consisting of polyetherketoneketone (PEKK) and hydroxyapatite (HA). This hybrid material boasts several unique features, including its high HA loading (up to 50 wt%), which is close to that of natural human bone; the homogeneous HA distribution in the PEKK matrix without phase separation; and the fact that the addition of HA has no effect on the molecular weight of PEKK. Nanoindentation analysis was used to investigate the mechanical properties of the composite, and its nano/microstructure variations were investigated through a structural model developed here. Through nanoindentation technology, the newly developed PEKK/HA hybrid biomaterial has an indentation modulus of 12.1 ± 2.5 GPa and a hardness of 0.42 ± 0.09 GPa, which are comparable with those of human bone. Overall, the new PEKK/HA biomaterial exhibits excellent biomechanical compatibility and shows great promise for application to dental and orthopedic devices.Keywords:polyetherketoneketone;hydroxyapatite;composite;hybrid;dental;orthopedic;orthodontic;high performance;mechanical compatibility
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JOURNAL OF APPLIED POLYMER SCIENCE
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2022
·Vol. 139
·期 43
·e53061
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IF 3.057
Binglun Gao,Lianwei Sun,Xin Chen,Xiaobo Zhai,Junchi Zheng,Xin Ye,Jianmin Lu,Anchao Feng,Liqun Zhang
The focus of this paper is to report the quantitative synthesis of bis-epoxy end functionalized polyisoprene (BETPI) macromonomers by anionic polymerization and reversible addition fragmentation chain transfer (RAFT) polymerization. For anionic polymerization, more stable and sterically hindered living anions polyisoprene (Li + -PIp-Li + ) react with epichlorohydrin (ECH) for the synthesis of well-defined BETPI. For the high-pressure RAFT polymerization, a novel bis-epoxy end functionalized trithiocarbonate (BODAAT) is designed as RAFT agent for the polymerization of isoprene monomer to obtain well-defined BETPI. The functionalities of the resulting BETPI are analyzed by Fourier transform infrared spectroscopy (FT-IR), NMR, and size exclusion chromatography (SEC). Through two polymerization methods, the BETPI with 600–1000 Da of molecular weight and over 75% of epoxy end capping rate is obtained, which can be further utilized as highly reactive liquid macromonomers.
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Nanomaterials
·
2022
·Vol. 12
·期 12
·2049
·
IF 5.719
Tianyu Gao,Jinwei Lin,Leilei Xu,Jianguo Guan
In living bodies, pH values, which are precisely regulated and closely associated with diseased cells, can act as an efficient biologically intrinsic indicator for future intelligent biomedicine microsystems. In this work, we have developed flask-like carbonaceous nanomotors (FCNMs), via loading Fe3O4nanoparticles (NPs) into a cavity, which exhibit a self-adaptive feature to a specific physiological pH by virtue of the pH-dependent dual enzyme-like activities of Fe3O4NPs. Specifically, the peroxidase-like activity of Fe3O4NPs in an acidic pH range, and the catalase-like activity in a near neutral and alkaline pH range, determine the products in the motion system (•OH, ions and O2), whose diffusions from the inner to the outside of the flask result in fluid movement providing the driving force for the movement of the FCNMs. Correspondingly, changes of the product concentrations and species in the physiological pH range (4.4–7.4) result, firstly, in velocity decrease and, then, with increase in pH, increase of the FCNMs occurs. Thanks to the non-linear velocity responsiveness, the FCNMs show intriguing pH taxis towards 6.8 (generally corresponding to the physiological pH in tumor microenvironments), where a maximum velocity appears. Furthermore, the superparamagnetic feature of the Fe3O4NPs simultaneously endows the FCNMs with the abilities to be magnetic-oriented and easily separated. This work could significantly increase the possibility of nanomotors for targeted therapy of tumors and next-generation biotechnological applications.Keywords:nanomotors;pH responsiveness;Fe3O4nanoparticles;dual enzyme-like activities;physiological pH chemotaxis
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ACS Catalysis
·
2022
·
IF 13.7
Liang Jiang,Guangyue Xu,Yao Fu
The conversion of lignin into value-added chemicals is one of the important ways for sustainable development. Herein, phytic acid, a biomass-derived chemical, was used as the phosphorus source and pore former to synthesize the AlPyOx support. After loading Ni, the Ni/AlPyOx catalysts were found to be highly active in the catalytic conversion of lignin model compounds to high-value-added chemicals under mild conditions. The benzyl phenyl ether (α-O-4 lignin model compound) could be completely converted into toluene and phenol with near-equivalent selectivity at 30 °C and 3 MPa H2. Diphenyl ether and 2-phenoxy-1-phenylethanol were also used as 4-O-5 and β-O-4 model compounds of lignin, respectively. The unique activity of Ni/AlP0.5Ox could be attributed to metallic Ni that interacts with AlP0.5Ox and the unique adsorption of substrates on the carrier. Lignin can also be degraded over Ni/AlP0.5Ox via selective cleavage of the C–O bond, and 26.60 wt % yield of identified monomers was obtained.
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Nanomaterials
·
2022
·Vol. 12
·期 11
·1896
·
IF 5.719
Qilin Mei,Han Xiao,Guomin Ding,Huizhi Liu,Chenglong Zhao,Rui Wang,Zhixiong Huang
Development of high-performance graphene-based microwave absorbing materials with low density and strong absorption is of great significance to solve the growing electromagnetic pollution. Herein, a controllable open-cell structure is introduced into graphene aerogels by the graphene oxide (GO) Pickering emulsion. The open-cell graphene aerogel (OCGA) with multiple microstructures shows a significantly enhanced microwave absorption ability without any additions. A high microwave absorption performance with the minimum value of reflection loss (RLmin) of −51.22 dB was achieved, while the material density was only 4.81 mg/cm3. Moreover, by means of centrifugation, the graphene cells were arranged by their diameter, and a gradient, open-cell graphene structure was first fabricated. Based on this unique structure, an amazing microwave absorption value of −62.58 dB was reached on a condition of ultra-low graphene content of 0.53 wt%. In our opinion, such excellent microwave absorption performance results from multiple reflection and well-matched impedance brought by the open-cell and gradient structure, respectively. In addition, the structural strength of the OCGA is greatly improved with a maximum increase of 167% due to the introduction of cell structure. Therefore, the OCGAs with the gradient structure can be an excellent candidate for lightweight, efficient microwave absorption materials.Keywords:ultralight graphene aerogels;open cell;gradient microstructure;various microwave absorption
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ACS Sustainable Chemistry & Engineering
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2022
·
IF 9.224
Heyu Li,Minghua Liu,Wenqi Zou,Yuancai Lv,Yifan Liu,Lihui Chen
In this study, Ni-metal–organic frameworks (MOFs) were used as precursors to obtain carbon-supported nickel composites (Ni@C) after calcination. The hydrodeoxygenation properties of the model compound and corncob lignin were investigated without an external hydrogenation source and initial pressure. Additionally, the effect of Ni@C on degradation of model compounds, corncob lignin, and benzyl phenyl ether (BPE) under different conditions was examined. The results showed that with isopropanol as the in situ hydrogen source, the conversion percentage of BPE was 90.2% and the yield of phenol was 88.3 wt % at 150 °C. The catalysts were characterized by scanning electron microscopy (SEM), X-ray diffraction (XRD), NH3 temperature-programmed desorption (NH3-TPD), X-ray photoelectron spectroscopy (XPS), and thermogravimetry (TG), and the lignin and bio-oil were characterized by gas chromatography–mass spectrometry (GC–MS) and two-dimensional heteronuclear single quantum coherence (2D-HSQC). It was found that the Ni@C catalyst with well dispersion, high support rate, and rich acid sites was successfully synthesized. In the process of degradation, the C–O ether bond in the structure of lignin was successfully broken to generate the phenolic monomer, and the high-efficiency hydrodeoxygenation of lignin was realized under mild conditions.
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SENSORS AND ACTUATORS B-CHEMICAL
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2022
·
IF 9.221
Yihan Wang,Jinfeng Quan,Jialei Zhang,Kejing Huang,Xuemei Wang,Hui Jiang
The fragments of molecular motors can be transported and operated autonomously along a track. Most molecular walker systems are assembled from DNA building modules, exhibiting great potential applications in biocomputing, drug transport, sensing, etc. Hereby, we report a DNA walker driven by endonuclease Nt.BbvC I that can autonomously induce “signal off” sensing platform for highly sensitive detection of tumor cells. DNA density and trajectory conformation can affect DNA walker properties. Molybdenum selenide@gold nanoparticles (MoSe 2 @AuNPs) are modified on the electrode surface as a scaffold to accommodate more hairpin probe (H1) and provide a good interface for DNA walking. Magnetic beads are used to enrich target tumor cells, release single-stranded DNA (S1) and trigger DNA walker-based amplification strategy. Upon addition of tumor cells, more DNA-methylene blue (DNA-MB) is cracked from the electrode surface. Benefiting from efficient electrode modification, magnetic enrichment, DNA walker and enzyme-assisted amplification, an ultra-high sensitivity electrochemical cell analysis is realized, with a detection limit of 2 cells mL −1 . More importantly, this DNA walker strategy is available for tumor cell analysis in clinical samples, suggesting the potential diagnostic applications.
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ACS Nano
·
2022
·
IF 18.027
Feng Wu,Yaqian Du,Jiani Yang,Boyang Shao,Zhensheng Mi,Yuanfei Yao,Ying Cui,Fei He,Yanqiao Zhang,Piaoping Yang
The nanocatalytic activity of nanozymes provides a vision for tumor treatment. However, the glutathione (GSH)-related antioxidant defense system (ADS) formed on the basis of excessive GSH in the tumor microenvironment limits its catalytic activity. Here, dendritic mesoporous silica nanoparticles (DMSNs) were employed as nanocarrier; ultrasmall Fe3O4 nanoparticles, Mn2+ ions, and glutaminase inhibitor Telaglenastat (CB-839) were subsequently integrated into large mesopores of DMSNs, forming DMSN/Fe3O4–Mn@CB-839 (DFMC) nanomedicine. This nanomedicine exhibits peroxidase mimicking activities under acidic conditions, which catalyzes the decomposition of hydrogen peroxide (H2O2) into hydroxyl radical (•OH). This also promotes the formation of lipid peroxides, which is required for ferroptosis. Furthermore, this nanomedicine can effectively deplete the existing GSH, thereby enhancing reactive oxygen species (ROS)-mediated tumor catalytic therapy. Moreover, the introduced CB-839 blocks the endogenous synthesis of GSH, further enhancing GSH depletion performance, which reduces the excretion of oxaliplatin (GSH-related resistance) from tumor cells, thereby restoring the chemical sensitivity of oxaliplatin. The dual GSH depletion property significantly weakens the GSH-related ADS and restores the chemical sensitivity of oxaliplatin, leading to the high DFMC-induced apoptosis and ferroptosis of tumor cells. Our developed nanomedicine based on integrated nanotechnology and clinical drug may aid the development of tumor treatment.
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FUEL
·
2022
·
IF 8.035
Zhi Yang,Bowen Luo,Riyang Shu,Zhuojie Zhong,Zhipeng Tian,Chao Wang,Ying Chen
Hydrodeoxygenation (HDO) is an indispensable reaction in the field of fuel and chemical production, and the synergistic effect of metal–acid sites in the catalyst makes great influence to it. Herein, a bifunctional catalyst of Ru/C combined with phosphotungstic acid (HPW) was employed for the hydrodeoxygenation (HDO) of lignin-derived compounds to make full use of the synergistic effect of active metal–acid sites. HPW possessed a temperature-controlled phase-transfer behavior, which made it dispersed well on the surface of Ru/C catalyst and resulted in a close integration of acid site with metal site. Ru/C-HPW catalyst also owned the advantage of high reaction rate and good recyclability, which exhibited no obvious catalytic activity loss after 5 runs. Lignin-derived phenolic compounds including monomers and dimers enabled to obtain an efficient transformation to cycloalkanes at the temperature of 200 °C. Moreover, a high HDO reaction efficiency of raw lignin-oil was also observed in this study, with the increasing hydrocarbon content from 5.5% to 78.9%. This novel catalytic system can achieve a high HDO efficiency under mild conditions.
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Journal of Materials Chemistry B
·
2022
·Vol. 10
·期 23
·4501-4508
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IF 7.571
Xi Xiao,Bingzhu Zheng,Qiang Zheng,Zijie Lu,Dong Cen,Xiujun Cai,Xiang Li,Renren Deng
Peroxynitrite anion (ONOO−), a product derived from reaction between reactive oxygen species (ROS) and nitric oxide (NO), is considered to be a more toxic reactive species than most ROS for cancer photodynamic therapy (PDT). To promote the PDT effect, a viable method is to develop rational strategies for efficient ONOO− generation at targeted tumor sites. Herein, a heterostructure nanocomposite containing ZnO-coated lanthanide nanoparticles (LnNPs) is reported for ONOO−-based PDT. In this nanocomposite, Nd3+-doped LnNPs are employed to realize efficient NIR-light-triggered ROS generation by activating the triplet state of chlorin-e6 (Ce6) photosensitizers via a direct lanthanide-to-triplet sensitization mechanism. Meanwhile, ZnO in the composite catalyzes the decomposition of S-nitrosoglutathione (GSNO) to generate NO in the tumor microenvironment. The coupled system allows the combination of photo-induced ROS and NO to produce ONOO−, leading to drastically promoted cancer cell apoptosis and tumor growth inhibition. This study establishes a new apoptosis-inducing PDT agent, which is potentially active in drug resistant malignancies.
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ACS Nano
·
2023
·
IF 17.1
Hongwei Liao,Shengfei Yang,Zeyu Liang,Lin Xiao,Shangzhi Xie,Peihua Lin,Fan Xia,Chunyan Fang,Qian Chen,Daishun Ling,Fangyuan Li
Replication stress (RS) induced by DNA damage plays a significant role in conferring the anticancer effects of radiotherapy and is tightly associated with radioresistance of cancer cells. Amplification of RS represents an effective approach to improving the efficacy of radiotherapy, although the development of selective RS amplifiers remains an unexplored frontier. We herein present an RS nano amplifier (RSNA) consisting of a catalytic FePt nanoparticle loaded with the chemotherapeutic doxorubicin (DOX), which selectively exacerbates RS in cancer cells by promoting replication fork (RF) catastrophe. RSNA converts the excessive reactive oxygen species (ROS) in cancer cells into oxygen, enhancing the DNA-damaging effects of radiotherapy to create more template lesions that impede RF progression in coalition with DOX. After radiation, ROS scavenging by RSNA accelerates RF progression through damaged template strands, increasing the frequency of RF collapse into double-strand breaks. Moreover, pretreatment with RSNA accumulates cancer cells in the S phase, exposing more RFs to radiation-induced RS. These effects of RSNA convergently maximize RS in cancer cells, effectively overcoming the radioresistance of cancer cells without affecting normal cells. Our study demonstrates the feasibility of selectively amplifying RS to boost radiotherapy.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Kaixu Yu,Ying Chen,Lu Zhang,Yongqiang Zheng,Jinlin Chen,Zhenhua Wang,Xiaogang Yu,Kehan Song,Yimin Dong,Fanxiu Xiong,Zijian Dong,Hao Zhu,Gaohong Sheng,Meipeng Zhu,Xi Yuan,Hanfeng Guan,Jiaqiang Xiong,Yi Liu,Feng Li
Ferroptosis is characterized by iron accumulation and lipid peroxidation. However, a clinical dose of Fe3O4 nanoparticles could not cause effective ferroptosis in tumors, and the mechanism is yet to be completely understood. In this study, using RNA-seq data, we found that tumor cells could feedback-activate the antioxidant system by upregulating Nrf-2 expression, thus avoiding ferroptosis caused by Fe3O4 nanoparticles. We also found that DHJS (a probe for ROS generation) can antagonize Nrf-2 expression when it synergizes with Fe3O4 nanoparticles, thus inducing ferroptosis in tumor cells. Considering these findings, we created a biomimetic hybrid cell membrane camouflaged by PLGA-loaded Fe3O4 and DHJS to treat osteosarcoma. The hybrid cell membrane endowed the core nanoparticle with the extension of blood circulation life and enhanced homologous targeting ability. In addition, DHJS and Fe3O4 in nanoparticles prompted synergistically lethal ferroptosis in cancer cells and induced macrophage M1 polarization as well as the infiltration of CD8(+) T cells and dendritic cells in tumors. In summary, this study provides novel mechanistic insights and practical strategies for ferroptosis induction of Fe3O4 nanoparticles. Meanwhile, the synthesized biomimetic nanoparticles exhibited synergistic ferroptosis/immunotherapy against osteosarcoma.
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