ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Liying Hao,Jikui Sun,Qingyin Wang,Haijiao Xie,Xiangui Yang,Qiang Wei
As an atom-economical reaction, the direct generation of dimethyl carbonate (DMC) and ethylene glycol (EG) via the transesterification of CH3OH and ethylene carbonate (EC) has several promising applications, but the exploration of carriers with high specific surface areas and novel heterogeneous catalysts with more basic sites remains a long-standing research challenge. For this purpose, herein, a nitrogen-doped mesoporous carbon (NMC, 439 m2/g) based K–O2 Lewis base catalyst (K–O2/NMC) with well-dispersed strongly basic sites (2.23 mmol/g, 84.5%) was designed and synthesized. The compositions and structures of NMC and K–O2/NMC were comprehensively investigated via Fourier transform infrared spectroscopy, X-ray diffraction, X-ray photoelectron spectroscopy, scanning electron microscopy, transmission electron microscopy, N2 adsorption–desorption, CO2 temperature-programmed desorption, and contact angle measurements. The optimal structural configuration and electron cloud distribution of the K–O2/NMC catalyst were simulated using first-principles calculations. The electron transfer predominantly manifested as a flow from K–O to C–O/C–N, and the interatomic interactions between each atom were enhanced and exhibited a tendency for a more stable state after redistribution. Furthermore, the adsorption energies (Eads) of CH3OH at K–O–O and K–O–N sites were −1.4185 eV and −1.3377 eV, respectively, and the O atom in CH3OH exhibited a stronger adsorption tendency for the K atom at the K–O–O site. Under the optimal conditions, the EC conversion, DMC/EG selectivity, and turnover number/frequency were 80.9%, 98.6%/99.4%, and 40.5/60.8 h–1, respectively, with a reaction rate constant (k) of 0.1005 mol/(L·min). Results showed that the heterogeneous K–O2/NMC catalyst prepared herein greatly reduced the reaction cost while guaranteeing the catalytic effect, and the whole system required a lower reaction temperature (65 °C), a shorter reaction time (40 min), and a lower catalyst amount (2.0 wt % of EC). Therefore, K–O2/NMC can be used as a catalyst in different transesterification reactions.
研究领域:
催化化学
·
材料科学
·
绿色化学
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产品关联
DOI
PubMed
高影响因子
Advanced Healthcare Materials
·
2024
·
IF 10
Ming-Xuan Liu,Yan-Chao Liu,Yu-Ting Cai,Ying-Ying Gu,Ya-Qi Zhu,Nan Zhang,Wei-Zhong Zhu,Yong-Hong Liu,Lei Yu,Qi-Tao Zhang,Xiao-Ling Zhang
Hypoxia can aggravate tumor occurrence, development, invasion, and metastasis, and greatly inhibit the photodynamic therapy (PDT) effect. Herein, carbon nitride (CNs)-based DNA and photosensitizer co-delivery systems (BPSCNs) with oxygen-producing functions are developed to address this problem. Selenide glucose (Seglu) is used as the dopant to prepare red/NIR-active CNs (SegluCNs). The tumor-targeting unit Bio-PEG 2000 is utilized to construct BPSCNs nanoparticles through esterification reactions. Furthermore, DNA hydrophobization is realized via mixing P53 gene with a positively charged mitochondrial-targeted near-infrared (NIR) emitting photosensitizer (MTTPY), which is encapsulated in non-cationic BPSCNs for synergistic delivery. Ester bonds in BPSCNs@MTTPY-P53 complexes can be disrupted by lipase in the liver to facilitate P53 release, upregulated P53 expression, and promoted HIF-1α degradation in mitochondria. In addition, the oxygen produced by the complexes improved the hypoxic microenvironment of hepatocellular carcinoma (HCC), synergistically downregulated HIF-1α expression in mitochondria, promoted mitochondrial-derived ferroptosis and enhanced the PDT effect of the MTTPY unit. Both in vivo and in vitro experiments indicated that the transfected P53-DNA, produced O 2 and ROS by these complexes synergistically led to mitochondrial-derived ferroptosis in hepatoma cells through the HIF-1α/SLC7A11 pathway, and completely avoiding PDT resistance caused by hypoxia, exerting a significant therapeutic role in HCC treatment.
研究领域:
癌症生物学
·
药学
·
生物医学工程
·
分子生物学
·
治疗学
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Leilei Hou,Siyang Yan,Liping Liu,Jiaxu Liu,Guang Xiong
The TS-1 microsphere was facilely prepared via a direct spray drying of the mixture containing the nanocrystal TS-1 and mother liquor. The calcined TS-1 zeolites possess a hollow structure and numerous intercrystalline mesopores, which may facilitate the diffusion properties. Au nanoparticles were loaded on TS-1 support by utilizing a deposition–precipitation process to prepare the Au/TS-1-M catalysts for propylene epoxidation in the presence of H 2 and O 2 conditions. The effects of the Ti and Au loadings on the structure, porosity, morphology, and catalytic performances of the Au/TS-1 catalysts have been investigated by various techniques. Under the optimized synthesis conditions (Si/Ti molar ratio = 57, 0.49 wt% Au), a propylene conversion of 6.1 % and a PO selectivity of 91.7 % were obtained on the Au/TS-1 catalyst. A PO formation rate of 186.8 g PO ·kg cat. −1 ·h −1 was achieved at the 20th hour.
研究领域:
材料科学
·
催化化学
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产品关联
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2024
·
IF 18.5
Xichen Sun,Pengfei Wang,Liuyan Tang,Ningning Li,Yan-Ru Lou,Yuezhou Zhang,Peng Li
An effective method capable of simultaneously providing antibacterial activity, blood glucose regulation, and angiogenesis promotion for healing bacteria-infected diabetic wounds is not reported to date, but urgently required. In this study, a hydrogel composite ( γ -PGA/PDA/GOx/WO x (PPGW)), endowed with these desired attributes is fabricated by incorporating polydopamine (PDA), glucose oxidase (GOx), and tungsten oxide (WO x ) nanowires into the poly( γ -glutamic acid) ( γ -PGA) framework. The exceptional photothermal conversion properties of PDA facilitated notable antibacterial effects on bacteria-infected diabetic wounds; GOx regulated high blood glucose by consuming glucose and generating hydrogen peroxide (H 2 O 2 ); while WO x nanowires displayed remarkable photocatalytic abilities, converting H 2 O 2 into oxygen (O 2 ) when exposed to 808-nm near-infrared radiation. Density functional theory calculations and experiments are conducted to confirm the mechanism of WO x -mediated photocatalytic degradation of H 2 O 2 to produce O 2 . These transformations aided in alleviating the hypoxic conditions in wounds associated with diabetes, expediting angiogenesis, and fostering cell crawling and proliferation. Consequently, the multifunctional hydrogel dressing PPGW, featuring photothermal, antibacterial, and enzyme-catalyzed activity reduces hyperglycemia at the wound site. Moreover, photocatalytic O 2 production represents a promising strategy for addressing chronic bacteria-infected diabetic wounds.
研究领域:
生物医学工程
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材料科学
·
糖尿病研究
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Xueyi Zhang,Wenshuang Sun,Yue Wang,Zhen Li,Xianqiang Huang,Tielong Li,Haitao Wang
In this study, we prepared a micron zero-valent iron/ N -doped graphene-like biochar (mZVI/NGB) composite using a mechanochemical method for tetracycline (TC) degradation through O 2 activation. The mZVI and NGB components formed a strong coupling catalytic system, with mZVI acting as an electron pool and NGB as a catalyst for H 2 O 2 generation. Under circumneutral pH (5.0–6.8), the mZVI/NGB composite exhibited exceptional TC removal efficiency, reaching nearly 100 % under optimal conditions. It also showed good tolerance to co-existing anions, such as Cl - , SO 4 2- , and humic acid. Further studies found that the TC degradation mechanism was mainly ascribed to the non-radical pathway ( 1 O 2 and electron transfer), and the Fe 2+ /Fe 3+ redox cycle on the composite's surface also played a crucial role in maintaining catalytic activity. This research contributes to the development of advanced materials for sustainable and effective water treatment, addressing pharmaceutical pollutant contamination in water sources.
研究领域:
环境科学
·
材料科学
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Jiahui He,Zhenlong Li,Jueying Chen,Jiaxin Wang,Lipeng Qiao,Baolin Guo,Juan Hu
It is still challenging to design stimuli-responsive smart hydrogel dressing to promote bacteria-infected diabetic wound healing from the whole healing stage by intelligently responding to external stimuli or wound microenvironment. In addition, nitric oxide (NO) and oxygen (O 2 ) have been shown to accelerate diabetic wound healing by promoting angiogenesis and alleviating hypoxia. A series of NIR/glucose stimuli-responsive multifunctional smart hydrogels with NO/O 2 dual gas-releasing properties was designed based on N-carboxyethyl chitosan-grafted-phenylboronic acid (CECP), oxidized dextran (OD), ε-polylysine (EPL)-coated manganese dioxide (EMn), and β-cyclodextrin-reduced graphene oxide/N, N’-di-sec-butyl-N, N’-dinitroso-1,4-phenylenediamine (rGB) via dual dynamic crosslinking to promote bacteria-infected diabetic wound healing. The added rGB and EMn as photothermal agents rapidly kill bacteria through photothermal therapy. Meanwhile, rGB endows CECP/OD/EMn/rGB hydrogels to release NO under NIR stimulation to promote angiogenesis. Nanozyme EMn with catalase (CAT)/superoxide dismutase (SOD)-like activity can scavenge ROS and release O 2 to alleviate hypoxia and oxidative stress. The phenylboronic acid in CECP forming phenylboronate ester structure endows hydrogel with glucose-controlled release of doxycycline. NIR/glucose stimuli-responsive CECP/OD/EMn/rGB hydrogels with NO/O 2 dual gas-releasing property in a full-thickness skin wound-infected diabetic model reduced the inflammation, promoted wound contraction, collagen deposition, angiogenesis, and alleviated wound hypoxia, providing new ideas for treating bacteria-infected diabetic wounds.
研究领域:
生物材料学
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医学工程
·
组织修复与再生
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产品关联
DOI
高影响因子
Journal of the American Chemical Society
·
2017
·
IF 13.858
Shuai Xu,Peng Zhou,Zehui Zhang,Changjun Yang,Bingguang Zhang,Kejian Deng,Steven Bottle,Huaiyong Zhu
Selective oxidation of 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) is one of the key reactions for producing chemical commodities from biomass and their derivatives. The challenge for this reaction is to develop an efficient catalytic process that can be conducted under mild conditions (room temperature and atmospheric pressure, using oxygen molecules in air as the oxidant) and a recyclable catalyst. Herein we report a photocatalyst of cobalt thioporphyrazine (CoPz) dispersed on g-C3N4 (abbreviated as CoPz/g-C3N4), which exhibits excellent catalytic activity toward the selective oxidation of HMF into FDCA under simulated sunlight using oxygen molecules in air as a benign oxidant. For example, an FDCA yield of 96.1% in an aqueous solution at pH = 9.18 is achieved at ambient temperature and air pressure. At lower pH (4.01), the product generated is 2,5-diformylfuran. Hence, it is possible to control the reaction outcome by control of the pH of the reaction system. g-C3N4 itself is not a suitable catalyst for the selective oxidation because under the experimental conditions g-C3N4 generates hydroxyl radicals that initiate processes that oxidize HMF directly to CO2 and H2O. CoPz on the other hand activates O2 to give singlet oxygen (1O2), which more controllably oxidizes HMF to FDCA albeit at a more moderate yield (36.2%). The strong interaction between the CoPz and g-C3N4 in the CoPz/g-C3N4 catalyst is experimentally evidenced, which not only improves accessibility of the CoPz sites and makes the catalyst recyclable but also disables the hydroxyl radical generation by g-C3N4 and promotes 1O2 generation on the CoPz sites, significantly enhancing the catalytic performance. This study demonstrates the potential for efficient non-noble metal photocatalysts for organic transformations driven by sunlight.
研究领域:
化学工程
·
催化科学
·
环境科学
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DOI
高影响因子
Small Methods
·
2022
·Vol. 6
·期 6
·2200178
·
IF 15.367
Rui Xu,Phei Er Saw,Lei Xu
Two-dimensional (2D) nanomaterials have attracted increasing attention in cancer theranostics due to their ultrahigh specific surface area resulting in more radicals and/or reactive oxygen species (ROS) generation in chemodynamic therapy (CDT). However, their biomedical prospects are greatly limited by poor biocompatibility, low dispersion, weak stability, and the potential threat of their high immunogenicity. Moreover, rapid depletion of ROS by the high level of antioxidants (e.g., glutathione) in cancer cells severely limits the therapeutic effects of cancer CDT. Herein, a robust method is developed to improve the biomedical application of 2D nanomaterials via constructing a 2D nanomaterials delivery nanoplatform with hemoglobin-based minerals biological coat for the safe encapsulation, long blood circulation, and controlled release of 2D nanomaterials. After intravenous administration and then internalization by cancer cells, the acidic microenvironment and high concentration of H 2 O 2 can trigger rapid release of Cu-T nanoscale metal-organic frameworks (nMOFs) from Cu-T@MH. Then, the released Cu-T nMOFs with simultaneous high ROS production and GSH depletion endow the Cu-T@MH nanoplatform with enhanced cancer CDT. Besides, the fluorescence recovery of tetrakis(4-carboxyphenyl) porphyrin in Cu-T nMOFs during the GSH depletion process can accurately visualize the cancer therapeutic action.
研究领域:
生物医学工程
·
肿瘤学
·
纳米医学
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DOI
PubMed
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2017
·Vol. 27
·期 43
·1700626
·
IF 12.124
Chi Zhang,Wei-Hai Chen,Li-Han Liu,Wen-Xiu Qiu,Wu-Yang Yu,Xian-Zheng Zhang
Conventional photodynamic therapy (PDT) has limited applications in clinical cancer therapy due to the insufficient O 2 supply, inefficient reactive oxygen species (ROS) generation, and low penetration depth of light. In this work, a multifunctional nanoplatform, upconversion nanoparticles (UCNPs)@TiO 2 @MnO 2 core/shell/sheet nanocomposites (UTMs), is designed and constructed to overcome these drawbacks by generating O 2 in situ, amplifying the content of singlet oxygen ( 1 O 2 ) and hydroxyl radical (•OH) via water-splitting, and utilizing 980 nm near-infrared (NIR) light to increase penetration depth. Once UTMs are accumulated at tumor site, intracellular H 2 O 2 is catalyzed by MnO 2 nanosheets to generate O 2 for improving oxygen-dependent PDT. Simultaneously, with the decomposition of MnO 2 nanosheets and 980 nm NIR irradiation, UCNPs can efficiently convert NIR to ultraviolet light to activate TiO 2 and generate toxic ROS for deep tumor therapy. In addition, UCNPs and decomposed Mn 2+ can be used for further upconversion luminescence and magnetic resonance imaging in tumor site. Both in vitro and in vivo experiments demonstrate that this nanoplatform can significantly improve PDT efficiency with tumor imaging capability, which will find great potential in the fight against tumor.
研究领域:
癌症治疗
·
纳米技术
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生物医学工程
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光化学
·
成像技术
✓ 已验证
DOI
高影响因子
Catalysts
·
2026
·Vol. 16
·期 4
·364
·
IF 4.5
Lihui Wang,Shao Zhang,Mingming Wang,Zhigang Wang,Xiaoyao Tan
The high-temperature proton ceramic membranes with simultaneous separation of hydrogen and oxygen exhibit promising applications in the catalytic conversion field. However, their separation performance often relies on external electrical circuits, which limits practical application. To overcome this limitation, doping strategies have emerged as a viable approach to develop triple-conducting (H+/e−/O2−) membranes for simultaneous hydrogen and oxygen separation in non-electrochemical mode. In this study, honeycomb-structured hollow fiber membranes were fabricated, and the effects of varying Fe3+and Y3+doping concentrations on hydrogen and oxygen permeation fluxes were systematically investigated. At the Fe3+doping level of 0.2 mol, the oxygen permeation flux of 0.692 mL min−1cm−2in BaCe0.6Zr0.2Fe0.2O3−δ(BCZF) was achieved at 1000 °C, while the hydrogen permeation flux was 0.201 mL min−1cm−2. The BaCe0.55Fe0.05Zr0.2Y0.2O3−δ(Fe-BCZY) hollow fiber membrane can enhance the hydrogen permeation flux by 75% at 1000 °C. Furthermore, during the simultaneous permeation of hydrogen and oxygen, a 1.7-fold enhancement in hydrogen permeation performance was achieved for the Fe-BZCY hollow fiber membrane at 1000 °C, and with oxygen permeation flux of 1.76 mL min−1cm−2at the same temperature. More significantly, a hydrogen permeation flux of 0.34 mL min−1cm−2can be achieved at 700 °C under simultaneous hydrogen and oxygen permeation, which is favorable for the application of membrane reactors in catalytic reactions.
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DOI
高影响因子
Batteries-Basel
·
2023
·Vol. 9
·期 5
·
IF 4
Ningning Feng,Chaoqiang Wang,Jing Wang,Yang Lin,Gang Yang
Lithium–oxygen (Li-O2) batteries have captured worldwide attention owing to their highest theoretical specific energy density. However, this promising system still suffers from huge discharge/charge overpotentials and poor cycling stability, which are related to the leakage/volatilization of organic liquid electrolytes and the inefficiency of solid catalysts. A mixing ionic liquid-based gel polymer electrolyte (IL-GPE)-based Li-O2battery, consisting of a 20 mM 2,5-di-tert-butyl-1,4-benzoquinone (DBBQ) 40 mM N-methylphenothiazine (MPT)-containing IL-GPE and a single-walled carbon nanotube cathode, is designed for the first time here. This unique dual redox mediators-based GPE, which contains a polymer matrix immersed with mixed ionic liquid electrolyte, provides a proper ionic conductivity (0.48 mS cm−1) and effective protection for lithium anode. In addition, DBBQ, as the catalyst for an oxygen reduction reaction, can support the growth of discharge products through the solution–phase pathway. Simultaneously, MPT, as the catalyst for an oxygen evolution reaction, can decompose Li2O2at low charge overpotentials. Hence, the DBBQ-MPT-IL-GPE-based Li-O2battery can operate for 100 cycles with lower charge/discharge overpotentials. This investigation may offer a promising method to realize high-efficiency Li-O2/air batteries.
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DOI
高影响因子
JOURNAL OF NANOBIOTECHNOLOGY
·
2024
·Vol. 22
·期 1
·1-15
·
IF 10.6
Li Jingchao,Wang Tingting,Shi Yuanfei,Ye Zichen,Zhang Xun,Ming Jiang,Zhang Yafei,Hu Xinyan,Li Yun,Zhang Dongsheng,Xu Qianhe,Yang Jun,Chen Xiaolan,Liu Nian,Su Xinhui
Radionuclides internal radiotherapy (RIT) is a clinically powerful method for cancer treatment, but still poses unsatisfactory therapeutic outcomes due to the hypoxic characteristic of tumor microenvironment (TME). Catalase (CAT) or CAT-like nanomaterials can be used to enzymatically decompose TME endogenous H 2 O 2 to boost TME oxygenation and thus alleviate the hypoxic level within tumors, but their effectiveness is still hindered by the short-lasting of hypoxia relief owing to their poor stability or degradability, thereby failing to match the long therapeutic duration of RIT. Herein, we proposed an innovative strategy of using facet-dependent CAT-like Pd-based two-dimensional (2D) nanoplatforms to continuously enhance RIT. Specifically, rationally designed 2D Pd@Au nanosheets (NSs) enable consistent enzymatic conversion of endogenous H 2 O 2 into O 2 to overcome hypoxia-induced RIT resistance. Furthermore, partially coated Au layer afford NIR-II responsiveness and moderate photothermal treatment that augmenting their enzymatic functionality. This approach with dual-effect paves the way for reshaping TME and consequently facilitating the brachytherapy ablation of cancer. Our work offers a significant advancement in the integration of catalytic nanomedicine and nuclear medicine, with the overarching goal of amplifying the clinical benefits of RIT-treated patients. Graphical abstract
研究领域:
肿瘤学
·
纳米医学
·
核医学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）