Chemical Science
·
2024
·Vol. 15
·期 24
·9173-9182
·
IF 7.6
Jiye Feng,Wenbiao Zhang,Danni Shi,Yingshuai Jia,Yi Tang,Yuying Meng,Qingsheng Gao
Multi-phase interfaces are promising for surmounting the energy barriers of electrochemical CO2 reduction involving multiple electron transfer steps, but challenges still remain in constructing interfacial micro-structures and unraveling their dynamic changes and working mechanism. Herein, highly active Ag/Cu/Cu2O heterostructures are in situ electrochemically restructured from Ag-incorporating HKUST-1, a Cu-based metal–organic framework (MOF), and accomplish efficient CO2-to-C2H4 conversion with a high faradaic efficiency (57.2% at −1.3 V vs. RHE) and satisfactory stability in flow cells, performing among the best of recently reported MOFs and their derivatives. The combination of in/ex situ characterizations and theoretical calculations reveals that Ag plays a crucial role in stabilizing Cu(I) and increasing the CO surface coverage, while the active Cu/Cu2O interfaces significantly reduce the energy barrier of C–C coupling toward the boosted ethylene production. This work not only proves MOFs as feasible precursors to derive efficient electrocatalysts on site, but also provides in-depth understanding on the working interfaces at an atomic level.
研究领域:
材料科学
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电化学
·
催化
·
能量转换
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DOI
PubMed
高影响因子
DYES AND PIGMENTS
·
2021
·
IF 4.889
Shijun Lin,Shuwen Liu,Guofei Dai,Xiaojin Zhang,Fan Xia,Yu Dai
Gold nanoparticles (AuNPs), as one of the major tools of fluorescence-quenching sensors, have been widely used in biochemical analysis through fluorescence resonance energy transfer (FRET) effect. With the development of chemistry and biochemistry, reaction-based fluorescent sensors have attracted increasing attention because of their unique selectivity, high sensitivity and rapid detection. Here we report a click-induced fluorescence-quenching sensor based on AuNPs for detection of copper ion (Cu 2+ ) and ascorbic acid (AA). A fluorescent dye Rhodamine B-(CH 2 CH 2 O) 4 -azide (RB-PEG 4 -N 3 ) is conjugated to the surface of AuNPs via Cu(I)-catalyzed azide-alkyne cycloaddition (CuAAC) in the presence of Cu 2+ and AA, leading to the fluorescence quenching of Rhodamine B. The sensor responds quickly (within less than 3 min). The fluorescent intensity linearly correlates with the concentration of Cu 2+ in the range of 0–108 μM. The limit of detection (LOD) for Cu 2+ is 5.8 μM. The concentration range for detection of AA is 0–3 mM. The LOD for AA is 0.13 mM. In addition, the application of the sensor is verified by performing detection in real samples such as fresh orange, juice, VC tablet, and lake water. This work expands the application of AuNPs-based fluorescence-quenching sensors for multi-component detection.
研究领域:
化学
·
生物化学
·
纳米技术
·
分析化学
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DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2018
·
IF 5.667
Lingli Lei,Wenyue Xie,Zhaoyang Chen,Ying Jiang,Yingshuai Liu
A novel colorimetric immunoassay strategy is developed based on metal ion chelation-induced color generation and alkaline phosphatase(ALP)-catalyzed signal amplification. The intense purple-colored Cu(I)-bicinchoninic acid (BCA) complex is utilized as a promising chromogenic reporter for the visual ALP-linked immunoassay. In the presence of target, ALP is introduced to catalyze the cascade conversion of L-ascorbic acid 2-phosphate (AAO) to L-ascorbic acid (AA), which results in Cu 2+ reduction to Cu + and subsequently in situ formation of purple-colored Cu(I)-BCA complex. The complex is water-soluble and exhibits a strong absorbance at 562 nm due to the ligand-to-metal charge-transfer (LMCT). The absorbance value is in turn proportional to the level of target analyte. Based on this concept, an ALP-linked colorimetric immunoassay is established with Cu(II)-BCA mixture as a color developing reagent for rabbit IgG detection, achieving a linear range from 0.1 ng mL −1 to 25 ng mL −1 and a LOD of 0.05 ng mL −1 . Its potentiality for practical application is also investigated by detection of a cancer biomarker, prostate specific antigen (PSA), in spiked human serum. A linear range from 0.5 ng mL −1 to 25 ng mL −1 and a LOD at 0.38 ng mL −1 are achieved, which is much lower than the cut-off value of PSA in human blood. The proposed method holds many advantages including low cost, good color stability, reliability and excellent compatibility with the existing ELISA platform, providing a promising colorimetric immunoassay platform for bio-chemical analysis in a variety of fields.
研究领域:
分析化学
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生物化学
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免疫学
·
医学诊断
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产品关联
DOI
高影响因子
TETRAHEDRON
·
2014
·
IF 2.817
Dazhuang Miao,Xuesong Shi,Guozhen He,Yao Tong,Zengqiang Jiang,Shiqing Han
N -(2-Chloro-phenyl)-2-halo-benzamides (halo=I/Br/Cl) as substrates were used for the one-pot synthesis of 2-arylbenzoxazole derivatives via copper-catalyzed intermolecular C–N/intramolecular C–O couplings with primary amines . This aryl amination offers clean reaction conditions and easy work-up in good yields by using CuI as catalyst, readily available 8-hydroxyquinoline as ligand, K 3 PO 4 as base, DMF as solvent.
研究领域:
有机化学
·
合成化学
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DOI
高影响因子
Catalysis Science & Technology
·
2020
·Vol. 10
·期 23
·8094-8107
·
IF 5.721
Yonghai Feng,Congming Lu,Huijie Wang,Minjia Meng,Yunlei Zhang,Dewei Rao,Lei Liu,Hengbo Yin
The aerobic catalytic oxidation of 1,2-propanediol (PDO) over non-noble metal (e.g. Cu) based catalysts usually suffers serious C3 product dissociation at high temperature, thus showing low lactic acid (LA) selectivity. Here, an alternative anaerobic catalysis strategy over spinel copper–iron-oxide magnetic nanoparticles (CuFeOx MNs) with the coexistence of Cu(I) and Cu(II) dual sites is developed for the catalytic transformation of PDO to LA with a quantitative yield of co-product H2 in basic aqueous solution. The absence of O2 is beneficial for enhancing LA production in comparison with the presence of O2. The synergy between Cu(I) and Cu(II) sites in CuFeOx MNs is vital for improving the catalytic performance as compared to Cu2O or CuO catalysts with Cu(I) or Cu(II) sites alone. Cu1Fe1Ox MNs with a Cu/Fe mole ratio of 1/1 exhibit 94.5% LA selectivity and 72.6% PDO conversion at 160 °C for 8 h. Experimental results and DFT calculations suggest that the spinel CuFeOx MN based catalytic PDO transformation follows a favorable pathway of PDO → hydroxyacetone → lactaldehyde → lactic acid for LA production. In addition to the catalytic PDO transformation, the use of CuFeOx MNs can be extended to favor high activity and selectivity in the catalytic transformation of glycerol to LA (98.5% selectivity) and ethylene glycol to glyceric acid (97.8% selectivity). This work highlights the design of an alternative non-noble metal-based CuFeOx MN catalyst for efficiently catalyzing the transformation of bio-based polyols into value-added carboxylic acids.
研究领域:
化学
·
材料科学
·
环境科学
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DOI
高影响因子
Advanced Science
·
2025
·
IF 14.1
Shengji Yuan,Hui Peng,Hairui Zhang,Ou Xu,Fei Wang,Wenchao Yang,Zhentao Du,Bingsuo Zou
Regarding global energy scarcity issues, it is imperative to establish sustainable plant production systems to promote smart agriculture. Addressing the critical demands of plant lighting and X-ray imaging in smart agriculture, a recyclable luminescent flexible film is developed on a filter paper and organic Cu(I) metal iodide, and establishes a bifunctional platform integrating plant growth lighting and plant root X-ray imaging. Specifically, [Ca(15-crown-5) 2 ]Cu 4 I 6 ·2C 3 H 7 NO·H 2 O and [Ca 2 (18-crown-6) 4 ]Cu 4 I 8 ·6H 2 O are synthesized through supramolecular assembly, which show yellow emission with the near-unity luminous efficiency under 450 nm excitation. Moreover, organic Cu(I) iodides exhibit bright X-ray radioluminescence with a maximum light yield of 110200 photons per MeV. Subsequently, a paper-based customizable large-area flexible film is prepared in situ through “ancient cloth dyeing process”, and demonstrates its application in single-component white light emitting diode and X-ray imaging. Combined white light and X-ray image fusion as well as multiangle imaging, the flexible film in the application of 3D image reconstruction is demonstrated. Furthermore, the flexible film can be recycled and reused in a N, N-dimethylformamide solution while maintaining excellent stability. Considering that the flexible film can be degraded by microorganisms in natural soil into plant nutrients and participate in the carbon loop, it is conducive to achieving carbon neutrality.
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DOI
PubMed
高影响因子
Signal Transduction and Targeted Therapy
·
2025
·Vol. 10
·期 1
·1-18
·
IF 52.7
Yue Yan,Li Shuoyuan,Su Qiang,Wan Xufeng,Li Qiaochu,Zhang Zhuang,Xu Hong,Zheng Fuyuan,Zhang Yangming,Tong Le,Cao Jian,Zhao Long,Chen Xiaoting,Li Qi,Zeng Yi,Wang Haoyang,Deng Yi,Zhou Zongke,Wang Duan
Conventional antibiotic strategies often fail to consistently suppress escaping planktonic bacteria and even induce antibiotic resistance, allowing implant-associated infections (IAIs) to persist. In this study, we demonstrated an antibiotic-free coating engineered with an herbal bioheterojunction featuring a shell-in-shell structure where Cu 2 O forms the core, strontium (Sr) is loaded in the inner shell, and curcumin (Cur) is nucleated in situ at the outer heterointerface (Cu 2 O-Sr/Cur). Ultrasound-triggered reactive oxygen species (ROS) generation by the outer heterostructure (Cu 2 O/Cur), coupled with Cu(I)-induced cuproptosis-like bacterial death, achieved antibacterial rates of 99.56% against S. aureus and 99.43% against E. coli . When ultrasonication ceases, the released Cu(I) undergoes disproportionation reactions to form Cu(II), which can chelate with Cur to form Cu-Cur metal complexes. These complexes exhibit enhanced antioxidative properties through self-catalytic regulation, the scavenging of ROS, and the activation of anti-inflammatory M2 macrophage phenotype. Moreover, strontium release from the inner shell simultaneously suppressed osteoclast activity and promoted osteogenesis, resulting in trabecular number and thickness increases of 129.03% and 56.71%, respectively, compared with those in control group. Therefore, our work establishes a sequential treatment strategy for the antibacterial properties and osteointegration ability of IAIs.
研究领域:
生物医学工程
·
抗菌材料
·
纳米医学
·
生物材料
·
感染控制
·
骨组织工程
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产品关联
DOI
PubMed
高影响因子
ANALYTICAL CHEMISTRY
·
2021
·
IF 6.986
Xianlong Zhang,Yongning Wu,Juhong Chen,Yan Yang,Guoliang Li
The copper(I)-catalyzed azide–alkyne cycloaddition (CuAAC) click reaction has drawn increasing attention in the field of analytical science. However, the poor stability of Cu(I) usually hinders not only the simplicity of the click reaction but also its applications in precise analyses. Therefore, the development of a nanocatalyst containing stable Cu(I) is of great significance for broadening the application of CuAAC-based assays. Herein, inspired by the active center structure of natural multicopper oxidases (MCOs), we successfully prepared a novel nanocatalyst containing abundant stable Cu(I) as an artificial “clickase” (namely, CCN) by using glutathione to stabilize Cu(I). The stability and enzyme-like catalytic activity in the CuAAC reaction of the prepared CCN clickase were studied, and the catalytic mechanism of the CCN clickase-mediated CuAAC reaction between 3-azide-7-hydroxycoumarin (Azide 1) and propargyl alcohol (Alkyne 2) was also revealed. Compared with the existing solid CuO nanocatalysts used in CuAAC-based assays, CCN clickases exhibited plenty of superior properties (including high stability, excellent catalytic activity, no requirements of dissolution and reducing agents/radical initiator during the detection, well-defined porosities benefiting the substrate diffusion, and good biocompatibility), which can greatly increase the reaction efficiency and shorten the detection time. Encouraged by these remarkable performances, CCN clickases were used as labels to establish a new catalytic click fluorescence immunoassay for foodborne pathogens. Notably, the proposed CCN clickase-based immunoassay exhibited high analytical performances for the quantification of Salmonella enteritidis in the linear range of 102–106 CFU/mL with a limit of detection as low as 11 CFU/mL. The developed method has also been used in the determination of S. enteritidis in food samples, showing its great potential in the detection of foodborne pathogens.
研究领域:
分析化学
·
纳米技术
·
免疫学
·
食品安全
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DOI
PubMed
高影响因子
Small
·
2023
·Vol. 19
·期 25
·2300938
·
IF 13.3
Jian Chen,Xin Pan,Xuanyu Zhang,Chen Sun,Congcong Chen,Xiaoqin Ji,Rui Chen,Lingling Mao
Chiral organic−inorganic hybrid metal halide materials have shown great potential for circularly polarized luminescence (CPL) related applications for their tunable structures and efficient emissions. Here, this work combines the highly emissive Cu 4 I 4 cubane cluster with chiral organic ligand R / S -3-quinuclidinol, to construct a new type of 1D Cu-I chains, namely Cu 4 I 4 ( R / S -3-quinuclidinol) 3 , crystallizing in noncentrosymmetric monoclinic P 2 1 space group. These enantiomorphic hybrids exhibit long-term stability and show bright yellow emission with a photoluminescence quantum yield (PLQY) close to 100%. Due to the successful chirality transfer from the chiral ligands to the inorganic backbone, the enantiomers show intriguing chiroptical properties, such as circular dichroism (CD) and CPL. The CPL dissymmetry factor ( g lum ) is measured to be ≈4 × 10 −3 . Time-resolved photoluminescence (PL) measurements show long averaged decay lifetime up to 10 µs. The structural details within the Cu 4 I 4 reveal the chiral nature of these basic building units, which are significantly different than in the achiral case. This discovery provides new structural insights for the design of high performance CPL materials and their applications in light emitting devices.
研究领域:
材料科学
·
光电
·
光子学
·
无机化学
·
有机-无机杂化材料
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DOI
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 14
·40534-40550
·
IF 5.8
Fang Lei,Wu Guojian,Yao Keyu,Zhang Dongyang,Zhou Yongchao
A novel heterogeneous catalyst named MoS 2 /MIL-53(Fe, Cu) (MMFC) was prepared by hydrothermal method and applied in a heterogeneous electro-Fenton (hetero-EF) system for lomefloxacin (LOM) degradation in this work. Under the optimal conditions of current density 3 mA/cm 2 , catalyst dosage 0.100 g/L, and initial pH 6, 93.5% LOM (2 mg/L) removal efficiency was achieved in the MMFC hetero-EF system within 60 min, indicating an obvious improvement compared with the MIL-53(Fe, Cu) hetero-EF system. The good catalytic activity was attributed to more effective active sites of the catalyst and the conversion of Fe(II)/Fe(III) and Cu(I)/Cu(II) promoted by Mo(IV) in MoS 2 , which could be inferred by scanning electron microscopy (SEM), transmission electron microscopy (TEM), and X-ray photoelectron spectroscopy (XPS) characterizations. The reusability and stability of MMFC were explored based on five cyclic experiments, and the average degradation efficiency reached 73.9%. Furthermore, the hetero-EF system could achieve the total removal of moxifloxacin and tetracycline within 6 min and 40 min, respectively. Quenching experiments revealed that the hydroxyl radicals (·OH) were the main reactive radicals while superoxide radicals (·O 2 − ) and singlet oxygen ( 1 O 2 ) played a certain part in LOM degradation. Finally, the possible mechanism of the hetero-EF process and LOM degradation pathways were proposed, including substitution, elimination, and cleavage of ring structures. Accounting for good catalytic performance, low preparation cost, and satisfactory versatility, the MMFC exhibited good potential to work as a hetero-EF catalyst for wastewater treatment.
研究领域:
环境科学
·
化学工程
·
材料科学
·
废水处理
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2016
·Vol. 27
·期 9
·9278-9285
·
IF 1.798
Liu Ziyu,Xu Guangliang,Zhang Ming,Xiong Kun,Meng Pingyuan
Cobalt ferrite/reduced graphene oxide (CoFe 2 O 4 /RGO) nanocomposites were initially prepared by the interaction of alkyne-functionalized CoFe 2 O 4 NPs and azide-functionalized graphene oxide (GO–N 3 ) via the Cu (I)-catalyzed click reaction. The morphology and structure of CoFe 2 O 4 /RGO were investigated by means of XRD, FTIR, TGA, TEM, SEM and the electromagnetic parameters were measured by vector network analyzer. For CoFe 2 O 4 /RGO composites with click reaction, the minimum reflection loss could reach −40 dB at 6.8 GHz with a matching thickness of 4.0 mm, and also it had a bandwidth below −10 dB ranging from 5.8 to 8.5 GHz. The CoFe 2 O 4 /RGO composites with click reaction exhibited better microwave absorbing performance than the physical mixture. Furthermore, the covalent ligation between CoFe 2 O 4 NPs and graphene oxide could make the composites have a promising future in electromagnetic wave absorption materials.
研究领域:
材料科学
·
纳米技术
·
电磁材料
·
化学
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产品关联
DOI
高影响因子
Acta Biomaterialia
·
2019
·
IF 6.638
Jingdong Rao,Ling Mei,Ji Liu,Xian Tang,Sheng Yin,Chunyu Xia,Jiaojie Wei,Dandan Wan,Xuhui Wang,Yashi Wang,Man Li,Zhirong Zhang,Qin He
Autophagy plays a key role in the stress response of tumor cells, which contributes to cancer cell survival and resistance to chemotherapy by degrading cytoplasmic proteins to provide energy and clear the hazardous substances. Therefore, combined treatment of chemotherapeutics and autophagy inhibitors is thought to obtain a desirable antitumor effect. Nanoparticles (NPs) show potential in tumor-targeting drug delivery because of the enhanced permeability and retention (EPR) effect. However, NPs with fixed particle size cannot achieve optimal delivery effect. Herein, a strategy based on Cu (I)-catalyzed click chemistry-triggered aggregation of azide/alkyne-modified micelles was developed for the co-delivery of the chemotherapeutic drug doxorubicin (Dox) and the autophagy inhibitor wortmannin (Wtmn). In vitro experiments showed that the size of micelles increased in a time-dependent manner, which enhanced micelle accumulation in both B16F10 and 4 T1 cells. The fluorescence resonance energy transfer (FRET) experiment and biodistribution study further demonstrated that the aggregation of micelles through click cycloaddition significantly improved the accumulation of drug-loading micelles at the tumor region. Furthermore, the decreased amount of autophagosomes observed by transmission electron microscopy (TEM), the declined expression of LC3-II, and the increased level of p62 by western blotting and immunohistochemistry (IHC) confirmed the obvious inhibition of autophagy induced by Dox/Wtmn co-loaded size-adjustable micelles, which had a synergistic effect in cancer suppression. In addition, the co-loaded size-adjustable micelles showed outstanding cytotoxicity and antitumor effect. Therefore, this strategy effectively suppressed melanoma and breast cancer in mice. Statement of Significance The therapeutic effects of chemotherapy can be limited by autophagy; hence, combined use of autophagy inhibitors with chemotherapeutics achieves desirable anticancer efficacy. In the present study, we designed size-adjustable micelles by modifying the click reaction substrate azide group and the alkyne group on the surface of micelles, and subsequently, the autophagy inhibitor wortmannin and the chemotherapeutic drug doxorubicin were co-loaded. The micelles could aggregate by click reaction at the tumor site when the catalysts were intratumorally injected. The results showed that the size-adjustable micelles achieved efficient drug delivery, penetration, and retention in tumors; through the combined effect of wortmannin-mediated autophagy inhibition and doxorubicin-mediated cytotoxicity, this strategy exerted significant anticancer effect in melanoma and breast cancer treatment.
研究领域:
药学
·
纳米技术
·
肿瘤学
·
生物医学工程
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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）