ANALYST
·
2023
·Vol. 148
·期 12
·2855-2860
·
IF 4.2
Bizhen Huang,Jing Ran,Ruishen Li,Wei Zhuang,Jiabi Chen,Haixin Guo
Early diagnosis of acute myocardial infarction (AMI) can significantly reduce mortality, which can be achieved by the highly sensitive detection of AMI-specific cardiac troponin I (cTnI) biomarkers. Herein a highly sensitive and portable photoelectrochemical (PEC) immunoassay for the detection of cTnI was innovatively fabricated based on an efficient photocurrent response of Cu2O coupling with a split-type enzymatic biocatalytic precipitation reaction with a digital multimeter readout. Initially, Cu2O cubic nanomaterials with a good photocurrent response were obtained by facile green room temperature synthesis and dropped on fluorine-doped tin oxide (FTO) plates as photoactive materials (Cu2O/FTO). In the presence of target cTnI, horseradish peroxidase (HRP) on the detection antibody catalyzes the substrate 4-chloro1-naphthol (4-CN) to produce insoluble precipitates of benzo-4-chlorohexadienone (4-CD) on Cu2O/FTO with the assistance of H2O2, resulting in a decrease in the photocurrent of the Cu2O/FTO electrode. To make the whole inspection process more concise and efficient, we used a flashlight and a digital multimeter as the excitation light source and reading device for the PEC sensing system, respectively. Under the optimal conditions of immunoreaction time, pH, and loading, the photocurrent of Cu2O/FTO decreased with increasing target cTnI concentration with a limit of detection (LOD) of 4.7 pg mL−1 in the operating range of 0.01–10 ng mL−1. It is of interest that the developed portable PEC immunoassay is also capable of detecting cTnI in human serum samples with acceptable accuracy compared to the reference cTnI enzyme-linked immunosorbent assay (ELISA) method while maintaining portability and sensitivity.
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高影响因子
BIOSENSORS & BIOELECTRONICS
·
2021
·
IF 10.618
Yingwen Wang,Dun Zhang,Yan Zeng,Peng Qi
Simultaneous multiple-target detection is essential for the prevention, identification, and treatment of numerous diseases. In this study, a novel strategy based on target-modulated competitive binding and exonuclease I (Exo I)-powered signal molecule release was established with the advantages of rapid response and high selectivity and sensitivity. The strategy holds substantial potential for the development of versatile platforms for the simultaneous detection of biological targets. To mitigate the low load capacity and time-consuming responsive process of the Zr-MOF system, UiO-67 was chosen to replace UiO-66 (a typical Zr-MOF) as the nanocarrier for encapsulating more signal molecules, whereby the assembled double-stranded DNA (dsDNA) structures of UiO-67 acted as gatekeepers to form dsDNA-functionalized MOFs. Additionally, Exo I was introduced into the system to accelerate the release of the signal molecules. In the presence of biological targets, the competitive binding between the targets and aptamers caused the hydrolysis of the free DNA sequence by Exo I, promoting the release of signal molecules and leading to a rapid and significant increase in the fluorescence intensity . For adenosine triphosphate (ATP) and cytochrome c (cyt c ), which were chosen as model biological targets, this sensor displayed detection limits as low as 5.03 and 6.11 fM, respectively. Moreover, the developed biosensor was successfully applied to the simultaneous detection of ATP and cyt c in spiked serum samples. Therefore, this strategy provides guidance for further research of biosensors for simultaneous multiple-target detection and propels the application of MOF carriers in biomedicine.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Zhiheng Gong,Wenye Zhong,Zuyun He,Qiuyu Liu,Haijun Chen,Deng Zhou,Nian Zhang,Xiongwu Kang,Yan Chen
Electrochemical nitrate reduction (NO 3 - RR) to synthesize ammonia is considered to be a promising strategy to enable artificial nitrogen cycle. Great efforts have been devoted to improving the efficiency and selectivity of the electrocatalysts for NO 3 - RR. Herein, we demonstrate that tuning the oxygen chemical environment via Ar plasma treatment is an effective approach to improve the NO 3 - RR activity of Cu 2 O. Combining synchrotron-based X-ray absorption spectroscopy and other advanced spectroscopy techniques, we find that plasma treatment can effectively promote the formation of oxygen vacancies and hydroxyl groups on Cu 2 O surface. In-situ diffuse-reflectance infrared Fourier transform spectroscopy and density functional theory calculation further reveal that oxygen vacancies and hydroxyl groups facilitate the adsorption of nitrate and proton transfer on the Cu 2 O surface, thus leading to improved ammonia selectivity. Our results clarify the critical role of surface oxygen species for NO 3 - RR and can guide the design of other electrocatalysts via surface engineering.
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JOURNAL OF MEDICINAL CHEMISTRY
·
2019
·
IF 6.054
Lan-Lan Lou,Fu-Qiang Ni,Lin Chen,Sharpkate Shaker,Wei Li,Rong Wang,Gui-Hua Tang,Sheng Yin
A germacrane sesquiterpenoid library containing 30 compounds (2–31) was constructed by structural modification of a major component aristolactone (1) from the traditional Chinese medicine Aristolochia yunnanensis. Compound 11 was identified as a promising anticardiac fibrosis agent by systematic screening of this library. 11 could inhibit the expression of fibronectin (FN), α-smooth muscle actin (α-SMA), and collagens in transforming growth factor β 1 (TGFβ1)-stimulated cardiac fibroblasts at a micromolar level and ameliorate myocardial fibrosis and heart function in abdominal aortic constriction (AAC) rats at 5 mg/kg dose. Mechanistic study revealed that 11 inhibited the TGFβ/small mother against decapentaplegic (Smad) signaling pathway by targeting TGFβ type I receptor (IC50 = 14.9 ± 1.6 nM). The structure–activity relationships (SARs) study indicated that the unsaturated γ-lactone ring and oxidation of C-1 were important to the activity. These findings may provide a new type of structural motif for future anticardiac fibrosis drug development.
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Nanoscale Advances
·
2023
·
IF 4.7
Yizhou Zhang,Yiru Wang,Zhengyi Zhang,Zhe Wang,Changyu Shao,Matthias Hannig,Zihuai Zhou,Baiping Fu
Calcium carbonate (CaCO3), possessing excellent biocompatibility, bioactivity, osteoconductivity and superior biodegradability, may serve as an alternative to hydroxyapatite (HAp), the natural inorganic component of bone and dentin. Intrafibrillar mineralization of collagen with CaCO3 was achieved through the polymer-induced liquid precursor (PILP) process for at least 2 days. This study aims to propose a novel pathway for rapid intrafibrillar mineralization with CaCO3 by sequential application of the carbonate-bicarbonate buffer and polyaspartic acid (pAsp)-Ca suspension. Fourier transform infrared (FTIR) spectroscopy, zeta potential measurements, atomic force microscopy/Kelvin probe force microscopy (AFM/KPFM), and three-dimensional stochastic optical reconstruction microscopy (3D STORM) demonstrated that the carbonate-bicarbonate buffer significantly decreased the surface potential of collagen and that CO32-/HCO3- ions could attach to collagen fibrils via hydrogen bond. The electropositive pAsp-Ca complexes and free Ca2+ ions are attracted to and interact with CO32-/HCO3- ions through electrostatic attractions to form amorphous calcium carbonate that crystallizes gradually. Moreover, like CaCO3, strontium carbonate (SrCO3) can deposit inside the collagen fibrils through this pathway. The CaCO3-mineralized collagen gels exhibited better biocompatibility and cell proliferation ability than SrCO3. This study provides a feasible strategy for rapid collagen mineralization with CaCO3 and SrCO3, as well as elucidating the tissue engineering of CaCO3-based biomineralized materials.
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Journal of Materials Chemistry B
·
2023
·Vol. 11
·期 44
·10632-10639
·
IF 7
Lijia Yao,Bingquan Chen,Hailong Wu,Yuanjing Cui,Guodong Qian
Combination therapies are an increasingly important part of the antitumor medicine armamentarium. However, developing desirable nanomaterials for combination therapies is still a great challenge. Herein, a biocompatible Cu(I)-doped metal–organic framework (MOF) (denoted as CuZn-ZIF) is designed as a novel dual-functional nanocarrier. Doxorubicin molecules are covalently bound to the surface of the CuZn-ZIF and released by the cleavage of chemical bonds in an acidic environment, demonstrating the capacity of controlled drug release. More importantly, CuZn-ZIF nanocarriers can simultaneously play the role of nanocatalysts, capable of catalyzing H2O2 into a highly reactive intracellular toxic hydroxyl radical (˙OH). An in vivo study reveals that nanoparticles exhibit high antitumor efficacy through the combined performance of DOX and Cu(I), proving the great potential of this copper(I)-based MOF for combined chemo-chemotherapy to improve therapeutic efficacy.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Jian Zhang,Ning Pu,Menglin Li,Wenhao Sang,Qing He,Qianqiu Tian,Wen Zhang
Interest in functional silver has rapidly grown over the years due to significant advances in separation, sensing, catalysis, and biomedical applications. Here we developed a new strategy to load single atomic silver species in the rigid and open unit of the fully conjugated benzimidazole-linked polymers (BILPs). Due to the well-defined chelating units of N-heterocycles, the Ag + ion species can be coordinated by N ligands and stabilized in the atomic level without aggregating into nanoscale Ag clusters and nanoparticles. The obtained Ag + -BILP-101 exhibits a selective binding property of Ag + ions from solutions. The ultrastable structure and the property of taking up metal species, endow BILPs with the advantages of functionalizing metal species. After the reduction by NaBH 4 , the Ag + ions were transferred into Ag nanoparticles. The substantial and intrinsic porosity of BILPs also gives excellent accessibility to Ag species loaded in the frameworks. The plentiful N-heterocycles and loaded Ag species show a synergistic/coadsorption effect for iodine vapor, and the charge transfer from frameworks promotes the formation of iodide ions. The iodine capture capacities of Ag + -BILP-101 and Ag 0 -BILP-101 reach 3.3 g/g and 3.7 g/g at 80 ℃, and still maintain 3.2 g/g and 3.5 g/g at 150 ℃, respectively. After ethanol elution, the residual iodine/Ag molar ratios in Ag + /Ag 0 -BILP-101 samples are still more than one (about 1.5), suggesting their strong affinity toward iodine. This work highlights the excellent selective Ag + ion binding and Ag species supporting properties of BILPs, which can extend to other porous organic framework platforms for various applications based on silver species-skeleton interactions.
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CHEMISTRY OF MATERIALS
·
2021
·
IF 9.811
Jinglong Huang,Binbin Su,Enhai Song,Maxim S. Molokeev,Zhiguo Xia
Low-dimensional hybrid metal halides demonstrate broad-band emission and high photoluminescence quantum yield (PLQY) acting as excellent candidates for a new generation of luminescent materials in lighting fields. However, most luminescent metal halides can only be excited by ultraviolet radiation, and the discovery of high-efficient emitters with broad-band excitation characteristics, especially upon efficient blue light irradiation, is a challenge. Herein, a zero-dimensional (0D) Cu(I)-based organometallic halide (18-crown-6)2Na2(H2O)3Cu4I6 (CNCI) was prepared with a green emission band centered at 536 nm and a near-unity PLQY (91.8%) upon excitation of 450 nm. Importantly, the ultrabroad excitation band covering a 300–500 nm range was observed in CNCI, and the luminescence mechanism has been discussed in detail. A white light-emitting diode (WLED) was fabricated with high luminous efficiency of 156 lm/W and a high color rendering index of 89.6. This work provides guidance for designing high-performance luminescent metal halides with suitable excitation characteristics and also promotes the application prospects of such materials in WLED fields.
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JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Jiafu Li,Jiahui He,Md. Tareq Aziz,Xiaocui Song,Ying Zhang,Zhiguang Niu
As a well known endocrine-disrupting and model chemical, bisphenol A (BPA) may pose a serious threat to human health, since it and its disinfection by-products (DBPs) have been detected in drinking water , urine, human colostrum, adipose tissue , and placenta samples. Although chlorinated BPAs (Cl-BPAs) and iodinated BPAs (I-BPAs) have been well studied, brominated BPAs (Br-BPAs), and mixed halogenated DBPs like bromo-iodo-BPAs (Br-I-BPAs), and bromo-chloro-iodo-BPAs (Cl-Br-I-BPAs) are less well understood. Notably, the role of iodide (I - ) during chlorination is not well understood, since the studies of the I-DBPs mainly focus on their genotoxicity and cytotoxicity. To understand the formation mechanisms of halogenated bisphenol A (HBPs) during chlorination with bromide (Br - ) and/or I - , and the role of I - during chlorination, three set of reactions were performed in the laboratory (“BPA + chlorine + Br - ”, “BPA + chlorine + I - ” and “BPA + chlorine + Br - +I - ” assigned as group A, B and C respectively). Thirty HBPs were identified and 18 of them were never reported before. I - increases the transformation rate of BPA into HBPs as I-BPAs act as intermediate HBPs during chlorination that easily react with HClO/ClO - and HBrO/BrO - to form Cl-BPAs and Br-BPAs. HIO/IO - showed higher reactivity towards BPA and HBPs than that of HBrO/BrO - and HClO/ClO - . The recycling of I - was observed in the reactions of “BPA + chlorine + I - ” and “BPA + chlorine + Br - +I - ”, which may explain why I - can induce BPA to transform into HBPs and suggests that I - may act as a catalyst during the BPA chlorination reactions. The reaction pathways are proposed which present the reactions of BPA and HBPs with HClO/ClO - , HBrO/BrO - , and HIO/IO - , as well as the recycling of I - . This study describes the potential DBP formation and transformation mechanisms of BPA and its 16 alternatives, as well as the role of I - on the transformation of phenol compounds during chlorination.
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ChemCatChem
·
2021
·Vol. 13
·期 20
·4325-4333
·
IF 5.686
Hongwei Deng,Chenyan Guo,Penghui Shi,Guohua Zhao
Graphical Electroreduction of CO 2 : The amino group is modified on the copper electrode with the cuprous oxide deposition layer by electrodeposition, and then the CO 2 is electrocatalytically reduced to ethylene on the surface, which promotes the efficient recycling of carbon resources in the ecosystem. Amino assisted protonation for carbon-carbon coupling during electroreduction of carbon dioxide to ethylene on copper(I) oxide reported by Penghui Shi, Guohua Zhao and co-workers from Shanghai University of Electric Power and Tongji University. The development of effective catalysts for the electrocatalytic carbon dioxide reduction reaction (CO 2 RR) to two-carbon (C 2 ) products is a practical approach to solve the energy crisis and stabilize the carbon cycle of the ecosystem. The production of electrocatalytic CO 2 RR with copper metal shows low selectivity and mainly generates one-carbon (C 1 ) products, hindering its wide practical application. The use of copper (I) oxide (Cu 2 O) in electrocatalysis has attracted intense research attention because it can more efficiently produce C 2 products with high energy density such as ethylene (C 2 H 4 ) and ethane (C 2 H 6 ). We use an amino-modified Cu 2 O catalyst (NH 2 −Cu 2 O) for electrocatalytic CO 2 RR to obtain significantly increased production of the CO and C 2 products. Electrochemical in-situ infrared spectroscopy analysis was used to detect the presence of the *COOH and *CHO reaction intermediates. Density functional theory calculations showed that the amino (−NH 2 ) modification reduces the free energy of the *CO→*CHO reaction that is the rate-determining step in C 2 H 4 production. Our results show that amino modification can promote the protonation of *CO and *CHO carbon-carbon coupling to produce C 2 H 4 . Thus, amino-modified copper-based catalysts are promising materials for application in electrocatalytic CO 2 RR to multi-carbon products.
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ANALYTICAL CHEMISTRY
·
2020
·
IF 6.785
Dexin Du,Jiangnan Shu,Mingquan Guo,Mohammad A. Haghighatbin,Di Yang,Zhiping Bian,Hua Cui
Recently, nanoluminophores with the potential-resolved multicolor electrochemiluminescence (PRMCECL) property have emerged and shown promising applications in sensitive, selective, and accurate bioassays, bioimaging, and multicolor emitting devices. However, only limited PRMCECL nanoluminophores and their applications in ratiometric biosensors eliminating proportional errors have been reported. Herein, a novel PRMCECL nanoluminophore was synthesized by encapsulating CdS quantum dots (CdSQDs) into MOF-5 (CdSQDs@MOF-5). Using K2S2O8 as a coreactant, two electrochemiluminescence (ECL) peaks, ECL-1 centered at 685 nm and ECL-2 centered at 475 nm, were observed at −1.4 and −1.8 V, respectively. Related ECL mechanisms have been proposed. Based on the potential-resolved ECL signals, a label-free differential ECL immunosensor for the determination of cardiac troponin I (cTnI) was established by assembly of poly(diallyldimethylammonium chloride), CdSQDs@MOF-5, and cTnI antibody-functionalized silver nanoparticles on the surface of the fluorine-doped tin oxide electrode subsequently. In the presence of cTnI, cTnI was captured by the sensing interface, leading to an increase in ECL-1 and ECL-2 intensity. cTnI could be determined in the range of 0.01–1000 pg/mL with a detection limit of 5.01 fg/mL using the intensity difference between ECL-1 and ECL-2. This work provides a new family member of PRMCECL nanoluminophores. The proposed label-free differential ECL immunosensor provides a new strategy based on potential-resolved ECL signals, which could effectively eliminate the additive error and show better sensitivity, selectivity, and accuracy for the detection of cTnI than the single-signal strategy and ratiometric strategy.
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RARE METALS
·
2020
·Vol. 40
·期 7
·1987-1994
·
IF 2.161
Wang Ya-Ting,Liu Men,Tang Nian,Li Sheng-Jian,Sun Yan,Wang Shi-Xiong,Yang Xiang-Jun
Abstract Solvent extraction based on ionic liquids is generally considered to be an environmentally benign and effective technology for gold(I) recovery. The aim of this work is to study gold(I) extraction from aurocyanide solution using fluorine-free ionic liquids [A336][SCN], [A336][MTBA] and [A336][Mal]. Various factors that affect gold(I) extraction (including concentration of ionic liquids, equilibrium pH, concentration of the modifier tributyl phosphate (TBP), reaction time and initial concentration of gold in an aqueous solution) were studied and optimized. The results indicate that the three Aliquat 336-based ionic liquids all exhibit excellent behaviors for gold(I) extraction. More than 99.8% of gold(I) can be extracted from the aqueous phase into the ionic liquid phase. The gold-loaded ionic liquids were characterized using infrared spectroscopy and mass spectrometry to study the extraction mechanism of gold(I). The results revealed that extraction of gold(I) into the ionic liquid phase was based on an exchange reaction between the anion Au(CN)
− 2
in aqueous solution and the anion SCN − in ionic liquid [A336][SCN]. The logarithmic relationship between distribution coefficient and TBP concentration indicates that two TBP molecules are involved in the formation of the extracted complex. The extracted complex was determined to be A336 + ·Au(CN)
− 2
·2TBP. In addition, the gold(I)-loaded ionic liquids can be efficiently stripped using NH 4 SCN, 2-methylthiobenzoic acid and methyl maltol. The results establish that Aliquat 336-based ionic liquids have potential application prospects in gold(I) recovery from cyanide solutions.
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