ANALYST
·
2023
·Vol. 148
·期 12
·2825-2833
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IF 4.2
Yanwen Chen,Liu Zhao,Baoshuai Zhang,Yuqing Guan,Cheng Yao,Xuan Xu
Due to the vital role of alkaline phosphatase (ALP) in clinical diagnoses and biomedical research, a sensitive and selective detection method for ALP activity is of considerable importance. Herein, a facile and sensitive colorimetric assay for the detection of ALP activity was developed based on Fe–N hollow mesoporous carbon spheres (Fe–N HMCS). Fe–N HMCS were synthesized by a practical one-pot method with aminophenol/formaldehyde (APF) resin as the carbon/nitrogen precursor, silica as the template and iron phthalocyanine (FePC) as the iron source. Thanks to the highly dispersed Fe–N active sites, Fe–N HMCS exhibited exceptional oxidase-like activity. In the presence of dissolved oxygen, Fe–N HMCS were able to effectively convert colorless 3,3′,5,5′-tetramethylbenzidine (TMB) into oxidized TMB (oxTMB) with blue color, while the reducing agent of ascorbic acid (AA) inhibited the color reaction. Based on this fact, an indirect and sensitive colorimetric sensing method was developed to detect alkaline phosphatase (ALP) with the assistance of the substrate L-ascorbate 2-phosphate (AAP). This ALP biosensor exhibited a linear range of 1–30 U L−1 and a limit of detection (LOD) of 0.42 U L−1 in standard solutions. In addition, this method was applied to detect ALP activity in human serum with satisfactory results. This work offers a positive reference for the reasonable excavation of transition metal–N carbon compounds in ALP-extended sensing applications.
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Journal of Cleaner Production
·
2023
·
IF 11.1
Chen Fang,Zixuan Hao,Yanlan Wang,Yingping Huang,Di Huang,Xiang Liu
Nanoreactors have been enlightened by enzymes to benefit from particular confinement for purpose of the acceleration of catalytic reactions and rendering them specific. Herein, we have first designed and synthesized the high-efficiency carbon nanotube-stabilized cobalt oxides nanoparticles (CoO x /CNT), via immobilization of CoO x nanoparticles onto carbon nanotube (CNT), for 3-aminophenol (3-AP) degradation via peroxymonosulfate (PMS) activation. Among them, carbon nanotube is used as a nanoreactor for efficient degradation of 3-AP over CoO x /CNT nanocomposite . The detailed physical characterizations illustrate that CoO x /CNT presented a nanotube-shaped structure, and some CoO x nanoparticles were encapsulated into CNT, and the molar ration of Co and O in CoO x was calculated to be 1:1.006, where CoO 1.006 might be the mixture of CoO and Co 3 O 4 . The comparison with other carriers (including MoS 2 , CeO 2 , ZnO and ZrO 2 ), CoO x /CNT provides the highest 3-AP degradation efficiency, highlighting the key role of CNT, as a nanoreactor, in CoO x /CNT for activating PMS to degrade 3-AP. The super-high catalytic activity of CoO x /CNT nanocomposite in the 3-AP degradation is owing to the specific confinement (encapsulation of some CoO x by carbon nanotubes). It seems the electron transfer from CNT to Co atom surface, enriched its surface electron cloud density, which is favorable for PMS activation. Quenching experiments and electron paramagnetic resonance (EPR) result have verified that SO 4 • - and OH• are the primary reactive oxygen species in 3-AP degradation over CoO x /CNT/PMS system. This study provides a new research orientation for the synthesis of efficient and stable carbon nanotube-encapsulated Co-based nanocatalyst for wastewater treatment .
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TALANTA
·
2022
·
IF 6.556
Mengzhen Ren,Yujie Zhang,Lanlan Yu,Lingbo Qu,Zhaohui Li,Lin Zhang
Nanozyme with the merit of excellent and adjustable catalytic activity, outstanding stability and low cost is a promising alternative for natural enzymes widely applied in a variety of fields. In the present study, a new two-dimensional cobalt-based MOF nanocomposite designated as MVCM@β-CD was synthesized. Combined with the strategies of increasing the ratio of Co(Ⅲ)/Co(Ⅱ) and modifying with small molecule β-cyclodextrin (β-CD), MVCM@β-CD displayed remarkably enhanced oxidase-mimicking activity, which was attributed to synergistic effect from large surface area of two dimensional Co-MOF nanosheet , numerous exposed active sites, high-proportioned trivalence of cobalt and regulating action of β-cyclodextrin. The addition of aminophenol isomers inhibited the catalytic oxidation process, resulting in different color change of the solution and UV–Vis absorption behaviors, based on which a sensitive ratiometric colorimetry for m -aminophenol ( m -Ap) and a simple colorimetric p -aminophenol ( p -Ap) detection method were developed with the detection limit of 0.16 μM and 1.01 μM, respectively. This method realized the colorimetric differentiation of aminophenol isomers, which provided a simple, accurate and low-cost approach for visual discrimination without complicated instrument and procedure, especially appropriate for on-site detection.
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ACS Biomaterials Science & Engineering
·
2022
·
IF 5.395
Yi Zhang,Siyuan Hao,Jingjie Zuo,Huiling Guo,Mingxing Liu,Hongda Zhu,Hongmei Sun
Combinatorial photothermal therapy and chemotherapy is an extremely promising tumor therapeutic modality. However, such systems still remain challenges in stimulus sensitivity, avoiding drug leakage, and therapeutic safety. To solve these problems, we engineered actively loaded doxorubicin (DOX) and gold nanorod (GNR) liposomes through embedding stiff hollow mesoporous silica nanoparticles (HMSNs) in the liposomal water cavity (HMLGDB) to resist the influence of shear force of GNRs to prevent drug leakage. Under 808 nm laser irradiation, the ambient temperature was raised greatly because of the photothermal conversion of GNRs, thereby rupturing the lipid layer and then triggering the DOX release. The results of in vitro experiments showed that the low concentration of HMLGDB (15 μg/mL) could effectively overcome the MCF-7 cells (human breast cancer cell line) by the increase of DOX concentration intracellularly and the good photothermal effect of GNRs. After intravenous injection, HMLGDB exhibited intratumor aggregation and PTT capacity. Furthermore, the combined chemo–photothermal antitumor strategy demonstrated a high inhibition of tumor growth and low damage to normal tissues. The developed hybrids provide a paradigm for efficient combinatorial photothermal therapy (PTT) and chemotherapy (CT).
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JOURNAL OF MOLECULAR LIQUIDS
·
2022
·
IF 6.633
Yuanyuan Cao,Shuyi Shan,Yitong Lu,Jialu Luo,Yilin Li,Rongzhang Hao
Low toxicity is one of the key properties for the sustainable application of polyethylene glycol-based deep eutectic solvents (PEG-based DESs) in separation, catalysis, biochemistry and analysis. However, the toxicity of PEG-based DESs is not reported and the rules for obtaining lower toxicity is needed to explore. Herein, the cytotoxicity of several PEG-based DESs against lung cancer cell (A549) was evaluated by CCK-8 assay, and strategies for the minimizing and tuning the toxicity of DESs are for the first time proposed from the aspects of mole ratio, hydrogen-bonding donor, hydrogen-bonding acceptor, components numbers, and solvent concentration. The results indicated that the DESs are more toxic than their individual components, and the toxicity order of DESs is generally in accordance with the individual components except for the hydrogen-bonding donor. This work would provide possible routes for the decrease of DESs toxicity for sustainable and green chemistry.
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ACS Applied Nano Materials
·
2023
·
IF 5.9
Hu Zhang,Jingkun Hu,Yongchuan Liu,Changxin Lin,Xiangxin Zhang,Yining Zhang
Capacitive deionization (CDI) based on the theory of a double electric layer has received much attention in the past two decades as a highly promising desalination technology, and carbon nanospheres are considered promising carbon-based electrode materials for CDI, which have been investigated by a large number of researchers. However, the isolation between the spheres greatly increases the contact resistance, limiting their application in CDI. To understand the effect of structure on the performance of CDI and to obtain a better CDI performance, solid carbon spheres and monodisperse hollow carbon spheres were prepared and compared with interconnected hollow carbon spheres (IHCSs). The resulting IHCSs, with their unique cavity structure and interconnected carbon walls, exhibited superior electrochemical performance and electrosorption capacity. In addition, we improved the electrical conductivity, surface wettability, and adsorption properties of the carbon nanospheres by incorporating nitrogen doping. By adjusting the amount of nitrogen functional groups in the carbon nanosphere precursors, we produced interconnected hollow carbon nanospheres with similar structures (particle size, specific surface area, and porosity) but different nitrogen contents and investigated the effects of different nitrogen contents on the CDI properties of hollow carbon nanospheres. The results indicated that interconnected hollow carbon nanospheres with a high nitrogen content (designated as NFs-2) demonstrated the best CDI performance, achieving an electrochemical adsorption capacity of 20.43 mg g–1 in a NaCl solution with a concentration of 500 mg L–1. Additionally, NFs-2 exhibited the largest specific surface area of 728 m2 g–1. Furthermore, NFs-2 displayed excellent cycle stability in a desalination cycle using a 100 mg L–1 NaCl solution, retaining up to 97.17% of its initial desalination capacity after 25 sorption–desorption cycles. These findings highlight the promising applications of NFs-2 in CDI technology.
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Surfaces and Interfaces
·
2023
·
IF 6.2
Chen Fang,Yanlan Wang,Wenkai Huang,Yingping Huang,Di Huang,Xiang Liu
Sulfite has recently been considered as the most potential alternative to peroxydisulfate and peroxymonosulfate for wastewater treatment because of its low ecotoxicity, low cost and abundant source. Although all sorts of homogeneous catalysts, such as Co 2+ , Cu 2+ , Fe 2+ , Mn 2+ , and so on, are developed for activating sulfites to generate SO 4 • − , it is of high significance to develop heterogeneous catalysts for wastewater treatment via sulfite activation. Herein, we have employed carbon nanosphere as an efficient support for CoO x nanoparticles on water decontamination via sulfite activation. The comparison with other carbon carriers (including carbon nanotubes and activated carbon) emphasized the vital role of CNS-600 in CoO x /CNS-600 for tetracycline (TC) degradation via Na 2 SO 3 activization. Because CNS-600 presented an uniform structure of nanosphere, with surface nitrogen and oxygen functional groups, which were favorable for Na 2 SO 3 activation and CoO x stabilization. This work proposes an efficient and heterogeneous Co-based nanomaterial for water decontamination via Na 2 SO 3 activization.
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Materials Today Energy
·
2023
·
IF 9.3
Li Qiao,Xingkun Wang,Ren Xu,Canhui Zhang,Kaiyue Chen,Kecheng Tong,Huanlei Wang,Shuixing Dai,Lei Chu,Minghua Huang
It is of paramount importance to develop highly efficient and Cl − corrosion-resistant bi-functional catalysts for the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) for application in seawater-based Zn-air batteries (S-ZABs), but the process remains full of challenges. Herein, a facile and effective strategy was adopted to fabricate the N-doped carbon shell armored ‘Janus’ Co/Co 9 S 8 heterojunction catalyst (denoted as Co/Co 9 S 8 -NMC). The well-defined ‘Janus’ structure endows the catalyst with a ‘synergistic effect’ between Co and Co 9 S 8 species, which can also accelerate the electron transfer via ‘Janus’ interfaces, thus boosting ORR/OER performance. Besides, N-doped carbon shells can be considered armor for protecting the catalyst from Cl − corrosion. By virtue of these merits, the resulting Co/Co 9 S 8 -NMC catalyst exhibits excellent catalytic activity for ORR and OER in seawater electrolyte, accompanied by a half-wave potential of 0.83 V and a low overpotential of 298 mV to achieve a current density of 10 mA/cm 2 . Besides, the S-ZABs based on the Co/Co 9 S 8 -NMC catalyst deliver a high maximum power density of 162.29 mW/cm 2 and robust stability over 600 h. This work advances the development of highly efficient bi-functional catalysts for S-ZABs.
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JOURNAL OF MOLECULAR STRUCTURE
·
2023
·
IF 3.8
Kang Luo,Wanlin Sun,Yuting Chi,Shuiqin Chai,Chengyu Sun,Wen Wu
Effectively killing microbial pathogens without inducing resistance is a challenge, especially in the treatment of infectious diseases. In this study, sulfur ( S )- and phosphorus (P)-doped carbon quantum dots (CQDs) were synthesized by one-step hydrothermal method using m -aminophenol as carbon source, thiourea and phosphoric acid as S and P dopants, respectively. Compared with S-CQDs, P doping could lead to a red-shift of the maximum emission wavelength. In addition, the as-prepared S-CQDs and S, P-CQDs exhibited unique antibacterial efficacy against both E. coli and S. aureus without developing drug resistance. In contrast, the S, P-CQDs had no preference for Gram-positive and Gram-negative bacteria, and they had a somewhat reduced bactericidal efficacy than that of S-CQDs, but S, P-CQDs had better bacteriostatic stability than S-CQDs. Such an excellent antibacterial effect might be attributed to the generation of a large number of intracellular reactive oxygen species (ROS), which disrupted the structure and the regular surface of bacterial cell. Consequently, the prepared S-CQDs and S, P-CQDs could be applied as antibacterial drugs with broad-spectrum antibacterial activity and without drug resistance.
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JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Jing Zhu,Hongwei Jiang,Wenwu Wang
The high toxicity and low biodegradability of the phenolic pollutants destroyed the balance of the environment and influenced human health seriously. Here, we developed a three-dimensional coloremetric sensor array for discriminating and determinating phenolic pollutants basing on the distinct Cu/nucleotides MOFs . Firstly, three laccase-mimic Cu/MOFs (Cu/AMP, Cu/CMP, and Cu/GMP) were obtained by regulating the molar ratio of Cu 2+ and nucleotides. Then the Cu/MOFs as the recognition elements of the sensor array catalyzed the pollutants-4-AAP-H 2 O 2 system, obtaining the colored benzoquinone products. Subsequently, the data array obtaining from the combined training matrix (3 Cu/MOFs × 6 pollutants × 5 replicates) was projected into a new dimensional space to obtain the 3D canonical scores, and classified into individual clusters by introducing LDA method. No overlap in their respective LDA plots for the six phenolic pollutants with different concentrations suggested the prominent discriminating performance of the sensor array. Furthermore, the sensor array exhibited high selectivity compared to the “lock-and-key” sensors even other active matrices coexisting in water samples. Importantly, the most influential discrimination factor was used to monitor the levels of the six targets, evidencing the potential application in assessing water pollution and maintaining human health.
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NEW JOURNAL OF CHEMISTRY
·
2023
·
IF 3.3
Yujie Zhang,Yingjiang Wang,Zhaohui Li,Lingbo Qu,Lanlan Yu
Nanozymes, which possess similar catalytic activities to natural enzymes, are considered promising alternatives to natural enzymes. In the present study, a new bimetallic Fe/Mn metal–organic framework (MOF) nanomaterial was synthesized by doping Mn in MIL-101(Fe). Despite the low doping amount of Mn, the Fe/Mn MOF displayed remarkably enhanced peroxidase-like activity, catalyzing the conversion of chromogenic substrate ABTS to blue-green ABTS˙+. Subsequently, the addition of environmental pollutant aminophenol isomers induced different color changes in a solution, which provided a simple and feasible approach to differentiate them by the naked eyes. Based on the effect of aminophenol isomers on the absorption spectrum of ABTS˙+, colorimetric methods were developed to quantitatively determine m-AP and p-AP with detection limits of 0.13 μM and 0.20 μM, respectively. Furthermore, taking advantage of a smart phone software-color recognizer to analyze the RGB value, a rapid detection method for m-AP was proposed, offering a solution to detect m-AP in the absence of any analytical instruments. This work verified the essential role of doping Mn in enhancing the enzyme-like activity of nanozymes. Simultaneously, the proposed simple, rapid, and accurate sensing method provided a new option to differentiate and determine aminophenol isomers, which has great potential for environmental application.
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FOOD CHEMISTRY
·
2022
·
IF 9.231
Jing Ren,Yanke Lu,Yehong Han,Fengxia Qiao,Hongyuan Yan
Perfluorooctanoic acid (PFOA) and perfluorooctane sulfonate (PFOS) are emerging pollutants that threaten food safety. Herein, a rapid, accurate, and selective method for determination of PFOA and PFOS in milk was established by using new molecularly imprinted phenolic resin (MIP-PR) as the adsorbent of dispersive filter extraction (DFE) combined with liquid chromatography-tandem mass spectrometry (LC-MS/MS). MIP-PR was synthesized at room-temperature using m-aminophenol, glutaraldehyde, and perfluorononanoic acid as the monomers, cross-linkers, and virtual templates, respectively, and exhibited rapid mass transfer (30 s), high selectivity (imprinted factors > 3.7), and large adsorption capacity (>54.6 mg/g). Compared with reported methods, the developed MIP-PR–DFE method is fast, selective, inexpensive, and shows good purification and enrichment efficiency. The proposed MIP-PR–DFE–LC-MS/MS exhibited low limits of detection (0.006–0.022 ng/mL), high recoveries (94.7–109 %), and good precision (RSDs ≤ 9.5 %). This study provides a new idea for the development of imprinted resin adsorbents for perfluorinated compound, and a new method for sample pretreatment for monitoring of PFOA and PFOS in food.
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