JOURNAL OF MEMBRANE SCIENCE
·
2023
·
IF 9.5
Junqiao Jiang,Min Xiao,Sheng Huang,Dongmei Han,Shuanjin Wang,Yuezhong Meng
Phosphoric acid (PA)-dependent proton conductivity and polymer-offered mechanical properties are contradictory in high-temperature proton exchange membranes (HT-PEMs). Microphase separation strategy contributes to achieve a tradeoff between proton conductivity and mechanical properties. Herein, a kind of phosphonic acid-imidazolium containing polymer (PICP) ionomeric membranes, in which acidophilic (imidazolium) and acidophobic groups (-PO 3 H 2 ) can be induced to form a microphase separation structure by PA, are firstly prepared. The acidophilic phase with adsorbed PA plays the role of proton conduction and the acidophobic phase can not only provides -PO 3 H 2 group synergistically conduct protons but also largely maintains the intrinsic mechanical properties. As a result, the PICP ionomeric membranes with microphase separation structure possess high proton conductivity (48 mS cm −1 , 160 °C) and satisfying mechanical strength (16.5 MPa) simultaneously at a moderate PA doping level (130 wt%). The fuel cell based on such HT-PEMs demonstrates a peak power density of 493 mW cm −2 and high voltage stability. This is the first report of phosphonic acid-imidazolium containing ionomeric membranes with satisfactory fuel cell performance and durability, representing a meaningful step towards practical HT-PEM fuel cells.
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HYDROMETALLURGY
·
2023
·
IF 4.7
Shaoping Feng,Kun Huang
Dialkylsulfide is considered as the most promising extractant for separating Pd(II) and Pt(IV) in industrial processes. However, the slow kinetics for Pd(II) extraction limits its extensive application. The development of new extractants with faster kinetics, high extraction efficiency, and exceptional Pd(II) separation selectivity has been a persisting goal over the past few decades. In this study, a new functionalized extractant, 1-methyl-2-(nonylthio)-1H-imidazole (MNI) containing both N and S atoms, was synthesized and employed to separate Pd(II) from mixed hydrochloric acid solutions with different initial Pd(II)/Pt(IV) concentration ratios. Experimental results revealed that MNI not only has a high selectivity for Pd(II) over Pt(IV) but also has faster kinetics for Pd(II) extraction than diisopentylsulfide (S201) under similar extraction conditions. In contrast to traditional dialkylsulfide extractants, MNI coordinates with Pd(II) ions via the N(5) atom in its imidazole ring to form Pd(MNI) 2 Cl 2 complexes, instead of using the S atom as with dialkylsulfide. The extraction mechanism involving the coordination between Pd(II) and MNI was demonstrated using the slope analysis method and ultraviolet (UV), Fourier-transform infrared (FT-IR), 1 H NMR, and 13 C NMR spectroscopic methods. The fast extraction kinetics between MNI and Pd(II) was possibly attributed to the high charge density of the N(5) atom in the imidazole ring, whereas the outstanding separation selectivity for Pd(II) was due to the strong affinity of the N(5) atom. The facile synthesis, high saturation capacity, excellent Pd(II) selectivity, and remarkable reusability endow MNI with potential applications in Pd(II) recovery from leach solutions of waste automotive catalysts and other secondary resources.
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JOURNAL OF AOAC INTERNATIONAL
·
2022
·Vol. 105
·期 6
·1596-1604
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IF 2.028
Long Fei,Zhu Qi,Li Yingping
BackgroundThe ratio fluorescent probe (RF-probe) has the characteristics of self-calibration and eliminating the influence of experimental factors (such as probe concentration, excitation intensity stability, and solution environment) in quantitative assays based on the linear relationship between the intensity ratio of two emission peaks and the concentration of analyte, especially in a complex biological matrix.ObjectiveHigh-luminescent Ag nanoclusters (AgNCs) were prepared at room temperature due to aggregation-induced emission (AIE) through the incorporation of trithiocyanuric acid (TA). Subsequently, a new RF-probe based on mixing of AgNCs-TA with nitrogen and sulfur co-doped carbon quantum dots (N, S-CQDs) was prepared for sensitively and selectively assaying sodium 2, 3-dimercaptopropane-1-sulfonate (DMPS).MethodsThe fluorescence of N, S-CQDs was quenched in the presence of the AgNCs-TA mainly deriving from the inner filter effect (IFE), and its fluorescence intensities at 440 and 650 nm could recover and drop upon the addition of DMPS (λex = 370 nm).ResultsThe RF-probe enables DMPS to be detected by fluorometry with a linear response in the 0.67–30.0 μmol/L concentration range and a 54.7 nmol/L detection limit (at 3σ/slope). At the same time, we also used the labeled recovery method to confirm the reliability of the method. The recoveries were 97.93–106.33%, and the corresponding standard deviations (RSD) were less than 1.87%.ConclusionThe N, S-CQDs/AgNCs-TA RF-probe can also semi-quantitatively monitor DMPS by naked eyes.HighlightsThe mechanism of fluorescence enhancement of the AgNCs by TA also were investigated by the N, S-CQDs/AgNCs-TA-DMPS system. What’s more, the RF-probe of N, S-CQDs/AgNCs-TA was successfully utilized to monitor DMPS in real samples.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
IF 6.371
Yuting Long,Hong Li,Wenbo Wang,Xinxin Yang,Zirui Liu
Ultrasensitive detection of highly toxic Cr(VI) is of paramount importance as trace amount of Cr(VI) will result in inevitable deterioration to human health and the environment. In this work, a novel methimazole-functionalized SERS optical fiber probe was used for the first time for Cr(VI) determination with ultrahigh sensitivity. A special functionalization process of methimazole was designed after successful fabrication of silver coated fiber probe via a SnCl 2 -sensitized solvothermal method. Dual functional methimazole guaranteed ultrahigh sensitivity and good stability of the SERS fiber probe for Cr(VI) detection. On one hand, methimazole functions as a Raman reporter which exhibits SERS peak intensity decline in the presence of Cr(VI). On the other hand, methimazole acts as an oxidation inhibitor via coordinating with silver atoms through the lone pair of nitrogen and sulfur atoms. The optimized SERS fiber probe not only presents good stability and excellent reproducibility, but also exhibits ultrahigh sensitivity (10 −11 M) which exceeds SERS or other techniques for Cr(VI) determination reported so far.
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ACS Applied Nano Materials
·
2022
·
IF 6.14
Cheng Zhang,Congying Shao,Junsheng Wang,Ziwei Li,Mengna Liang,Yongxiang Wang,Dan Liu,Shun Lu
Copper nanoclusters (CuNCs) with bright blue-emitting fluorescence have been synthesized via a simple one-pot process using 2-mercapto-1-methylimidazole (MMI) as a stabilizer. The as-prepared MMI-CuNCs exhibited a high quantum yield of 19.2%, a long luminescence lifetime of 10.57 μs, and excellent photostability. Significantly, the fluorescence intensities of MMI-CuNCs were effectively quenched with addition of Ag+ ions, and the MMI-stabilized CuNCs were developed as a sensitive fluorescent nanoprobe for the label-free determination of silver ions for the first time. The fluorescence sensor provided a fast linear response toward Ag+ in the range of 0.025–50 μM, with a detection limit of 6.7 nM. The fluorescence quenching mechanism was ascribed to an agglomeration-induced effect and static quenching. A fluorescence sensing platform was successfully applied for Ag+ detection in human serum samples with good accuracy and high reproducibility, signifying the practical applicability of the assay. Additionally, MMI-CuNCs displayed good solid-state blue emission and are suitable for security ink applications. The MMI-CuNCs were utilized as a color conversion layer to construct blue- and white-light-emitting diodes (LEDs) with excellent white light properties by a facile combination of MMI-CuNCs and UV LED chips. This result facilitates multiple functions of MMI-CuNCs in the application of label-free sensors, anticounterfeiting, and optical devices.
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Nanomaterials
·
2022
·Vol. 12
·期 2
·204
·
IF 5.719
Zhaoyu Liu,Dong Yao,Huiwen Liu,Hao Zhang
Packing luminescent metal nanoclusters (MNCs) into polymers and fabricating novel MNCs/polymer composite materials is effective in obtaining high-performance light-emitting diodes (LEDs). Herein, water soluble Cu and Au nanoclusters are encapsulated in polyvinyl alcohol (PVA) by a casting method. The obtained MNCs/PVA composite films are highly emissive with triple primary colors, and inherit the merits of PVA, such as transparency, flexibility, machinability, stability and self-healing ability. By employing the MNCs/PVA composite films as down-conversions, remote type monochromic and white LEDs are fabricated. The white LEDs (WLEDs) exhibit a maximum color rendering index (CRI) of 86 with a Commission Internationale de l’Eclairage (CIE) color coordinate of (0.33,0.35). By varying the three MNCs/PVA film arrangement, the correlated color temperature (CCT) of the WLEDs is tuned from 5582 to 9490 K, which signifies the possibility of MNCs/PVA as alternative light-emitting materials for advanced illumination and display in the future.Keywords:metal nanoclusters;fluorescence;polyvinyl alcohol;composite film;light-emitting diodes
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ADVANCED MATERIALS
·
2023
·
IF 29.4
Jun Li,Zhenhai Xia,Xiaowei Wang,Cheng Feng,Qingcheng Zhang,Xi'an Chen,Yun Yang,Shun Wang,Huile Jin
The acidic aqueous supercapacitors have been found to deliver appealing capacitive properties due to fast ion diffusion caused by the applied smallest size of hydrion. However, their practical applications are largely inhibited by the narrow electrochemical stability window of water (1.23 V). Herein, A nitrogen-enriched porous carbon materials (RNOPCs) is reported, consisting of varied nitrogen doping bonded on sp 2 and sp 3 carbon sites, which are capable of stimulating a wider potential window up to 1.4 V and thus resulting in a great enhancement of capacitive performance in aqueous acidic electrolytes. Together with the improved electrical conductivity and preferable hydrion diffusion, RNOPCs exhibit an ultrahigh volumetric capacitance (1084 F cm −3 ) in 0.5 M H 2 SO 4 . Besides, a fully packed RNOPCs-based symmetrical supercapacitor can deliver a high gravimetric and volumetric energy density of 31.8 Wh Kg −1 and 54.3 Wh L −1 respectively, approaching those of lead acid batteries (25–35 Wh Kg −1 ). The first-principles calculations reveal that the lone pair electrons of the doped nitrogen can be delocalized on its neighboring carbon atoms, improving charge uptakes and overpotentials. Such facile and scale-up production of carbon-based supercapacitors can bridge the gap of energy density between traditional supercapacitors and batteries in aqueous electrolytes.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2026
·
IF 4.8
Yi Wei Zhou,Yue Yu,Xin Lei Xu,Ying Gu,Zhen Chen,Lei Han
A HE-PBA with robust POD-like was prepared a facile co-precipitation strategy. • A smartphone-assisted colorimetric sensor was design for portable assay of MMI. • This sensor displayed high specificity and sensitivity for MMI detection. • This sensor has been triumphantly used to detect MMI in cosmetic samples. It is critical to exploit a sensitive, selective, and portable strategy for the credible detection of methimazole (MMI) for human health. Herein, high-entropy Prussian blue analogues (HE-PBAs) nanozyme were successfully fabricated by a facile co-precipitation strategy. The as-synthesized HE-PBAs possess robust peroxidase (POD)-like activity, which can trigger the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) to oxidized TMB (oxTMB) with the assistance of H 2 O 2 , generating a conspicuous chromogenic transition from colorless to blue. However, MMI can reduce oxTMB and consume the ROS, including •OH and O 2 •− , thereby suppressing the intrinsic POD-mimicking catalytic performance of HE-PBAs. Such an inhibitory effect reduces the absorbance of the sensing system and enables the gradual fading of the blue chromogenic signal. Based on this competitive inhibition mechanism, a novel colorimetric sensing platform was constructed for quantitative MMI determination. The developed sensor achieves high sensitivity toward MMI with a detection limit of 0.032 μM. Considering its simple operation and superior sensing performance, a portable and user-friendly sensor was also designed for visual sensing of MMI by combining a common smartphone. Moreover, this colorimetric sensor has been successfully applied for MMI detection in commercial cosmetic samples, demonstrating its potential practicality. This work not only provides a cheap, user-friendly, and portable sensing platform for visual detection of MMI in resource-limited settings, but also offers a rational design strategy for HEzymes. Download: Download high-res image (152KB) Download: Download full-size image
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Chemistry-Switzerland
·
2023
·Vol. 5
·期 3
·1990-1997
·
IF 2.1
Rui Wang,Yunyun Zheng,Yunsheng Xia
In this study, we present solid state processes for the fabrication of copper nanoclusters (NCs) and hierarchical supraparticles (SPs). To achieve this, copper salt and thiols are mixed and are then grinded for 10–15 min, and the nano-products are thereby obtained. Interestingly, it was found in this study that the formation of the NCs or SPs is completely dependent on the grinding methods that are used: with mechanical grinding, the products are several nanometer-sized NCs, whereas manual grinding in an agate mortar can obtain Cu SPs with diameters as low as 10 nm all the way up to 200 nm. The photoluminescence emission wavelength of the nano-products is located at ~680 nm. The Stokes shift of the obtained nanomaterials is more than 300 nm. The emission quantum yields of the Cu NCs and SPs are as high as 47.5% and 63%, respectively. Due to their facile fabrication processes and their favorable optical properties, the two as-prepared types of copper nano-materials exhibit great potential for bio-imaging and bio-sensing applications.Keywords:Cu nanoclusters;supraparticles;solid fabrication
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JOURNAL OF HAZARDOUS MATERIALS
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2020
·
IF 9.038
Xiang-Ping Zhang,Kai-Yuan Huang,Shao-Bin He,Hua-Ping Peng,Xing-Hua Xia,Wei Chen,Hao-Hua Deng
There is a continuing high demand to design effective sensors for the determination of heavy metal ions (HMIs) since they are hazardous to both human health and the environment. In this study, we reported a facile fluorescent sensor array for rapid discrimination of HMIs based on a single gold nanocluster (AuNC) probe. This AuNC probe was prepared by using 2-mercapto-1-methylimidazole (MMI) as a ligand and polyvinypyrrolidone (PVP) as a dispersing agent. The fluorescence emission of PVP/MMI-AuNC was observed to be closely related to the pH value of the aqueous solution, which displays yellow (λ max = 512 nm) and red (λ max = 700 nm) fluorescence at pH 12.0 and 6.0, respectively. Further experiments indicated that different HMIs can produce differential effects on the photoluminescence of PVP/MMI-AuNC and thus generate distinct fluorescent responses at 512 and 700 nm. On the basis of this phenomenon, a fluorescent sensor array based on the PVP/MMI-AuNC was then built by simply changing pH value in the sensor element. A total of seven HMIs had their unique response patterns and were successfully distinguished by hierarchical cluster analysis and linear discriminant analysis both in buffer solution and spiked water samples, achieving 100% identification accuracy. This study provides a simple and powerful fingerprinting sensing platform for multiple HMIs, showing broad application prospects in the field of environmental monitoring.
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Nanoscale
·
2020
·Vol. 12
·期 29
·15791-15799
·
IF 6.895
Hao-Hua Deng,Qiong-Qiong Zhuang,Kai-Yuan Huang,Paramasivam Balasubramanian,Zhen Lin,Hua-Ping Peng,Xing-Hua Xia,Wei Chen
As a new emerging candidate for solid-state phosphors, copper nanoclusters (CuNCs) have gained tremendous interest in the field of white light-emitting devices (WLEDs). However, their further applications are impeded by the low photoluminescence quantum yield (PLQY) and poor emission color tunability of CuNCs. This work demonstrates the synthesis of cyan and orange emitting CuNCs, and their combination as color conversion phosphors in WLEDs. The cyan and orange emitting CuNCs were prepared employing 2-mercapto-1-methylimidazole (MMI) and N-acetyl-L-cysteine (NAC), respectively, as stabilizing-cum-reducing agents. The dispersions of MMI-CuNCs and NAC-CuNCs are weakly emissive. However, after processing into powders, they both possess ultrahigh PLQYs (45.2% for MMI-CuNCs, and 64.6% for NAC-CuNCs) owing to the effect of aggregation-induced emission (AIE). All-CuNC based WLEDs are then designed and developed using powdered MMI-CuNC and NAC-CuNC samples on commercially available 365 nm GaN LED chips. They display acceptable white light characteristics with a Commission Internationale de l'Eclairage coordinate value and color rendering index of (0.26, 0.30) and 83, respectively. We believe that these cost-effective and eco-friendly CuNCs with interesting AIE properties will vigorously promote the development of high-quality WLEDs for commercial applications.
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ACTA PHARMACOLOGICA SINICA
·
2021
·Vol. 43
·期 4
·1059-1071
·
IF 6.15
Pan Hong,Shi Fu-guo,Fang Chao,Shi Jing-shan
Dendrobine is the main sesquiterpene alkaloid of Dendrobium nobile Lindl, which exhibits potent neuroprotective activity. However, its metabolism and disposition are little known. In this study, we investigated the metabolic characteristics of dendrobine in vitro and in rats. The metabolic stability and temporal profile of metabolites formation of dendrobine were assayed in human/rat liver microsomal and S9 fractions. Dendrobine metabolites were separated and identified mainly by UPLC-Q/Orbitrap MS. After oral administration of dendrobine (50 mg/kg) to rats, the accumulative excretion rate of dendrobine in feces, urine, and bile was 0.27%, 0.52%, and 0.031%, respectively, and low systematic exposure of dendrobine (AUC 0–∞ = 629.2 ± 56.4 ng·h/mL) was observed. We demonstrated that the elimination of dendrobine was very rapid in liver microsomal incubation (the in vitro elimination t 1/2 in rat and human liver microsomes was 1.35 and 5.61 min, respectively). Dendrobine underwent rapid and extensive metabolism; cytochrome P450, especially CYP3A4, CYP2B6, and CYP2C19, were mainly responsible for its metabolism. Aldehyde dehydrogenase, alcohol dehydrogenase and aldehyde oxidase were involved in the formation of carboxylic acid metabolites. By the aid of in-source fragmentation screening, hydrogen/deuterium exchange experiment, post-acquisition processing software, and available reference standards, 50 metabolites were identified and characterized in liver microsomal incubation and in rats. The major metabolic pathways of dendrobine were N -demethylation, N -oxidation, and dehydrogenation, followed by hydroxylation and glucuronidation. Collectively, the metabolic fate of dendrobine elucidated in this study not only yields benefits for its subsequent metabolism study but also facilitates to better understanding the mode of action of dendrobine and evaluating the pharmacologic efficiency of the high exposure metabolites.
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