JOURNAL OF RAMAN SPECTROSCOPY
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2022
·Vol. 53
·期 8
·1386-1393
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IF 2.727
Tong-Jiang Li,Bao-Ying Wen,Yue-Jiao Zhang,Lin Zhang,Jian-Feng Li
Organophosphorus (OPs) compounds have received enormous attention due to high neurotoxicity. However, the complex detection environment makes it very difficult to detect the OPs compounds at extremely low-concentration. Therefore, it is vital to develop a high sensitive analytical method for the detection of low-concentration OPs compounds at complex environment. Here, we proposed a novel surface-enhanced Raman scattering (SERS) substrate based on the core-shell structure Au@ZrO 2 for the detection of extremely low-concentration OPs compounds. By using above SERS substrate, we tested different kinds of OPs compounds and obtained excellent detection results. The detection limit of methyl parathion and triazophos can reach 0.01 mg/kg. Meanwhile, under the actual system (orange peel), the detection limit of the methyl parathion and triazophos also can reach 0.5 and 0.1 mg/kg, respectively. In addition, the above substrate is also very effective for the detection of dimethyl methylphosphonate (DMMP), a simulant for the chemical warfare agent (sarin), and the detection limit can reach 100 mg/kg. Besides, we also verified the reproducibility and stability of Au@ZrO 2 , which showed excellent properties. The relative standard deviation (RSD) of the SERS signal intensity for 20 tests was 6.38% and the enhancement ability of Au@ZrO 2 can remain stable within 30 days. These results show that the proposed Au@ZrO 2 SERS substrate has great potential in the detection of OPs compounds at extremely low-concentration in the complex detection environment.
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MATERIALS CHEMISTRY AND PHYSICS
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2022
·
IF 4.778
Zhenhu Guo,Jingsong Lu,Wensheng Xie,Xuezhong Li,Hong Wu,Lingyun Zhao
The strategic design for fabricating metal phenolic networks (MPNs) at different dimension brings potential possibilities to obtain MPNs-based system with controlled structure, biologically tunable physicochemical properties and high responsiveness behavior. Considering adequate Fe ions within Fe-based materials, self-supplied metal ions for polyphenol to form coating layer on the surface are served as a novel and facile strategies to obtain metal-based phenolic networks composites. Combing these, herein, a simple, green and fast strategy was performed to fabricate recyclable Fe@Fe 3+ -tannic acid-Au (Fe@MPNs-Au) system with high efficiency to catalyze the reduction of 4-nitrophenol. The obtained experimental results showed that the catalytic rate of Fe@MPNs-Au for 4-nitrophenol could be improved from 0.4398 min −1 to 1.5804 min −1 with the increase of Au loading. Additionally, the increased Fe 3+ -tannic acid MPNs layer thickness could also enhance the catalytic rate of Fe@MPNs-Au from 0.2226 min −1 to 2.085 min −1 . More importantly, the superior magnetic properties contributed by Fe core make it possible to be easily separated and collected by a magnet from the solution after multiple catalytic reduction reaction. Finally, we hope this strategy can provide a novel paradigm for fabricating metal-based phenolic networks system by in situ coordinating reaction between self-supplied Fe sources and phenolic molecules.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
·
IF 5.518
Xiaoli Liu,Hongxia Zhang,Junping Ma,Jianbin Zheng
A novel non-enzymatic nitrite (NO 2 − ) electrochemical sensor was fabricated based on Au-poly(thionine) and tin oxide/graphene nanosheets (Au-PTH/SGN) nanocomposites . The morphology, composition and structure of the nanocomposites were characterized by Transmission electron microscopy, Energy dispersive X-ray spectroscopy, Fourier transform infrared spectroscopy , X-ray diffraction and X-ray photoelectron spectroscopy. And the results indicated that homogeneous Au NPs with a size of approximate 80 nm and network nanostructure of PTH were attached on the surface of SGN nanomaterials. It had been also verified to satisfactory electrochemical results. The linear range of the proposed sensor was five orders of magnitude wide with the range of 0.2–127.7 (R 2 = 0.9991) and 127.7–2800 (R 2 = 0.9983) μmol L −1 , the detection limit was determined to be 0.06 μmol L −1 (S/N=3) and the sensitivity were 61.92 and 43.19 μA (mmol L −1 ) −1 cm −2 , respectively. Compared with the similar type of NO 2 − sensors previously reported, the linear range was expanded by at least an order of magnitude and the detection limit was kept at the same level as the lowest. Furthermore, the constructed Au-PTH/SGN/GCE displayed fast response, excellent stability, reproducibility, and high anti-interference ability for NO 2 − detection. Moreover, the as-proposed electrode was successfully applied for detecting NO 2 − in tap water and sewage samples with recoveries ranging from 97.3% to 103.0%97.3%-103.0% and 98.7–102.6%, respectively. The present work is expected to provide a useful route and reference for designing novel high performance electrochemical sensors and broaden the applications of sensors .
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JOURNAL OF MATERIALS RESEARCH
·
2022
·Vol. 37
·期 8
·1475-1485
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IF 2.909
Xu Jiaopeng,Chen Yingbo,Cao Ming,Wang Chuanfeng,Guo Pengfei
Solar steam generation (SSG) system greatly improves the efficiency of water evaporation through heat localization, which has broad application prospects at seawater desalination and wastewater treatment. In this paper, polyamide 6-graphene oxide (PA6-GO) membrane was fabricated by nonsolvent-induced phase separation of a solution with GO-modified PA6 in formic acid. Furthermore, the PA6-GO membrane was modified by vacuum filtration of self-assembly gold nanoparticles on its surface for solar stem generation. The composite membrane obtained a light absorption rate of nearly 99.8%. Under the irradiation of 1 kW m −2 , the evaporation rate of 1.1 kg m −2 h −1 was obtained and the evaporation efficiency also reached to 75.6%. The evaporation system has the characteristics of low cost, high stability, strong acid, and alkali corrosion resistance, suggesting great potentials in seawater desalination and sewage treatment. Graphical abstract
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CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Caiqin Wang,Cheng Qian,Ting Hu,Xiaofei Yang
It is significant to promote the efficiency of solar fuel cells via improving the utilization of solar in photoelectrocatalysis. In this work, hydrogenated TiO 2 (H-TiO 2 ) nanoparticles with Ti 3+ and/or oxygen vacancy (V O ) defects were obtained and have extended light absorption to visible light region. As a photochemical component, H-TiO 2 was further coupled with Au nanoparticles to assemble photoelectrocatalyst to apply in photo-assisted electrooxidation of ethanol. Due to the existence of defects in H-TiO 2 , the peak current density on Au/H-TiO 2 is improved by 5.4% with the assistance of light irradiation, and even up to 18.3% under simulated sunlight illumination, which is much higher than that on Au/W-TiO 2 (W-TiO 2 loaded Au) under the light irradiation. Meanwhile, it is demonstrated that the charge transfer is improved on Au/H-TiO 2 with Vo due to the existence of Vo, improving the separation of excited electrons and holes. Density function theory (DFT) based theoretical calculations illustrate that the energy barrier of reaction intermediates on Au-TiO 2 with Vo defects is lower than that without Vo, indicating that Au-TiO 2 with Vo is more energetically favorable. This work highlights the possibility of using defective semiconductor nanomaterials to combine photocatalysis and electrocatalysis in solar fuel cells and to further improve the efficiency of fuel cells under solar full spectrum.
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APPLIED SURFACE SCIENCE
·
2022
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IF 7.392
Weiping Liao,Haoyi Lin,Jiaxing Zhang,Jiaqi Wang,Kaixuan Yang,Ting Su,Hongying Lü,Zhiguo Zhu
2,5-Furandicarboxylic acid (FDCA) is a potential substitute of petroleum-based terephthalic acid to manufacture polymer. The selective aerobic oxidation of renewable 5-hydroxymethylfurfural (HMF) to FDCA is a promising and appealing route for establishing sustainable and environmentally friendly chemical process. Au catalysts have exhibited exceptional catalytic performances for this highly anticipated chemical transformation, where the used support intensively impacts the catalytic productivity from the standpoint of metal-support and guest organic-support interactions. Herein, Sn-Beta zeolite was straightforward and rapidly synthesized via structural reconstruction without the auxiliary of any solvents, which was adopted as support for Au catalyst to construct bifunctional catalysts. As for Au/Sn-Beta sample, Lewis acid sites were related to Sn 4+ ions in the zeolite framework, while electronic properties and particle size of Au species were capable of being modulated by Au dosages. In addition, charge transfer from Au species to framework Sn 4+ ions resulted in the formation of Au δ+ species. Au/Sn-Beta catalyst with metal-Lewis acid cooperative active sites showed unique catalytic productivity of FDCA product in the aerobic oxidation of HMF to FDCA, whose catalytic performance was correlated with Lewis acid amounts as well as geometric and electronic effect of Au particle. Reaction mechanism analysis revealed the pathway and concrete step that Lewis acid site functioned. The aim is to provide some guidance for constructing a task-specific multifunctional supported catalyst from the view of support-enhanced effect for the catalytic conversion of biomass resource with multi-functional-groups.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Jixiang Ji,Ruru Li,Hao Zhang,Yingnan Duan,Qian Liu,Haozhi Wang,Zhurui Shen
To date, the efficient photocatalytic conversion of CO 2 into high-value C2 products remains a great challenge. Herein, the Au-CeO 2 nanocomposite with Au-O-Ce sites at the micro-interface was developed to achieve a highly selective conversion of CO 2 into C 2 H 6 . This can be partially ascribed to the formation of key intermediates of COCO* was confirmed via in-situ Fourier transform infrared (FTIR) spectroscopy, indicating that the Au-CeO 2 micro-interface could prompt the multi-electron reduction of CO* before desorption, and enable the production of C2 species. Moreover, theoretical calculations suggested that Au-O-Ce sites at the micro-interface could reduce the energy barriers for the formation of COOH* and COCO*, facilitating the production of C 2 H 6 . Therefore, the Au-CeO 2 nanocomposite exhibited a C 2 H 6 production rate of 11.07 µmol g −1 h −1 and high electron selectivity of 93.1 % (product selectivity: 65.3 %), which is comparable with most state-of-the-art photocatalysts.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2022
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IF 4.831
Yazhou Qin,Shusheng Yin,Mingjie Chen,Weixuan Yao,Yingsheng He
The problem of opioid abuse has become a global problem. Thus, creating an urgent need for highly sensitive detection of opioid substances. In this work, we developed a method for the controllable preparation of Ag@Au nanocrystals (Ag@Au NCs) for highly sensitive SERS detection of fentanyl and its analogs. By regulating the concentration of ligands on the surface of silver seed, we successfully prepared Ag@Au NCs with three different morphologies, including core-satellite, yolk shell and hollow structure. Firstly, we explored the SERS-enhancing effect of Ag@Au NCs with different morphology using rhodamine 6G as the molecule to be tested. The results show that the core-satellite Ag@Au NCs has the best SERS effect, and the lowest detection concentration for R6G reached to 10 -10 M. Furthermore, we used the prepared core-satellite Ag@Au NCs to detect fentanyl and its five analogs, including carfentanyl, furanylfentanyl, thiofentanyl, 4-fluorobutyrfentanyl and N-4-piperidylacetanilide. Trace detection was achieved for the above six substances. For the environmental water samples spiked with fentanyl, the calculated recovery was 89.2% with an RSD value of 7.3%. Moreover, in order to realize the qualitative analysis of the characteristic peaks of different fentanyl analogs, we performed DFT calculations on the Raman spectra of the above-mentioned 6 substances. By analyzing the DFT calculation results, conventional Raman spectroscopy and SERS spectroscopy, we realized the distinction of six fentanyl analogs with similar structures.
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Frontiers in Pharmacology
·
2022
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IF 5.988
Chenxi Li,Rui Liu,Yurong Song,Youwen Chen,Dongjie Zhu,Liuchunyang Yu,Qingcai Huang,Zhengjia Zhang,Zeyu Xue,Zhenglai Hua,Cheng Lu,Aiping Lu,Yuanyan Liu
Rheumatoid arthritis (RA) is a chronic inflammatory disease, characterized by synovial inflammation in multiple joints. Triptolide (TP) is a disease-modifying anti-rheumatic drug (DMARD) highly effective in patients with RA and has anti-inflammatory properties. However, its clinical application has been limited owing to practical disadvantages. In the present study, hyaluronic acid (HA) hydrogel-loaded RGD-attached gold nanoparticles (AuNPs) containing TP were synthesized to alleviate the toxicity and increase therapeutic specificity. The hydrogels can be applied for targeted photothermal-chemo treatment and in vivo imaging of RA. Hydrogel systems with tyramine-modified HA (TA-HA) conjugates have been applied to artificial tissue models as surrogates of cartilage to investigate drug transport and release properties. After degradation of HA chains, heat was locally generated at the inflammation region site due to near-infrared resonance (NIR) irradiation of AuNPs, and TP was released from nanoparticles, delivering heat and drug to the inflamed joints simultaneously. RA can be penetrated with NIR light. Intraarticular administration of the hydrogels containing low dosage of TP with NIR irradiation improved the inflamed conditions in mice with collagen-induced arthritis (CIA). Additionally, in vitro experiments were applied to deeply verify the antirheumatic mechanisms of TP-PLGA-Au@RGD/HA hydrogels. TP-PLGA-Au@RGD/HA hydrogel treatment significantly reduced the migratory and invasive capacities of RA fibroblast-like synoviocytes (RA-FLS) in vitro , through the decrease of phosphorylation of mTOR and its substrates, p70S6K1, thus inhibiting the mTOR pathway.
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CALPHAD-COMPUTER COUPLING OF PHASE DIAGRAMS AND THERMOCHEMISTRY
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2022
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IF 2.004
C. Zhang,Y. Wan,X.H. Liang,M.H. Rong,G.T. Ma,L. Li,C.H. Hu,Chengying Tang
Au–Co nanoparticles (NPs) were prepared by water-phase chemical reduction method with metal precursor. The samples were coated with silica by Stöber method and characterized by ultraviolet and visible spectrophotometer (UV–vis), transmission electron microscopy (TEM) to obtain the absorption spectrum , size, composition distribution of the nanoparticles. The melting behaviors of the prepared Au 8 Co 2 NPs and Au 6 Co 4 NPs were examined by differential scanning calorimetry (DSC). It was observed by DSC measurements that two endothermic effects existed in range of 700.0 K–1350.0 K, corresponding to the melting temperatures of the nanoparticles and the bulk Au–Co alloys, respectively. The surface tension, surface segregation and surface energy of Au–Co NPs of particle size and temperature were calculated by the Butler's equation. On the basis of the obtained experimental results and the Gibbs free energy contributed by surface effects of pure elements and alloys at nanoscale, the nanophase diagrams of Au–Co system with various sizes were optimized. It was indicated that the calculated nanophase diagrams were in good agreement with the experimental results. The calculated eutectic temperatures decreased with the decrease of the size.
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Frontiers in Chemistry
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2022
·
IF 5.545
Qian Ningkang,Ji Liang,Li Xiao,Huang Jingbo,Li Junjie,Wu Xingqiao,Yang Deren,Zhang Hui
Combining the core-shell structure with the optimization of surface composition and structure in the shell is a fantastic strategy to enhance the electrocatalytic performances. Here, we synthesized trimetallic Au@PtxSny core-shell nanoparticles (NPs) with tunable composition and structure of Pt-Sn alloyed shells. Impressively, the Au@PtSn core-shell NPs with hexagonal PtSn alloyed shells exhibited the highest mass activity and specific activity toward ethanol oxidation reaction (EOR) in alkaline electrolyte, which are 13.0 and 12.7 times higher than those of the commercial Pt/C. In addition, the Au@PtSn core-shell NPs displayed the best stability compared to commercial Pt/C, with only 44.8% loss vs. 86.8% loss in mass activity after 1,000 s due to the stronger anti-poisoning ability for reaction intermediates. The theory calculations reveal that the introduction of Au core and alloying Pt with Sn both endow Pt with an appropriate d-band center, and thus effectively boosting the EOR activity.
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RSC Advances
·
2022
·Vol. 12
·期 34
·21875-21884
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IF 4.036
Ruimeng Sun,Ruijuan Lv,Yang Zhang,Ting Du,Yuhan Li,Lixia Chen,Yanfei Qi
The catalytic properties of bimetallic nanoparticles have been widely studied by researchers in many fields. In this paper, core–shell Cu/Au nanoparticles (Cu/Au NPs) were synthesized by a simple and mild one-pot method, and their peroxidase activity was proved by catalyzing the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) with color change to blue. The change of solution color and absorbance strongly depends on the concentration of H2O2, so it can be used for direct detection of H2O2 and indirect detection of glucose. What's more, GSH can efficiently react with the hydroxyl radicals from H2O2 catalyzed by core–shell Cu/Au NPs to inhibit the production of ox-TMB. Thus, the concentration of GSH can be determined by the decrease in the absorbance of the solution at 652 nm. The results showed that our proposed strategy had good detection range and detection limit for the detection of glucose and GSH. This method has been used in the detection of practical samples and has great application potential in environmental monitoring and clinical diagnosis.
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