ACS Applied Materials & Interfaces
·
2020
·
IF 8.758
Jingyu Lei,Jiahang Chen,Huiming Zhang,Ahmad Naveed,Jun Yang,Yanna Nuli,Jiulin Wang
Sulfurized pyrolyzed poly(acrylonitrile) (S@pPAN) demonstrates high sulfur utilization, no polysulfide dissolution, no self-discharge, and extremely stable cycling. Its precursor, PAN, directly determines the performances of cathode materials, including the sulfur content and its utilization for S@pPAN composite materials. Adopting PAN with the molecular weight approaching 550,000 as the precursor, the sulfur content in S@pPAN approaches 55 wt %, and its reversible specific capacity was 901 mAh g–1(composite) at 50 °C with sulfur utilization over 98%. Moreover, it enabled stable cycling and excellent high rate capability with a specific capacity of 645 mAh g–1 at 5 C. These significantly enhanced electrochemical properties are mainly due to the high molecular weight of the PAN precursor, which provides more space to accommodate amorphous sulfur, along with improved interfacial resistance of S@pPAN.
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JOURNAL OF MOLECULAR RECOGNITION
·
2021
·Vol. 34
·期 11
·e2930
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IF 2.137
Haipeng Ye,Ji Shao,Yanpeng Shi,Siwei Tan,Kewen Su,Ling Zhang,Xiaoyue Shan
In this study, magnetic molecularly imprinted polymers (MMIPs) were prepared and used as sorbents for extraction of S-phenylmercapturic acid (S-PMA) from urine samples, followed by high-performance liquid chromatography ultraviolet-visible (HPLC-UV/Vis) analysis. The MMIPs were synthesized by the copolymerization reaction of (phenylthio) acetic acid (template molecule), methacrylic acid (functional monomers) and ethylene glycol dimethacrylate (cross-linkers). The morphology, structure property and surface groups of the prepared MMIPs were characterized by scan electron microscopy, transmission electron microscopy, infrared spectroscopy, X-ray diffraction pattern, thermogravimetric analyses, Brunauer-Emmett-Teller and vibrating sample magnetometer. The selectivity of the MMIPs was investigated in the presence of interferents. Various parameters affecting the S-PMA extraction efficiency were investigated, including MMIPs amount, pH, sample volume, desorption solvent, as well as extraction and desorption time. The obtained optimal parameters were as follows: MMIPs amount (20 mg), pH (3.0), sample volume (5 mL), desorption solvent (methanol/acetic acid [9/1, v/v]), extraction time (30 minutes) and desorption time (2 minutes). The method was validated according to the Food and Drug Administration Guidance for Industry on Bioanalytical Method Validation. The calibration curve for the analyte was linear in the concentration range of 0.030-1.0 mg/L ( r = 0.9995). The LOD and LOQ of the method were 0.0080 and 0.0267 mg/L, respectively. The enrichment factor of the MMIPs was 5. The relative standard deviations of intra- and inter-day tests were in the range of 3.8-5.1% and 3.9-6.3%, respectively. The recoveries at three different concentrations of 0.10, 0.50 and 0.80 mg/L ranged between 95.2% and 98.6%. In addition, the MMIPs could be reused for at least eight times. The proposed method was successfully applied to the determination of S-PMA in urine samples. In addition, this developed method could be used as a tool in the early screening and clinical diagnosis of benzene intoxication.
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Journal of Materials Chemistry A
·
2019
·Vol. 7
·期 39
·22453-22462
·
IF 10.733
Liang Yan,Bing Zhang,Junlu Zhu,Zhonggang Liu,Haiyan Zhang,Yunyong Li
Exploring highly efficient and cost-effective electrocatalysts has become imperative for neutral-pH water splitting, which is environmentally friendly and can reduce the cost of electrolysis systems. Here, we report an effective strategy to design a novel type of callistemon-like Zn and S codoped CoP nanorod clusters by introducing both Zn and S into cobalt phosphide, thereby creating electrocatalysts for highly efficient and stable neutral water splitting. The best Zn and S codoped CoP nanorod clusters on carbon paper (Zn,S–CoP NRCs/CP) require overpotential values of 67 and 391 mV for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) at 10 mA cm−2 in 1.0 M phosphate-buffered solution, respectively. Remarkably, this enables a neutral electrolyzer to deliver 10 mA cm−2 at a low cell voltage of 1.70 V, which is superior to those afforded by the Pt/C/CP‖IrO2/CP couple and most of the state-of-the-art electrocatalysts. Impressively, this electrolyzer can be powered by an AA battery (∼1.5 V). Density functional theory computations and systematic experiments have verified that the improved HER and OER activities originate from the optimized electronic structures that can facilitate the adsorption and desorption of hydrogen intermediates after introducing Zn and S and accelerating the formation of oxygenated intermediates on CoOOH, respectively. This work provides a new strategy to boost the performance of transition metal phosphides for neutral water or seawater splitting.
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SOLAR ENERGY
·
2019
·
IF 4.674
Huiling Cai,Liquan Yao,Yingsen Xia,Chunyan Dao,Jianmin Li,Limei Lin,Zhiping Huang,Guilin Chen
In this work, a three-step (sulfurization-selenization-sulfurization) annealing process was designed to optimize the surface constitution of Cu 2 ZnSn(S, Se) 4 (CZTSSe) thin films, which was prepared by oxide nanoparticles-based approach. The devices with the Mo/CZTSSe/CdS/ZnMgO/ZnO:Al/Al structure were fabricated and their performances were studied. The additional post-sulfurization with low toxicity sulfur powder has negligible impact on the structure, morphology and composition of CZTSSe bulk, however, it improves open circuit voltage of device significantly. The open circuit voltage can be increased significantly from 408 mV (without surface sulfurization) to 497 mV (with surface sulfurization). This is benefited from the increase of surficial sulfur content and the broadening of the surface band-gap of the CZTSSe thin film. The result is confirmed by X-ray photoelectron spectroscopy analysis. Such a crucial three-step annealing process promotes the power conversion efficiency from 4.71% (2-step) to 6.37% (3-step), which is the champion efficiency of oxide precursor derived CZTSSe solar cell.
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CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Shizong Wang,Yong Liu,Jianlong Wang
In this study, the iron and sulfur co-doped graphite carbon nitride (FeO y /S-g-C 3 N 4 ) was easily prepared by one-step pyrolysis using thiourea and ferric chloride hexahydrate as precursors and applied to activate peroxymonosulfate (PMS) for the degradation of sulfamethoxazole (SMX). The characterization results showed that iron existed as Fe 2 O 3 and Fe 3 O 4 . Partial nitrogen atoms in the frame of g-C 3 N 4 were substituted by sulfur atoms. FeO y /S-g-C 3 N 4 can effectively activate PMS to produce sulfate radicals, hydroxyl radicals and singlet oxygen contributing to the SMX degradation. According to the density functional theory (DFT) calculation, the co-doping of iron and sulfur altered the charge density and its distribution of g-C 3 N 4 surface, which enhanced the PMS activation. The effect of initial concentrations of SMX and PMS, pH, temperature and inorganic ion concentrations on SMX degradation was investigated. 0.8 mM of PMS could degrade up to 10 mg/L of SMX. The initial pH had no obvious effect on the SMX degradation. Higher temperature accelerated the SMX degradation, and the activation energy was calculated to be 43.7 kJ/mol. The effect of inorganic ions was dependent on their initial concentration. Based on the comparison of XPS spectrum before and after reaction, the decreased catalytic activity of FeO y /S-g-C 3 N 4 after five cycle reuse was due to the breakdown of surface functional groups. Seven intermediate products were identified, and the possible degradation pathway was proposed. This study could provide a facile and cost-effective method to synthesize the efficient activator of PMS, and a mechanistic insight into PMS activation by FeO y /S-g-C 3 N 4 for the degradation of emerging pollutants in water and wastewater.
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CARBON
·
2019
·
IF 7.466
Jian Yang,Fei Xiang,Heng Guo,Liping Wang,Xiaobin Niu
It has been a major challenge to dispose the unrenewable high-performance polymers (HPPs) after their large-scale application in our society. Here we report an approach to reuse one kind of HPP as carbon and sulfur sources in synthesizing nitrogen and sulfur dual-doped honeycomb-like porous carbon catalysts for oxygen reduction reaction. Briefly, poly(phenylene sulfide sulfone) with S atoms in polymer chain as sulfur source, dicyandiamide as nitrogen source and SiO 2 nanoparticles as hard-template are pyrolyzed in designed temperatures under argon atmosphere. Then N, S dual-doped carbon catalysts (N, S@C) are obtained after subjected etching treatment. By adjusting moderate amount of SiO 2 , the optimized catalyst (denoted as N, S@C M -1000) pyrolyzed at 1000 °C, shows best ORR electrocatalytic activity in alkaline environment. Impressively, when N, S@C M -1000 is used as a cathode catalyst, the corresponding assembled zinc-air batteries exhibit a maximum power density of 90 mW cm −2 with long-term durability and high rate capacity. Therefore, this work provides a feasible way to resolve and reuse the unrenewable HPP for synthesizing heteroatom doped carbon-based catalysts.
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APPLIED SURFACE SCIENCE
·
2019
·
IF 5.155
Weixuan Zeng,Yuan Bian,Sheng Cao,Anquan Zhu,Lulu Qiao,Yongjin Ma,Pengfei Tan,Quanyin Ma,Rui Dong,Jun Pan
Visible light-driven photocatalytic hydrogen production has been deemed a potential means to solve the increasingly serious energy shortage problem. Herein, two dimensional (2D) Sr 2 Ta 2 O 7 /S-doped g-C 3 N 4 nanocomposites that applied in photocatalytic water reduction were fabricated through thermal condensation of thiourea with hydrothermal-prepared Sr 2 Ta 2 O 7 . The resulted Sr 2 Ta 2 O 7 /S-doped g-C 3 N 4 nanocomposite exhibited enhanced hydrogen evolution rate (11.36 μmol g −1 h −1 ) under visible light irradiation, which is about 3.5 times higher than that of pure S-doped g-C 3 N 4 . In light of the UV–vis diffuse reflectance spectroscopy, Mott-Schottky curve and photoluminescence spectra, the enhanced photocatalytic performance could be mainly attributed to the conduction band difference between Sr 2 Ta 2 O 7 and S-doped g-C 3 N 4 . In addition, transient photoluminescence spectra, electrochemical impedance spectra and photocurrent responses proved that the presence of Pt cocatalyst also plays an important role in facilitates the transport of photoexcited electron-hole pairs, subsequently promoting the photocatalytic performance.
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Energy Technology
·
2019
·Vol. 7
·期 9
·1900247
·
IF 3.163
Pengyuan Gao,Yun Lu,Shuyi Deng,Xun Cui,Qing Zhang,Yingkui Yang
Homogeneous confinement of metal oxide nanoparticles into the heteroatom-doped carbon matrix is highly desirable but remains challenging to develop high-performance anode materials. Herein, a facile simultaneous polymerization of 2-thiophenemethanol (ThM) and titanium ethoxide (TTEO) is proposed to incorporate ultrafine anatase TiO 2 nanocrystals into the continuous S-doped carbon framework by carbonizing the as-produced TiO 2 /poly(2-thiophenemethanol) composites. This in situ crafting process spatially suppresses the growth of TiO 2 by the polymerization of ThM, thus producing size-adjustable TiO 2 nanocrystals (5–50 nm) by tailoring the ratio of TTEO to ThM. It is found that smaller TiO 2 nanocrystals are generated using the lower TTEO-to-ThM ratio. When used as lithium-ion batteries (LIBs) anode, TiO 2 /S-doped carbon (TSC) shows larger reversible capacity, superior rate capability, and better cycling stability compared to pure TiO 2 . A typical TSC with the smallest TiO 2 nanocrystals (8 nm) shows the reversible capacity as high as 386 mAh g −1 at 50 mA g −1 , and retains 55% of initial capacity at 500 mA g −1 , and 96.8% capacity after 500 cycles at 1000 mA g −1 . The excellent electrochemical performance is attributed to the shortened ion diffusion path of ultrafine TiO 2 and the improved electronic conductivity, structural stability, and surface/interface nature by the S-doped carbon matrix.
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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
·
2019
·
IF 3.571
Bowen Tang,Wu Dai,Lijun Qi,Qi Zhang,Chunni Zhang
A delta class glutathione S-transferase gene (BoGSTd2) is identified from Bradysia odoriphaga for the first time. Developmental expression analysis showed that expression of BoGSTd2 is significantly higher in the fourth instar larval stage and the adult stage. Tissue-specific expression analysis found that BoGSTd2 was expressed predominantly in the midgut and Malpighian tubules in the fourth instar larvae and the abdomen of adults. Expression of BoGSTd2 was significantly upregulated following exposure to chlorpyrifos and clothianidin. In vitro inhibition and metabolic assays indicated that recombinant BoGSTd2 could not directly metabolize chlorpyrifos and clothianidin. Nevertheless, disk diffusion assays indicated that BoGSTd2 plays an important role in protection against oxidative stress. RNAi assays showed that BoGSTd2 participates in the elimination of reactive oxygen species induced by chlorpyrifos and clothianidin. These results strongly suggest that BoGSTd2 plays an important role in chlorpyrifos and clothianidin detoxification in B. odoriphaga by protecting tissues from oxidative stress induced by these insecticides.
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Journal of the Taiwan Institute of Chemical Engineers
·
2019
·
IF 3.834
Hongyu Cen,Zhenyu Chen,Xingpeng Guo
N and S co-doped carbon dots (N, S-CDs) were synthesized and used as corrosion inhibitors for the first time in this study. The inhibition performance of N, S-CDs for carbon steel in CO 2 -saturated NaCl solution was investigated. Results showed that N, S-CDs can effectively protect carbon steel from corrosion and the inhibition efficiency increases as the concentration of N, S-CDs increases, reaching 93% at 50 mg/L. Even at the low concentration, such as 10 mg/L N, S-CDs, the corrosion current density reduces from 1.472 × 10 −4 A·cm −2 in the blank condition to 2.99 × 10 −5 A·cm −2 after 12 h immersion. N, S-CDs can adsorb on carbon steel through their functional groups and nanoparticles made up of N, S-CDs can form a hydrophobic film on the metal surface, whose thickness was about 40 nm. A theoretical model is established to describe the inhibition mechanism of N, S-CDs.
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APPLIED SURFACE SCIENCE
·
2019
·
IF 5.155
Maiyong Zhu,Qi Chen,Jingjing Tang,Wenjing Wei,Songjun Li
The combination of carbon and iron oxide has recently attracted increasing research interest in energy conversion and storage . Here, the hybrid nanostructure with N, S-codoped Fe 3 O 4 supported/embedded on/in N-doped porous carbon (NS-Fe 3 O 4 @N-PC) nanococoon was prepared via direct pyrolysis of core@shell β-FeOOH@Polypyrrole (β-FeOOH@PPy) composite. Benefiting from the synergistic effect of high redox activity of NS-Fe 3 O 4 and excellent electrical conductivity as well as good mechanical stability of N-PC, the obtained NS-Fe 3 O 4 @N-PC exhibited an enhanced specific capacitance of 866 F/g at 1 A/g along with excellent rate capability (383 F/g at 10 A/g) and improved cycling stability (78.2% of initial capacitance retained after 5000 cycles test) while applied as electrode materials of supercapacitor . Significantly, the asymmetric supercapacitor devices assembled using NS-Fe 3 O 4 @N-PC as anodes and commercial carbon nanotubes as cathodes can achieve a large stack energy density of 38.9 Wh/Kg at a stack power density of 700.2 W/Kg along with good stability (only 8.4% decay of initial capacitance after 5000 cycles at 4 A/g). The present work may provide a general approach for fabricating other metal oxide@carbon hybrid nanomaterials for various applications.
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JOURNAL OF NANOBIOTECHNOLOGY
·
2019
·Vol. 17
·期 1
·1-14
·
IF 5.345
Gasmalla Hind Baballa,Lu Xiaoquan,Shinger Mahgoub Ibrahim,Ni Lubin,Chishti Aadil Nabi,Diao Guowang
Background Iron oxide nanocomposites have received a great attention for their application in various fields like physics, medicine, biology, and material science etc., due to their unique properties, such as magnetism, electrical properties, small size, biocompatibility and low toxicity. Methods Fe 3 O 4 /Ag 3 PO 4 @WO 3 nanocomposites with different weight percent of Ag 3 PO 4 were successfully prepared through fabricated Ag 3 PO 4 /Fe 3 O 4 with WO 3 via in situ fabrication method, electrospinning involved precursor solution preparation and spinning to enhance photocatalyst performance under simulated sunlight for the degradation of methylene blue (MB) and antibacterial activity against Staphylococcus aureus ( S. aureus ). Results The photocatalytic degradation of methylene blue (MB) under simulated light irradiation indicated that the nanocomposite with 0.25 mg of Ag 3 PO 4 has the best activity. An additional advantage of these photocatalysts is magnetic recoverability, using external magnetic field and photocatalytic stability of the nanocomposites was evaluated for three cycles. In addition, using different scavengers, holes (h + ) and superoxide radical (O
·−) 2
radicals and hydroxide radical ( · OH) were identified the main oxidative species in the degradation reaction of methylene blue. Conclusions The results reveal that Fe 3 O 4 /Ag 3 PO 4 @WO 3 -0.25 nanocomposites have photocatalytic and antibacterial activity against S. aureus. The photocatalyst and mechanism based on the enhancement of electron transfer processes between Ag 3 PO 4 and WO 3 nanoparticles.
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