DYES AND PIGMENTS
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2019
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IF 4.018
Long Ma,Sixuan Xiao,Nan Wu,Shan Zhao,Debao Xiao
In the field of electrochromism , multicolor systems have ever been explored due to their potential applications in areas such as electrochromic displays. In this work, two benzene-centered organic salts, 4,4′,4''-(benzene-1,3,5-triyl)tris(1-propylpyridylium) bromide TPP 3+ 3Br − and 4,4′,4''-(benzene-1,3,5-triyl)tris(1-benzylpyridylium) bromide TBP 3+ 3Br −, were successfully synthesized and further incorporated as electrochromic materials to fabricate gel based all-in-one electrochromic devices (ECDs), respectively. It was found that, the ECDs based on these two materials displayed multicolor electrochromic behaviors, optical contrast was unambiguously exceeded 67.9%, coloration efficiency was as high as 327.7 cm 2 /C, and coloring voltage was less than −1.2 V. Considering the overall electrochromic performances of the 1,3,5-tris(4-pyridylium) bromides, it is expected that the multicolor ECDs may be applicable in the development of electrochromic enhancement of latent fingerprint based on the principle of color contrast for those deposited on the conductive and nonconductive substrates with a series of colors.
研究领域:
材料科学
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电化学
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显示技术
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DOI
高影响因子
JOURNAL OF POLYMER SCIENCE PART A-POLYMER CHEMISTRY
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2013
·Vol. 51
·期 11
·2409-2415
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IF 3.543
Jing Li,Xufeng Ni,Jun Ling,Zhiquan Shen
Polymerization of diethyl vinylphosphonate (DEVP) is achieved by using lanthanide tris(borohydride) complexes, Ln(BH 4 ) 3 (THF) 3 (Ln = Y, La, Nd, Sm, Gd, Dy, Lu) as an initiator. The characteristics and mechanism of polymerization as well as the properties of the resulting poly(diethyl vinylphophonate)s (PDEVPs) are studied. The effects of the lanthanide elements, the molar ratios of monomer to initiator ([ M ]/[ln]), reaction temperature and time on polymerization have been investigated in detail. The optimized polymerization conditions are 40 °C, 1 h in bulk with [ M ]/[ln] = 300. The kinetic study indicates that the polymerization of DEVP undergoes a controlled manner as the molecular weights (MWs) of PDEVPs increase with monomer conversion linearly maintaining moderate MW distribution (1.7–1.9). Additionally, a coordination anionic polymerization mechanism is proved by end-group analysis with ESI mass and 1 H NMR spectroscopy. The obtained PDEVPs have low glass transition temperature ( T g = −62 °C) and high thermal decomposition temperature ( T d > 300 °C) determined by differential scanning calorimetry and thermogravimetric analysis respectively. The thermosensitive behavior of PDEVP is characterized by evaluating the lower critical solution temperature of PDEVP in water by ultraviolet transmittance. © 2013 Wiley Periodicals, Inc. J. Polym. Sci., Part A: Polym. Chem. 2013, 51, 2409–2415
研究领域:
高分子化学
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材料科学
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Lei Xu,Shaoyu Tang,Dan Li,Xiao Ma,Yunqing Zhu,Jianjiang Lu,Junfeng Niu
The current study presents a comprehensive and novel attempt to degrade aqueous tri(2-chloroethyl) phosphate (TCEP) by metal-oxide-coated Ti anodes for the first time. Six metal-oxide-coated Ti electrodes (Ti/SnO 2 -Sb, Ti/SnO 2 -Sb/PbO 2 , Ti/SnO 2 -Sb/La-PbO 2 , Ti/SnO 2 -Sb/Ce-PbO 2 , Ti/SnO 2 -Sb/Ga-PbO 2 and Ti/SnO 2 -Sb/Zr-PbO 2 ) were prepared and characterized. Ti/SnO 2 -Sb/La-PbO 2 showed the highest pseudo-first-order reaction rate constant (2.1 × 10 −2 min −1 ) and lowest energy consumption (21.35 Wh L −1 ) in the degradation of 1 mg L −1 TCEP at 10 mA cm −2 , mainly because of its highest oxygen evolution potential and OH production. Higher current density and neutral condition favored TCEP degradation, while the presence of Cl − or NO 3 − could suppress the degradation. In the electrochemical degradation of 10 mg L −1 TCEP, mineralization percentage of 48.0% (mineralization current efficiency of 0.30%) and PO 4 3− release percentage of 72.7% were achieved at 150 min. By the attack of OH on the C O and C Cl bonds in TCEP molecular structure, products of chloroethanol, Cl − and PO 4 3− were released, with the major electrocatalytic degradation pathways of dechlorination and hydroxylation. Based on the results of flow cytometry, the relative toxicity to Escherichia coli effectively decreased to 4.93% in TCEP degradation. Compared with the UV-AOPs, electrochemical oxidation process is proved to be feasible and effective for mineralization and detoxification of TCEP in water.
研究领域:
环境科学
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化学工程
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电化学
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水处理
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毒理学
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DOI
高影响因子
ANALYTICAL CHEMISTRY
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2018
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IF 6.042
Fato Tano Patrice,Kaipei Qiu,Li-Jun Zhao,Essy Kouadio Fodjo,Da-Wei Li,Yi-Tao Long
Inspired by the addition-elimination catalytic mechanism of natural pyrroloquinoline quinone (PQQ) containing proteins, PQQ-modified hybrid nanomaterials have been increasingly developed recently as biomimetic heterogeneous electrocatalysts. However, up until now, no existing electrochemical approach was able to assess the intrinsic catalytic activity of PQQ sites, impeding the design of efficient PQQ-based electrocatalysts. Herein, in this work, we introduced a new method to calculate the turnover frequency (TOF) of any individual PQQ functional group for electrocatalytic oxidation of tris(2-carboxyethyl)phosphine (TCEP), through the study of single PQQ-decorated carbon nanotube (CNT) collisions at a carbon fiber ultramicroelectrode by chronoamperometry. The core advantage of this approach is being able to resolve the number of PQQ catalytic sites grafted on each individual CNT, so that the charge of any CNT collision event can be accurately translated into the intrinsic activity of the respective PQQ functional groups. The resulting collision-induced current responses clearly showed that the functionalization of CNTs with PQQ could indeed enhance its catalytic performance by 3 times, reaching a TOF value of 133 s–1 at 1.0 V vs Ag/AgCl. Such a single CNT collision technique, which is proposed for the first time in this work, can open up a new avenue for studying the intrinsic (electro)catalytic performance at a molecular level.
研究领域:
生物化学
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材料科学
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电化学
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DOI
PubMed
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
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2021
·
IF 7.963
He Liu,Jiahao Liang,Xiaodong Du,Rui Wang,Ting Tang,Xueqin Tao,Hua Yin,Zhi Dang,Guining Lu
Organophosphorus esters (OPEs), one kind of the emerging contaminants with high frequency of detection, is rather refractory in natural environment, thus posing great threat to human health. This study investigated the feasibility and mechanism of tris(2-chloroethyl) phosphate (TCEP) degradation in thermally activated persulfate (TAP) system. Influence of impact factors, such as PDS dosage, temperature, initial pH, and presence of natural water matrix (Cl − , NO 3 − , H 2 PO 4 − , NH 4 + , humic acid), were evaluated. Results showed that 100% degradation of TCEP can be achieved in TAP system in 40 min at 60 °C. SO 4 ·− as the dominant oxidant for TCEP degradation was proved by quenching experiment and verified by EPR analysis. Alkaline condition exerted great inhibitory effect by affecting the constituents of oxidative radicals. It is suggested that Cl − and H 2 PO 4 − at lower dosages promoted the degradation by stimulating ·OH production and forming oxidative radicals with better selectivity . Intermediates identified by high resolution mass spectrometer was suggested less toxic than TCEP by ECOSAR program. Meanwhile, the illustrated oxidation mechanism mainly involved radical attack at C Cl bond and cleavage of C O bond, as further confirmed by frontier electron density calculation and wavefunction analysis. Moreover, cyclic degradation of TCEP indicated the constant release of SO 4 ·− in 450 min, suggesting high efficiency and stability of PDS in TAP system. Four selected OPEs achieved complete removal in TAP system and their degradation discrepancy was further discussed based on the distinctive structures. Altogether, TAP technology can be used as an efficient method in TCEP removal with great potential for application.
研究领域:
环境科学
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化学工程
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DOI
PubMed
高影响因子
JOURNAL OF RARE EARTHS
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2020
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IF 3.104
Xiaoru Zhao,Xinyu Jiang,Dongming Peng,Jie Teng,Jingang Yu
Three-dimensional (3D) graphene oxide-tris(4-aminophenyl)amine (GO-TAPA x:y ) composites with different GO-to-TAPA mass ratios ( x : y ) were prepared by a facile one-step ultrasonic treatment. GO-TAPA x : y composites were characterized by scanning electron microscopy (SEM), nitrogen (N 2 ) adsorption-desorption isotherms, Fourier transform infrared spectroscopy (FTIR), X-ray photoelectron spectroscopy (XPS) and thermogravimetric analysis (TGA). Behavior and mechanism of GO-TAPA x:y composites for the adsorption of rare earth elements (REEs) were investigated. The adsorption capacities of GO-TAPA 1:2 composite for Yb 3+ , Er 3+ , Nd 3+ , La 3+ and Y 3+ are 30.88, 26.52, 20.60, 11.24 and 10.52 mg/g, respectively. Effects of some important parameters including GO-to-TAPA mass ratios, contact time, reaction temperature and initial Yb 3+ concentration on the adsorption were evaluated in detail. FTIR spectral and XPS analyses show that the metal complexations and ion exchanges between nitrogen/oxygen-containing species of the adsorbents and REEs are involved in the adsorption procedure besides the conventional adsorption based on specific surface area, indicating the introduction of specific molecules onto GO is beneficial to its adsorption ability. The convenient reusability and applicability of GO-TAPA x : y composites toward real samples also demonstrate their feasibility in the enrichment of REE ions.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2023
·
IF 8.6
Ding Ling Gao,Yan Xue Xue,Fei Fei Dai,Yu Xiang Liu,Na Qin,Ya Yuan Zhang,Jian Hua Chen,Qian Yang
In this study, polyaniline-p-phenylenediamine (PAPD) was employed as an amino monomer to fabricate a polyaniline-p-phenylenediamine composite membrane (PAPD/PES) with a nanoparticle-like surface morphology. Additionally, we used interfacial polymerization of Tris(hydroxymethyl)aminomethane (THAM) to hydroxylate the PAPD/PES composite membrane, resulting in the formation of a TPAPD/PES composite membrane. THAM is an economical and environmentally friendly monomer, rarely used for surface modification of composite membranes through interfacial polymerization. Following the introduction of THAM, a significant abundance of hydroxyl groups appeared on the membrane’s surface, enhancing its hydrophilicity and electronegativity. This, in turn, improved both flux and rejection capabilities. Simultaneously, the introduction of THAM led to the formation of a hydration layer growing on the membrane’s surface, further enhancing its antifouling performance. The optimal polymerization concentration (0.5 mol/L) of THAM was used to synthesize the TPAPD/PES composite membrane, resulting in a flux of 84.18 L m −2 h −1 bar −1 , which was 1.46 times higher than that of the PAPD/PES composite membrane before polymerization. Additionally, the phosphate rejection rate was determined to be 92.14 % (with an initial phosphate concentration of 10 mg P/L). Long-time running and operating pressure tests results confirmed the remarkable stability of the TPAPD/PES composite membrane. Furthermore, the phosphate separation property of the TPAPD/PES composite membrane was evaluated using real wastewater samples (with an initial phosphate concentration of 1.03 mg P/L) as the research object. After separation, the permeate displayed a phosphate concentration of 0.28 mg P/L, meeting the first-class A standard for urban sewage treatment in China (0.5 mg P/L). This indicates that the prepared TPAPD/PES composite membrane has significant potential for practical application.
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高影响因子
CHINESE JOURNAL OF CATALYSIS
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2016
·
IF 2.628
Tingting Zhang,Chuansheng He,Linbo Li,Yuqing Lin
The oxygen reduction reaction (ORR) is traditionally performed using noble-metals catalysts, e.g. Pt. However, these metal-based catalysts have the drawbacks of high costs, low selectivity, poor stabilities, and detrimental environmental effects. Here, we describe metal-free nitrogen-doped carbon nanoblocks (NCNBs) with high nitrogen contents (4.11%), which have good electrocatalytic properties for ORRs. This material was fabricated using a scalable, one-step process involving the pyrolysis of tris(hydroxymethyl)aminomethane (Tris) at 800 °C. Rotating ring disk electrode measurements show that the NCNBs give a high electrocatalytic performance and have good stability in ORRs. The onset potential of the catalyst for the ORR is −0.05 V (vs Ag/AgCl), the ORR reduction peak potential is −0.20 V (vs Ag/AgCl), and the electron transfer number is 3.4. The NCNBs showed pronounced electrocatalytic activity, improved long-term stability, and better tolerance of the methanol crossover effect compared with a commercial 20 wt% Pt/C catalyst. The composition and structure of, and nitrogen species in, the NCNBs were investigated using Fourier-transform infrared spectroscopy, scanning electron microscopy, X-ray photoelectron spectroscopy, and X-ray diffraction. The pyrolysis of Tris at high temperature increases the number of active nitrogen sites, especially pyridinic nitrogen, which creates a net positive charge on adjacent carbon atoms, and the high positive charge promotes oxygen adsorption and reduction. The results show that NCNBs prepared by pyrolysis of Tris as nitrogen and carbon sources are a promising ORR catalyst for fuel cells.
研究领域:
材料科学
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电化学
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纳米技术
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催化
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DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
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2024
·
IF 8
Seokjoon Kim,Seungjin Lee,Seokhwan Kim,Jiye Shin,Byung Seok Cha,Eun Sung Lee,Ki Soo Park
Globally, over 200 million people are at risk of exposure to high levels of arsenic due to increasing environmental pollution; thus, there is high demand for detection methods to monitor arsenic contamination in the natural environment. In this study, we developed a cost-effective method for detecting arsenite [As(III)] ions using sodium dodecyl sulfate (SDS)-coated gold nanoparticles (AuNPs) and Tris. Positively charged Tris molecules induce aggregation of AuNPs by neutralizing the negative charge of SDS; however, this is prevented by the presence of As(III), which has a high affinity for AuNPs. This proposed method is able to detect 5 parts per billion (ppb) and 1.85 ppb of As(III) through naked eye and spectrophotometric measurements, respectively. Furthermore, a chitosan-based lateral flow (LF) strip was devised to enhance the visual signal intensity by concentrating AuNPs on its test zone, since AuNPs of lower concentration were more effective for detecting low As(III) concentrations. As a result, As(III) was detected at 500 parts per trillion (ppt) without any interference from other metal ions, which is a 10-fold improvement from solution-based assays. Importantly, the colorimetric signal amplification strategy (using the chitosan-based LF strip) is versatile and can be applied to many other AuNP- or nanomaterial-based technologies. The proposed system enables the detection of As(III) in facility-limited or point-of-care settings, making it ideal for use in underdeveloped countries because it requires a small sample volume (approximately 20–30 µL) with a small amount of AuNPs, and takes only 10 min to generate colorimetric results.
研究领域:
环境科学
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纳米技术
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分析化学
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DOI
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
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2024
·
IF 8.2
Sujing Wang,Na Zheng,Qirui An,Xiaoqian Li,Yining Ji,Yunyang Li,Changcheng Chen,Zhifei Xiu
The flame retardant tri (1, 3-dichloro-2-propyl) phosphate (TDCIPP) is widely present in environmental media and organisms. People have paid much attention to the growth and developmental toxicity of TDCIPP, but there is little information about its cardiotoxicity and potential mechanisms. In this study, marine medaka ( Oryzias melastigma ) embryos were exposed to TDCIPP solutions (0, 0.05, 0.5, 5, and 50 μg/L) for 21 days to investigate the adverse effects of TDCIPP on cardiac development. The results showed that TDCIPP exposure altered the heart rate at different stages of embryonic development. In addition, 50 μg/L TDCIPP resulted in increased sinus venosus (SV)–bulbus arteriosus (BA) distance, pericardial cysts, and cardiac linearization in newly hatched fish. During embryonic development, the expression level of key genes regulating cardiac development is disturbed. The early stage of cardiac development is the sensitive window period for the toxic effects of TDCIPP. Oxidative stress was observed in newly hatched juveniles, but no significant lipid peroxidation damage was observed. In addition, vitellogenin (VTG) levels in juvenile fish were significantly reduced. Our results show that TDCIPP exposure induces cardiotoxicity in marine medaka embryos, which is induced in the early stages and promotes heart defects by amplifying inflammatory responses at a later stage.
研究领域:
环境毒理学
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发育生物学
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心血管毒理学
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DOI
PubMed
高影响因子
Nanomaterials
·
2021
·Vol. 11
·期 7
·1757
·
IF 5.076
Xiaohua Ma,Dehua Deng,Ning Xia,Yuanqiang Hao,Lin Liu
Nanocatalysts are a promising alternative to natural enzymes as the signal labels of electrochemical biosensors. However, the surface modification of nanocatalysts and sensor electrodes with recognition elements and blockers may form a barrier to direct electron transfer, thus limiting the application of nanocatalysts in electrochemical immunoassays. Electron mediators can accelerate the electron transfer between nanocatalysts and electrodes. Nevertheless, it is hard to simultaneously achieve fast electron exchange between nanocatalysts and redox mediators as well as substrates. This work presents a scheme for the design of electrochemical immunosensors with nanocatalysts as signal labels, in which pyrroloquinoline quinone (PQQ) is the redox-active center of the nanocatalyst. PQQ was decorated on the surface of carbon nanotubes to catalyze the electrochemical oxidation of tris(2-carboxyethyl)phosphine (TCEP) with ferrocenylmethanol (FcM) as the electron mediator. With prostate-specific antigen (PSA) as the model analyte, the detection limit of the sandwich-type immunosensor was found to be 5 pg/mL. The keys to success for this scheme are the slow chemical reaction between TCEP and ferricinum ions, and the high turnover frequency between ferricinum ions, PQQ. and TCEP. This work should be valuable for designing of novel nanolabels and nanocatalytic schemes for electrochemical biosensors.Keywords:electrochemical immunosensor;nanocatalyst;redox cycling;quinone
研究领域:
生物传感
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分析化学
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DOI
PubMed
高影响因子
AQUATIC TOXICOLOGY
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2020
·
IF 4.346
Hui Hao,Siliang Yuan,Shiyang Cheng,Qian Sun,John P. Giesy,Chunsheng Liu
As a typical organophosphorus flame retardant, tris (2-chloroethyl) phosphate (TCEP) has been widely detected in various environmental media. Toxicity of TCEP to vertebrates have been investigated, but potential effects on lower trophic level species were unknown to date. In this study, toxic effects and molecular mechanisms of toxic actions of TCEP on the aquatic protozoan Tetrahymena thermophila were evaluated by use of phenotypic observations, transcriptome sequencing analysis and real-time quantitative PCR detection. Exposure to 0.044, 0.411 or 4.26 mg/L TCEP for 5 days decreased the theoretical population, cell viability, number of cilia and cell size of Tetrahymena thermophila in a time- and dose-dependent manner. Meanwhile, RNA-Seq analysis indicated that exposure to 4.26 mg/L TCEP significantly changed expression of 2932 genes (up-regulation: 1228; down-regulation: 1704). Of these, expressions of 9, 10 and 17 genes that were enriched in soluble N-ethylmaleimide-sensitive factor attachment protein receptor (SNARE) interaction in vesicular transport, proteasome and endocytosis pathway respectively were down-regulated. Data collected during this study suggested that exposure to high concentrations of TCEP might affect growth and reproduction of Tetrahymena thermophila through down-regulating transcriptional levels of genes encoding proteins associated with vesicle trafficking, proteasome and endocytosis.
研究领域:
环境毒理学
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分子生物学
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原生动物学
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DOI
PubMed
高影响因子
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