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Photocatalytic degradation of methyl orange using ZnO/TiO composites

Ming GE , Changsheng GUO , Xingwang ZHU , Lili MA , Wei HU , Yuqiu WANG , Zhenan HAN ,

《环境科学与工程前沿（英文）》 2009年 第3卷 第3期   页码 271-280 doi: 10.1007/s11783-009-0035-2

摘要： ZnO/TiO composites were synthesized by using the solvothermal method and ultrasonic precipitation followed by heat treatment in order to investigate their photocatalytic degradation of methyl orange (MO) in aqueous suspension under UV irradiation. The composition and surface structure of the catalyst were characterized by X-ray diffraction (XRD), field emission scanning electron microscope (FE-SEM), and transmission electron microscopy (TEM). The degradation efficiencies of MO at various pH values were obtained. The highest degradation efficiencies were obtained before 30min and after 60min at pH 11.0 and pH 2.0, respectively. A sample analysis was conducted using liquid chromatography coupled with electrospray ionization ion-trap mass spectrometry. Six intermediates were found during the photocatalytic degradation process of quinonoid MO. The degradation pathway of quinonoid MO was also proposed.

关键词： photocatalytic degradation     methyl orange     ZnO/TiO2 composites     high performance liquid chromatography mass spectrometry (HPLC-MS)    

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Simultaneous quantification of several classes of antibiotics in water, sediments, and fish muscles by liquidchromatography–tandem mass spectrometry

WEI Yimei,ZHANG Yuan,XU Jian,GUO Changsheng,LI Lei,FAN Wenhong

《环境科学与工程前沿（英文）》 2014年 第8卷 第3期   页码 357-371 doi: 10.1007/s11783-013-0580-6

摘要： Precise and sensitive methods for the simultaneous determination of different classes of antibiotics, including sulphonamides, fluoroquinolones, macrolides, tetracyclines, and trimethoprim in surface water, sediments, and fish muscles were developed. In water samples, drugs were extracted with solid-phase extraction (SPE) by passing 1000 mL of water through hydrophilic lipophilic balanced (HLB) SPE cartridges. Sediment samples were solvent-extracted, followed by tandem SPE (strong anion exchange (SAX) + HLB) clean-ups. Fish muscles were extracted by a mixture of acetonitrile and citric buffer (80:20, v/v) solution, and cleaned by SPE. Liquid chromatography–tandem mass spectrometry (LC-MS/MS) with multiple reaction monitoring (MRM) detection was employed to quantify all compounds. The recoveries for the antibiotics in the spiked water, sediment, and fish samples were 60.2%–95.8%, 48.1%–105.3%, and 59.8%–103.4%, respectively. The methods were applied to samples taken from Dianchi Lake, China. It showed that concentrations of the detected antibiotics ranged from limits of quantification (LOQ) to 713.6 ng·L (ofloxacin) in surface water and from less than LOQ to 344.8 μg·kg (sulphamethoxazole) in sediments. The number of detected antibiotics and the overall antibiotic concentrations were higher in the urban area than the rural area, indicating the probable role of livestock and human activities as important sources of antibiotic contamination. In fish muscles, the concentration of norfloxacin was the highest (up to 38.5 μg·kg ), but tetracyclines and macrolides were relatively low. Results showed that the methods were rapid and sensitive, and capable of determining several classes of antibiotics from each of the water, sediment, and fish matrices in a single run.

关键词： antibiotics     liquid chromatography–tandem mass spectrometry (LC-MS/MS)     water     sediment     fish muscle    

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Perfluorocarboxylic acids (PFCAs) and perfluoroalkyl sulfonates (PFASs) in surface and tap water around Lake Taihu in China

Yong QIU, He JING, Hanchang SHI,

《环境科学与工程前沿（英文）》 2010年 第4卷 第3期   页码 301-310 doi: 10.1007/s11783-010-0236-8

摘要： Perfluorinated compounds (PFCs) are ubiquitously distributed in the environment mainly as perfluoro-carboxylic acids (PFCAs) and perfluoroalkyl sulfonates (PFASs). In this paper, six PFCAs and two PFASs were quantified in surface and tap water samples from 12 sites around Lake Taihu near Shanghai City in East China. Predominant PFCs were perfluorooctanoic acid (PFOA) and perfluorooctane sulfonate (PFOS), of which the concentration ranges were 6.8–206 and 1.2–45 ng·L, the geometric means were 35.3 and 9.4 ng·L, and the median (quartile range) values were 31.4 (34.4) and 10.4 (10.7) ng·L, respectively. Other PFCs were also detected but in much lower concentrations than PFOA. The sources of the PFCs were expected to be direct industrial discharges in the Lake Taihu area, and this area was also a possible source of PFCs contaminations in Shanghai district in the downstream. PFCs distributions were found different in the upstream, downstream and north part of Lake Taihu. Occurrences of PFCs in the tap water in Lake Taihu area indicated their exposure to the local people. A brief estimation of the environmental risks by PFCs implied no acute or immediate risks from PFCs to local human health, but chronic risks from PFOA in the tap water should be considered in the downstream regions.

关键词： surface and tap water     perfluorocarboxylic acids (PFCAs)     perfluoroalkyl sulfonates (PFASs)     Lake Taihu area     ultra performance liquid chromatography with tandem mass spectrometry (UPLC-MS)    

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Freshwater algae chemotaxonomy by high-performance liquid chromatographic (HPLC) analysis

Yansong HOU, Wei LIANG, Liping ZHANG, Shuiping CHENG, Feng HE, Zhenbin WU

《环境科学与工程前沿（英文）》 2011年 第5卷 第1期   页码 84-91 doi: 10.1007/s11783-010-0283-1

摘要： The study of community composition of algae is essential for understanding the structure and dynamics of the aquatic ecosystem and for evaluating the eutrophic level of the water body. A high-performance liquid chromatographic (HPLC) method based on a reverse-phase C nonpolar column was developed for the main algal taxa, which includes cyanophytes, bacillariophytes, euglenophytes, dinophytes, and chlorophytes. Based on the elution order using HPLC, 19 pigments were identified, and they were chlorophyllide , 19′-butanoyloxyfucoxanthin, chlorophyll + , phephorbides , peridinin, methyl-chlorophyllide , fucoxanthin, neoxanthin, violaxanthin, myxoxanthophyll, diadinoxanthin, diatoxanthin, lutein, zeaxanthin, chlorophyll allomer, chlorophyll , chlorophyll allomer, chlorophyll , and β,β-carotene. A comparison study of cell microscopic counts and accessory pigment analysis indicated that HPLC analysis could be a useful tool for monitoring phytoplankton communities and their abundance.

关键词： high-performance liquid chromatographic (HPLC)     algae     pigment     chemotaxonomy    

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Trace analysis of off-flavor/odor compounds in water using liquid-liquid microextraction coupled withgas chromatography—positive chemical ionization-tandem mass spectrometry

Jian LU,Paul S. WILLS,P. CHRIS WILSON

《环境科学与工程前沿（英文）》 2016年 第10卷 第3期   页码 477-481 doi: 10.1007/s11783-015-0820-z

摘要： A rapid, inexpensive and laboratory friendly method was developed for analysis of off-flavor/odor compounds in fresh and salt water using gas chromatography with chemical ionization-tandem mass spectrometry. Off-flavor/odor compounds included geosmin, 2-methylisoborneol (MIB), 2-isobutyl-3-methyoxypyrazine (IBMP), and 2-isopropyl-3-methoxypyrazine (IPMP). Using this method, a single sample can be extracted within minutes using only 1 mL of organic solvent. The ion transitions for IPMP, IBMP, MIB, and geosmin were 153>121, 167>125, 152>95, and 165>109, respectively. The linearity of this method for analyzing MIB ranged from 4 to 200 ng·L , and from 0.8 to 200 ng·L for the other analytes. Method recoveries ranged from 97% to 111% and percent relative standard deviations ranged from 3% to 9%, indicating that the method is accurate, precise, and reliable.

关键词： off-flavor/odor compounds     liquid-liquid microextraction     gas chromatography-tandem mass spectrometry    

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Detecting

Chengkun WANG, Xiaojian ZHANG, Jun WANG, Chao CHEN

《环境科学与工程前沿（英文）》 2012年 第6卷 第6期   页码 770-777 doi: 10.1007/s11783-012-0412-0

摘要： nitrosodimethylamine (NDMA) and several other nitrosamines have been detected as disinfection by-products in drinking waters in many countries around the world. An ultra-performance liquid chromatography-tandem mass spectrometry method with solid phase extraction sample preparation was developed to study the occurrence of nitrosamines in several water treatment plants and distribution systems in China. Isotope labeled nitrosodi- propylamine-d14 (NDPA-d14) was selected as the internal standard for quantification. The solid phase extraction procedures including pH, enrichment process and MS/MS parameters including capillary voltage, cone gas flow, cone voltage, collision energy were optimized to give average recoveries of 26% to 112% for nine nitrosamine species. The instrument detection limits were estimated to range from 0.5 to 5 μg·L for the nine nitrosamine species. NDMA and several other nitrosamines were found at fairly high concentrations in several water treatment plants and distribution systems. NDMA was found in all locations, and the highest concentrations in cities B, G, T, and W were 3.0, 35.7, 21.3, and 19.7 ng·L , respectively. A wide range of nitrosamines concentrations and species were observed in different locations. Higher concentrations of nitrosamines were detected in distribution systems that were further away from the treatment plants, suggesting that the contact time between the residual disinfectant and natural organic matter may play an important role in the formation of these compounds.

关键词： N-nitrosamines     water treatment plant     distribution system     ultra-performance liquid chromatography-tandem mass spectrometry    

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An efficient resin for solid-phase extraction and determination by UPLCMS/MS of 44 pharmaceutical personal

Feng Zhu, Zhijian Yao, Wenliang Ji, Deye Liu, Hao Zhang, Aimin Li, Zongli Huo, Qing Zhou

《环境科学与工程前沿（英文）》 2020年 第14卷 第3期 doi: 10.1007/s11783-020-1228-y

摘要： A hydrophilic resin (GCHM) was facile synthesis and characterized. Average absolute recovery of GCHM (75.6%) performs better than Oasis® HLB. Detection limits of method (SPE-UPLC-MS/MS) ranged between 0.03 and 0.6 ng/L. 22 PPCPs were determined in environmental waters ranging from 0.5 to 1590 ng/L. In this study, a hydrophilic resin named GCHM was fabricated based on poly(N-vinyl pyrrolidone-co-divinylbenzene), characterized, and applied as a solid-phase extraction (SPE) material. Up to 44 pharmaceuticals and personal care products (PPCPs) belonging to 10 classes were recovered in environmental water samples. Different variables affecting extraction, such as adsorbent amount, sample pH, and loading speed, were optimized. Under optimal conditions, the average absolute recovery of 44 PPCPs was 75.6% using GCHM, indicating a better performance than the commercial Oasis® HLB. SPE with home-made hydrophilic polymeric sorbent followed by ultra-performance liquid chromatography and tandem mass spectrometry was validated, and the method achieved good linearity (r2>0.991, for all analytes). In addition, the method detection limits of target compounds ranged from 0.03 to 0.6 ng/L. The developed method was applied to determine PPCPs in 10 environmental water samples taken from the Yangtze River, Huaihe River, and Taihu Lake, 1 groundwater sample from Changzhou in Jiangsu Province, 1 wastewater sample from Xiamen and 2 seawater samples from the Jiulong River in Fujian Province, China. In these samples, 22 compounds were determined at levels ranging from 0.5 to 1590 ng/L.

关键词： Hydrophilic resin     Solid phase extraction     Pharmaceuticals and personal care product     Ultra-performance liquid chromatography and tandem mass spectrometry     Environmental water    

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Simultaneous analysis of five taste and odor compounds in surface water using solid-phase extraction and gas chromatography-massspectrometry

Wenfeng SUN, Ruibao JIA, Baoyu GAO

《环境科学与工程前沿（英文）》 2012年 第6卷 第1期   页码 66-74 doi: 10.1007/s11783-010-0257-3

摘要： In this paper, a method using solid-phase extraction (SPE) and gas chromatography-mass spectrometry (GC-MS) was developed to simultaneously analyze five taste and odor compounds in surface water, i.e., 2-methylisoborneol (2-MIB), 2,4,6-trichloroanisole (TCA), 2-isopropyl-3-methoxy pyrazine (IPMP), 2-isobutyl-3-methoxy pyrazine (IBMP), and -1,10-dimethyl- -9-decalol (geosmin, GSM). The mass spectrometry was operated in selective ion monitoring (SIM) mode. Three kinds of SPE columns and three eluting solvents were compared, the C18 column was chosen as optimum SPE column, and methanol was chosen as the optimum eluting solvent. It was found that the method showed good linearity in the range of 1–200 ng·L and gave detection limits of 0.5–1.5 ng·L for individual compounds. Good recoveries (93.5%–108%) and relative standard deviations (1.58%–7.31%) were also obtained. Additionally, concentrations of these taste and odor compounds in Jinan’s surface and drinking water were analyzed by applying this method, and the results showed that GSM and 2-MIB were the dominant taste and odor compounds in Jinan’s raw water.

关键词： solid-phase extraction (SPE)     gas chromatography-mass spectrometry (GC-MS)     taste and odor compounds     surface water     micropollutant    

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Fast determination of tobramycin by reversed-phase ion-pair high performance liquid chromatography with

Liang ZHU, Jingkang WANG

《化学科学与工程前沿（英文）》 2013年 第7卷 第3期   页码 322-328 doi: 10.1007/s11705-013-1348-z

摘要： A simple and direct method without a derivation step for routine analysis of tobramycin has been developed. This method used reversed-phase ion-pair high performance liquid chromatography (HPLC) with a refractive index (RI) detector and a C18 column which is stable at pH above 1.00. The presence of 4.50 mg·mL trifluoroacetic acid (TFA) in the mobile phase improved the protonation of tobramycin and the formation of ion-pairs, and thus reduced its hydrophility. This unique separation–detection combination showed good linearity with correlation coefficients 0.9996 in the concentration range of 0.25–2.50 mg·mL . The quantitation limit and detection limit were determined to be 0.23 mg·mL and 0.071 mg·mL , respectively. Tobramycin was recovered in 98.00%, 98.84% and 99.64% for tobramycin solutions at concentrations of 2.25 mg·mL , 1.50 mg·mL and 0.75 mg·mL , respectively. The relative standard deviations for six spiked samples ranged from 0.20% to 2.40%, indicating a good reproducibility of this method.

关键词： tobramycin     aminoglycoside     refractive index detector     high-performance liquid chromatography     ion-pairing    

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Determination of persistent organic pollutants by gas chromatography/laser multiphoton ionization/time-of-flightmass spectrometry

Osamu SHITAMICHI, Taiki MATSUI, Yamei HUI, Weiwei CHEN, Totaro IMASAKA

《环境科学与工程前沿（英文）》 2012年 第6卷 第1期   页码 26-31 doi: 10.1007/s11783-011-0374-7

摘要： An authentic mixture of polychlorinated biphenyls was measured using a short wide-bore capillary column for the group separation of major components present in an actual sample of Kanechlor. The limits of detection were improved by ca. 2 fold in comparison with those obtained using a conventional capillary column, since the retention time was reduced and the amount of analytes introduced into the mass spectrometer per unit time could be increased. On the other hand, surface-water and sediment samples containing polycyclic aromatic hydrocarbons (PAHs) were collected from the river located in the vicinity of a waste water treatment plant. Even acenaphthylene, a minor component of the mixture could be measured for the sediment sample, and the concentrations were determined for several heavy PAHs. As demonstrated, a technique involving laser multiphoton ionization/time-of-flight mass spectrometry was useful as a sensitive and selective analytical tool for the trace analysis of persistent organic pollutants in an environmental sample.

关键词： polychlorinated biphenyls (PCBs)     polycyclic aromatic hydrocarbons (PAHs)     laser multiphoton ionization/time-of-flight mass spectrometry (MPI/TOF-MS)    

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Characteristics and removal mechanism of the precursors of N-chloro-2,2-dichloroacetamide in a drinking water treatment process at Taihu Lake

《环境科学与工程前沿（英文）》 2021年 第15卷 第5期 doi: 10.1007/s11783-020-1338-6

摘要：

• N-Cl-DCAM, an emerging N-DBP in drinking water was investigated.

关键词： N-chloro-2     2-dichloroacetamide     Liquid chromatography with tandem mass spectrometry     Precursors     Removal efficiency     Ozonation integrated with biological activated carbon    

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Application of high-speed counter-current chromatography coupled with high performance liquid chromatography

Shengguo DENG, Zeyuan DENG, Yawei FAN, Jing LI, Rong LIU, Dongmei XIONG,

《化学科学与工程前沿（英文）》 2009年 第3卷 第4期   页码 375-382 doi: 10.1007/s11705-009-0247-9

摘要： Quercetin-3--sambubioside Quercetin-3--β-D-xylopyranosyl (1→2)-β-D-glucopyranoside was separated and purified by semi-preparative high-speed counter-current chromatography (HSCCC) with a two-phase-solvent system composed of ethyl acetate-n-butanol–water (4∶1∶5, v/v) from the leaves of (Lotus). A total of 5.0mg of the targeted compound with a purity of 98.6% as determined by high performance liquid chromatography (HPLC) was obtained from 100m g of the crude extract cleaned up by AB-8 macroporous resin in a one-step separation. Quercetin-3--sambubioside was a novel flavonoid glycoside from the leaves of , and its chemical structure was identified by means of ESI-MS, 1D NMR and 2D NMR.

关键词： two-phase-solvent     flavonoid glycoside     high-speed counter-current     macroporous     counter-current chromatography    

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Effects of fatty acid chain length and degree of unsaturation on the surface activities of monoacyl trehaloses

Yue-E SUN, Wenshui XIA, Xueyan TANG, Zhiyong HE, Jie CHEN,

《化学科学与工程前沿（英文）》 2009年 第3卷 第4期   页码 407-412 doi: 10.1007/s11705-009-0255-9

摘要： The surface properties of monoacyl trehaloses with different acyl chains were investigated at 30°C, 40°C, 50°C, and 60°C. Monoacyl trehaloses were enzymatically synthesized and purified with silica gel column chromatography and semi-preparative high-performance liquid chromatography (HPLC), and the purity of products was identified by mass spectrometry (MS) and nuclear magnetic resonance (NMR). The surface tension of monoacyl trehalose in pure water was measured using Doüy ring method at different temperatures. The critical micelle concentrations (CMC), surface tension at the CMC, , and residual area per molecule, , were estimated from the curves. The CMC value of unsaturated monoacyl trehalose was affected by both the degree of unsaturation and the acyl chain length, and the effect of chain length on the CMC value was much stronger than that of the unsaturation degree. However, there was no significant dependency of the value and a values on the chain length or the unsaturated degree.

关键词： high-performance liquid     tension     different     spectrometry     chromatography    

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Pyrolysis behaviors of oil sludge based on TG/FTIR and PY-GC/MS

Wei SONG, Jianguo LIU, Yongfeng NIE,

《环境科学与工程前沿（英文）》 2010年 第4卷 第1期   页码 59-64 doi: 10.1007/s11783-009-0152-y

摘要： Pyrolysis is an alternative technology for oil sludge treatment. Thermogravimetric Analysis-Fourier Transform Infrared Spectroscopy and Pyrolysis-Gas Chromatography/Mass Spectrometry were employed to investigate the pyrolysis process and products of oil sludge. The pyrolysis process was divided into five stages: drying and gas desorption, oil volatilization, main pyrolysis, semi-coke charring, and mineral decomposition. The main reaction temperatures ranged from 497.6 K to 753.2 K. The products were mainly composed of pairs of alkane and alkene (carbon number ranges from 1 to 27). The mechanisms consisted of random chain scission followed by end chain scission at high temperatures with volatilization occurring during the whole process. This study is useful not only for the proper design of a pyrolysis system, but also for improving the utilization of liquid oil products.

关键词： oil sludge     pyrolysis     Thermogravimetric Analysis-Fourier Transform Infrared Spectroscopy (TG-FTIR)     Pyrolysis-Gas Chromatography/Mass Spectrometry (PY-GC/MS)    

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High-throughput metabolomics reveals the perturbed metabolic pathways and biomarkers of Yang Huang syndrome

Heng Fang, Aihua Zhang, Xiaohang Zhou, Jingbo Yu, Qi Song, Xijun Wang

《医学前沿（英文）》 2020年 第14卷 第5期   页码 651-663 doi: 10.1007/s11684-019-0709-5

摘要： High-throughput metabolomics can clarify the underlying molecular mechanism of diseases via the qualitative and quantitative analysis of metabolites. This study used the established Yang Huang syndrome (YHS) mouse model to evaluate the efficacy of geniposide (GEN). Urine metabolic data were quantified by ultra-performance liquid chromatography–tandem mass spectrometry. The non-target screening of the massive biological information dataset was performed, and a total of 33 metabolites, including tyramine glucuronide, aurine, and L-cysteine, were identified relating to YHS. These differential metabolites directly participated in the disturbance of phase I reaction and hydrophilic transformation of bilirubin. Interestingly, they were completely reversed by GEN. While, as the auxiliary technical means, we also focused on the molecular prediction and docking results in network pharmacological and integrated analysis part. We used integrated analysis to communicate the multiple results of metabolomics and network pharmacology. This study is the first to report that GEN indirectly regulates the metabolite “tyramine glucuronide” through its direct effect on the target heme oxygenase 1 . Meanwhile, heme oxygenase-1, a prediction of network pharmacology, was the confirmed metabolic enzyme of phase I reaction in hepatocytes. Our study indicated that the combination of high-throughput metabolomics and network pharmacology is a robust combination for deciphering the pathogenesis of the traditional Chinese medicine (TCM) syndrome.

关键词： metabolomics     liquid chromatography-mass spectrometry     metabolites     metabolic pathways    

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标题 作者 时间 类型 操作

Photocatalytic degradation of methyl orange using ZnO/TiO composites

Ming GE , Changsheng GUO , Xingwang ZHU , Lili MA , Wei HU , Yuqiu WANG , Zhenan HAN ,

期刊论文

Simultaneous quantification of several classes of antibiotics in water, sediments, and fish muscles by liquidchromatography–tandem mass spectrometry

WEI Yimei,ZHANG Yuan,XU Jian,GUO Changsheng,LI Lei,FAN Wenhong

期刊论文

Perfluorocarboxylic acids (PFCAs) and perfluoroalkyl sulfonates (PFASs) in surface and tap water around Lake Taihu in China

Yong QIU, He JING, Hanchang SHI,

期刊论文

Freshwater algae chemotaxonomy by high-performance liquid chromatographic (HPLC) analysis

Yansong HOU, Wei LIANG, Liping ZHANG, Shuiping CHENG, Feng HE, Zhenbin WU

期刊论文

Trace analysis of off-flavor/odor compounds in water using liquid-liquid microextraction coupled withgas chromatography—positive chemical ionization-tandem mass spectrometry

Jian LU,Paul S. WILLS,P. CHRIS WILSON

期刊论文

Detecting

Chengkun WANG, Xiaojian ZHANG, Jun WANG, Chao CHEN

期刊论文

An efficient resin for solid-phase extraction and determination by UPLCMS/MS of 44 pharmaceutical personal

Feng Zhu, Zhijian Yao, Wenliang Ji, Deye Liu, Hao Zhang, Aimin Li, Zongli Huo, Qing Zhou

期刊论文

Simultaneous analysis of five taste and odor compounds in surface water using solid-phase extraction and gas chromatography-massspectrometry

Wenfeng SUN, Ruibao JIA, Baoyu GAO

期刊论文

Fast determination of tobramycin by reversed-phase ion-pair high performance liquid chromatography with

Liang ZHU, Jingkang WANG

期刊论文

Determination of persistent organic pollutants by gas chromatography/laser multiphoton ionization/time-of-flightmass spectrometry

Osamu SHITAMICHI, Taiki MATSUI, Yamei HUI, Weiwei CHEN, Totaro IMASAKA

期刊论文

Characteristics and removal mechanism of the precursors of N-chloro-2,2-dichloroacetamide in a drinking water treatment process at Taihu Lake

期刊论文

Application of high-speed counter-current chromatography coupled with high performance liquid chromatography

Shengguo DENG, Zeyuan DENG, Yawei FAN, Jing LI, Rong LIU, Dongmei XIONG,

期刊论文

Effects of fatty acid chain length and degree of unsaturation on the surface activities of monoacyl trehaloses

Yue-E SUN, Wenshui XIA, Xueyan TANG, Zhiyong HE, Jie CHEN,

期刊论文

Pyrolysis behaviors of oil sludge based on TG/FTIR and PY-GC/MS

Wei SONG, Jianguo LIU, Yongfeng NIE,

期刊论文

High-throughput metabolomics reveals the perturbed metabolic pathways and biomarkers of Yang Huang syndrome

Heng Fang, Aihua Zhang, Xiaohang Zhou, Jingbo Yu, Qi Song, Xijun Wang

期刊论文