FUEL
·
2019
·
IF 5.128
Xiu Chen,Haidong Li,Linzhou Zhang,Quan Shi,Suoqi Zhao,Chunming Xu
In the present paper, the molecular composition of sulfidic and thiophenic compounds in petroleum samples were selectively characterized by positive-ion electrospray ionization (ESI) Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) after cyclohexanone peroxide (CYHPO) oxidation followed by methylation . The sulfidic compounds in petroleum were mainly oxidized to sulfones by CYHPO while most of thiophenic compounds were not reacted. In the followed methylation process, the unreacted thiophenic compounds were converted to methylsulfonium. After using ammonium formate (HCOONH 4 ) as a promoter, the obtained sulfidic sulfones (O 2 S 1 class species) were selectively ionized in the form of N 1 O 2 S 1 class species under positive-ion ESI FT-ICR MS. The thiophenic methylsulfonium salts in the oxidation-methylation products were also identified by positive-ion ESI FT-ICR MS as S 1 class species. This analytical scheme was evaluated by a variety of model compounds and then applied successfully to diesel, VGO and crude oil samples to obtain the molecular composition of sulfidic and thiophenic compounds. In addition, the molecular type of biomarkers and other compounds in petroleum samples can be identified by this analytical scheme.
研究领域:
分析化学
·
石油化学
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DOI
高影响因子
Science China-Chemistry
·
2013
·Vol. 56
·期 7
·863-873
·
IF 1.327
Wang LiTao,He Chen,Liu Yang,Zhao SuoQi,Zhang YaHe,Xu ChunMing,Chung Keng H.,Shi Quan
A vacuum topped Canadian oilsands bitumen (VTB) was subjected to solvent precipitation and subsequently characterized by elemental analysis, gel permeation chromatograph (GPC), 1 H-NMR spectroscopy and negative-ion electrospray ionization (ESI) Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS). Effects of experimental conditions such as solvent types ( n -C 5 , n -C 6 , and n -C 7 ), solvent purity, and solvent washing time on asphaltenes yields, bulk composition, and molecular composition of detectable heteroatom compounds in ESI source were determined. Elemental nitrogen and sulfur were enriched in asphaltenes while elemental oxygen had comparable content in maltenes and asphaltenes. Molecular composition of asphaltenes varies with separation conditions. The N 1 and O 1 species identified by ESI FT-ICR MS were enriched in maltenes. The O 2 species exhibited two different double bond equivalents (DBE) distributions and solubility in normal paraffin solvents, indicating two types of molecular structures. Multi oxygen atom containing compounds mainly detected in asphaltenes. Compound class distributions are similar for maltenes derived from n -C 5 , n -C 6 , and n -C 7 , as well as for asphaltenes. The cyclic paraffin impurities in normal paraffin solvents had a significant influence on asphaltenes yields and heteroatom molecular composition. A portion of neutral N 1 species and acidic O 2 species adsorbed on asphaltenes could be dissolved by increasing washing time. Cautions should be exercised when interpreting the properties and composition of asphaltenes obtained with different experimental conditions.
研究领域:
石油化学
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分析化学
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DOI
高影响因子
WATER RESEARCH
·
2021
·
IF 11.236
Bingliang Zhang,Xuening Wang,Zhuoyao Fang,Shu Wang,Chao Shan,Si Wei,Bingcai Pan
ABSTRACT Ultraviolet-based advanced oxidation processes (UV-AOPs) are very promising in advanced treatment of municipal secondary effluents. However, the transformation of dissolved effluent organic matter (dEfOM) in advanced treatment of real wastewater, particularly at molecular level, remains unclear. In this study, Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR-MS) coupled with multiple statistical analysis were performed to better understand the transformation of dEfOM in UV/H 2 O 2 , UV/persulfate (UV/PS), and UV/chlorine treatments. An obvious increase in oxygen content of dEfOM was observed after every UV-AOPs treatment, and the detailed oxygenation processes were further uncovered by mass difference analysis based on 24 types of typical reactions. Generally, UV/H 2 O 2 process was subjected to the most oxygenation reactions with the typical tri-hydroxylation one (+3O), whereas di-hydroxylation reaction (+H 2 O 2 ) was dominant in UV/PS and UV/chlorine processes. Additionally, the three UV-AOPs shared the majority of precursors, and more proportions of unique products were identified for each process. The precursors with lower H/C and higher aromaticity were readily degraded by UV/chlorine over UV/H 2 O 2 and UV/PS, with the products featuring lower molecular weight. Moreover, dEfOM of high aromaticity tended to produce chlorinated byproducts through addition reactions in chlorination and UV/chlorine processes. Among these UV-AOPs, the highest reduction of both acute toxicity and specific UV absorbance at 254 nm (SUVA 254 ) was observed for UV/chlorine, implying the potential for UV/chlorine process in advanced treatment of wastewater. In addition, acute toxicity was highly correlated with SUVA 254 and CHOS compounds. This study is believed to help better understand the different fates of dEfOM in real wastewater during UV-AOPs treatment.
研究领域:
环境科学
·
废水处理
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DOI
PubMed
高影响因子
CATALYSIS TODAY
·
2021
·
IF 6.766
Jiyuan Fan,Saumitra Saxena,Chengkun Xiao,Jinlin Mei,Gang Wang,Aiping Chen,Wen Zhang,Haidong Li,Aijun Duan,William L. Roberts
Oxidative desulfurization of model oil and heavy fuel oil (HFO) was investigated under mild conditions using H 2 O 2 as an oxidant and acetonitrile as an extractant. The influence factors in the oxidation and extraction processes were evaluated and optimized. The molecular characteristics of the raw feedstock and the desulfurized oils, and the corresponding extraction phases were systematically analyzed by APPI FT-ICR MS, 1 H NMR, etc. The results showed that the desulfurization rate of dibenzothiophene reached 97.7% after 10 min reaction, while the sulfur removal efficiency of HFO was 30.7% under optimized conditions. The structures of sulfur compounds were described in heteroatom type, carbon number distribution vs unsaturation degree. The detected main sulfur-containing compounds are S 1 , S 2 , S 3 , NS, OS, O 2 S, O 2 S 2 , and O 4 S 2 . Based on the APPI FT-ICR MS results, it can be found that almost all the S 1 species have been transformed into sulfone after the oxidation process. Furthermore, the sulfone of O 2 S 1 and O 4 S 2 species in extraction phases were in double bond equivalent (DBE) range from 9 to 25 and carbon number with ≤ 40. 1 H NMR results showed that the α to aromatic CH 3 combined naphthenic CH-CH 2 group accounted for 73.2% in the extraction phase.
研究领域:
化学工程
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分析化学
·
环境科学
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DOI
高影响因子
JOURNAL OF PHARMACEUTICAL AND BIOMEDICAL ANALYSIS
·
2023
·
IF 3.4
Siyue Li,Yuanfang Sun,Yutong Gao,Xinying Yu,Chun Zhao,Xiuping Song,Fei Han,Jia Yu
Alzheimer’s disease (AD) threatens elderly human health and still lacks effective treatment. Our previous work showed that LGZGD possessed a neuroprotective effect on the Aβ 25-35 -induced neurotoxicity in differentiated PC12 cells, indicating that LGZGD may be a potential drug for treatment of AD. However, its pharmacodynamic substances which show anti-inflammatory and anti-oxidant stress activities are still unrevealed. This research aims to reveal the pharmacodynamic substances of LGZGD on Aβ 25-35 -induced PC12 cell model of AD based on a spectrum-effect relationship study by using HPLC-FT-ICR-MS method and multivariate statistical analysis. Firstly, the chemical composition spectra of different combinations of LGZGD were recorded by HPLC-FT-ICR MS. Subsequently, Aβ 25-35 -induced PC12 cell model of AD was established and pharmacodynamic experiments were conducted to evaluate their anti-inflammatory and anti-oxidant activities, respectively. Finally, the potential pharmacodynamic substances were screened out through spectrum-effect relationship study accompanied by multivariate statistical analysis including bivariate correlation analysis (BCA), grey relational analysis (GRA), principal component analysis (PCA), partial least squares regression analysis (PLSR). As a result, a total of 96 chemical consistents in different combinations of LGZGD were discovered. Among them, 7 components such as isoglabrolide, licorice saponin E2, licorice saponin N2 and licoisoflavanone were directly linked with the anti-inflammatory effects, and 14 constituents such as tumulosic acid, polyporenic acid C, dehydrotumulosic acid, dehydropachymic acid, and pachymic acid were directly correlated with the anti-oxidative stress activities. In conclusion, we combined the HPLC-FT-ICR-MS spectra with pharmacodynamic indicators to develop the spectrum-effect relationships of LGZGD for the first time, and successfully revealed its potential pharmacodynamic substances in the treatment of AD from the anti-inflammatory and antioxidant pathways in the cell model.
研究领域:
药理学
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神经科学
·
分析化学
·
中医药
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产品关联
DOI
PubMed
高影响因子
WATER RESEARCH
·
2025
·
IF 12.4
Yuanna Zhang,Wenjun Sun,Wenxuan Yin
The widespread application of UV/H 2 O 2 is limited by the empirical operational practices, which can lead to excessive energy, chemical input and the generation of uncontrollable by-products. This study presents a precise regulation approach based on the characteristics of free radical generation/reaction and the chemical transformation of organics, assessed through a pilot experiment. The findings indicated that increasing H 2 O 2 dosage was more effective than increasing UV dose in enhancing •OH generation and pollutant removal. As the H 2 O 2 dosage and UV dose increased, the relative influence of water quality on pollutant removal gradually diminished. Dissolved organic matter (DOM) in the water quality background accounted for the largest proportion of •OH scavenging (76.4 %) and the most complex component. Moreover, changes in operating conditions were accompanied by the uncontrollable production of low-molecular-weight (LMW) DOM. Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) revealed the chemical transformation of LMW DOM at the molecular level. Higher H₂O₂ dosages triggered more extensive oxidative degradation, resulting in more complex effluent compositions. Considering treatment efficiency, energy consumption, and effluent product composition, H₂O₂ dosages of 5–10 mg/L and UV doses of 350–450 mJ/cm² were identified as optimal. This research contributes to the efficient purification of organic micropollutants in water using UV/H 2 O 2 technology with low energy consumption, minimal chemical input, and relatively controllable by-products.
研究领域:
环境科学
·
水处理技术
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2022
·
IF 11.357
Yuanze Sun,Xinfei Li,Xiaomin Li,Jie Wang
Biodegradable polymers are promoted as promising alternatives for conventional non-degradable plastics, but they may also negatively impact soil ecosystems. Here, we estimated the effects of biodegradable (polylactide (PLA) and polybutylene succinate (PBS)) and non-biodegradable (polyethylene (PE) and polystyrene (PS)) microplastics at a concentration of 1% (w/w) on dissolved organic matter (DOM) in two soil types, a black soil (BS) and a yellow soil (YS), by using fluorescence excitation-emission matrix spectroscopy and ultrahigh-resolution Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR-MS). PBS significantly increased the contents of soil dissolved organic carbon (DOC) and the relative intensities of protein-like components. The turnover rates of soil DOM were statistically higher in PBS treatments (0.106 and 0.196, p < 0.001) than those in other microplastic groups. The FT-ICR-MS results indicated that more labile-active DOM molecules were preferentially obtained in biodegradable microplastic treatments, which may be attributed to the polymer degradation. The conventional microplastics showed no significant effects on the optical characteristics but changed the molecular compositions of the soil DOM. More labile DOM molecules were observed in BS samples treated with PE compared to the control, while the conventional microplastics decreased the DOM lability in YS soil. The distinct priming effects of plastic-leached DOM may trigger the DOM changes in different soils. This study provided important information for further understanding the impact of microplastics on soil carbon processes.
研究领域:
环境科学
·
土壤学
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DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 3
·123046
·
IF 7.5
Guangrong Sun,Dongquan Li,Feiyang Huang,Haibing Cong
It is a considerable challenge to identify and characterize halogenated nucleotide analogs, owing to the lack of authentic standards and the diversity of their structures. Nevertheless, nontargeted identification through high-resolution mass spectrometry (HRMS) provides an effective solution to this problem. In this study, typical nucleotides were selected as model compounds, and their binding products with N,N-dimethyl-p-phenylenediamine (DMPA) were identified to verify the feasibility of the derivatization method. The solid-phase extraction (SPE) pretreatment method and derivatization conditions were optimized to achieve optimal derivatization efficiency and detection sensitivity. Specifically, DMPA labeling was conducted at 60°C for 90 min, and the molar ratios of DMPA and 1-ethyl-3-(3-(dimethylamino)propyl)carbodiimide hydrochloride (EDC) to nucleotides were set as 5 × 10 4 and 5 × 10 3 , respectively. Ultimately, the integration of chemical derivatization with HRMS analysis significantly enhanced the detection efficiency of the target compounds. As a result, using this optimized and model compound-validated method, 22 halogenated nucleotide analogs in a single natural water body were tentatively identified, and their precise molecular formulas were assigned by FT-ICR MS. The findings for this water body could provide new perspectives for the identification of emerging compounds in similar aquatic environments and offer novel approaches for elucidating the molecular characteristics of such pollutants.
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DOI
高影响因子
FUEL
·
2020
·
IF 5.578
Xiu Chen,Haidong Li,Linzhou Zhang,Quan Shi,Suoqi Zhao,Chunming Xu
Molecular-level characterization of sulfur-containing compounds has attracted particular attention due to its relative high abundance and negative impact on the refining process. In this paper, a novel analytical method for selective ionization of sulfidic and/or isolated thiophenic compounds (thiophene rings that are not condensed with aromatic systems) and condensed thiophenic compounds (thiophene rings that are condensed with aromatic systems, DBE ≥ 6, DBE = number of rings plus double bonds to carbon) in petroleum samples was developed by using fluoroboric acid (HBF 4 ) as ionization promoter. Positive-ion electrospray ionization [(+) ESI] Fourier transform ion cyclotron resonance mass spectrometry was followed to characterize the molecular composition. Sulfidic and/or isolated thiophenic compounds were mainly ionized as protonated molecular ions ([M+H] + ), while condensed thiophenic compounds (DBE ≥ 6) were mainly ionized as molecular radical cations (M + ). The method was validated by various sulfur-containing model compounds and then applied to vacuum gas oil, crude oil and heavy oil samples. (+) ESI coupled with HBF 4 additive is a simple method for selective ionization of sulfides and thiophenes in high-sulfur-content petroleum samples and has the potential for the characterization of sulfides and thiophenes in other complex mixtures.
研究领域:
化学
·
能源科学
·
分析化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Chengzhi Zhou,Jiaqi Wang,Zongyu Yan,Zhouying Xie,Yuandong Wu,Qianwei Liang,Yanlong Sun,Ya-nan Zhang
Dissolved black carbon (DBC), particularly its optically active fraction, plays a crucial role in the photodegradation of organic pollutants. However, the transformation mechanisms of DBC's optical properties and molecular composition in UV/chlorine process remain poorly understood. In this study, we systematically investigated the photochemical evolution of rice straw-derived DBC prepared at two pyrolysis temperatures (300 °C and 500 °C) under UV/chlorine treatment, as well as their impacts on the photodegradation of acetamiprid (ACT). The results demonstrate that DBC 300 exhibited strong light absorption capacity, high aromaticity, large molecular weight, and abundant lignin-like components, whereas DBC 500 contained higher heteroatom (N, S) content, greater protein-like constituents, and enhanced reducing capacity and electron transfer capability. Under UV irradiation alone, the content of condensed aromatics, lipid-like compounds, and molecular diversity in DBC were enhanced. In contrast, chlorination reduced the light absorption capacity, humification degree, and molecular diversity of DBC. Photodegradation of ACT was primarily promoted by the generation of excited triplet DBC ( 3 DBC ⁎ ). With increasing chlorine concentration, the electron transfer capability of 3 DBC 300 ⁎ decreased, whereas that of 3 DBC 500 ⁎ increased, leading to weakened and enhanced promotion effects on ACT photodegradation, respectively. The photodegradation pathways of ACT mainly involved demethylation, hydroxylation, oxidation and C N bond cleavage. Furthermore, the photodegradation products of ACT exhibited increased toxicity toward rat and Daphnia magna , while demonstrating reduced mutagenic potential. This study provides critical insights into the photochemical transformation processes and underlying molecular mechanisms of DBC during UV/chlorine treatment.
研究领域:
环境化学
·
水处理技术
·
光化学
·
分析质谱学
·
污染物降解
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DOI
高影响因子
Environmental Science-Nano
·
2023
·Vol. 10
·期 5
·1220-1231
·
IF 7.3
Shishu Zhu,Yijun Mo,Wendan Luo,Zihan Xiao,Chao Jin,Rongliang Qiu
Soil dissolved organic matter (SDOM) forms the corona and affects the colloidal mobility of Cr (hydr)oxides. Such processes are important in evaluating Cr immobilization effectiveness. This study for the first time found that the SDOM composition instead of electrostatic interactions accounted for the significant differences in the aggregation and deposition kinetics of short-range-order Cr(OH)3 Cr(OH)3 and crystalline Cr2O3. The molecular-scale composition of SDOM associated with Cr (hydr)oxides was investigated using Fourier transform-ion cyclotron resonance-mass spectrometry (FT-ICR-MS) and Fourier transform-infrared spectroscopy (FT-IR). Low molecular-weight aromatic compounds with multiple carboxyl groups and amphiphilic segments preferentially associated with Cr(OH)3, whereas Cr2O3 mainly adsorbed high molecular-weight hydrophobic compounds. The molecular composition of SDOM associated with colloids depended on the singly coordinated hydroxyl content of Cr (hydr)oxides. The aggregation and deposition of Cr(OH)3 significantly increased with increasing SDOM loading due to the formation of more thermodynamically stable coprecipitates in solution or on the silica surface via bridging of carboxylates. A secondary zonal layer on Cr(OH)3 inhibited the coprecipitation of Cr(OH)3 with SDOM under a high SDOM loading. In contrast, the aggregation and deposition of Cr2O3 decreased with increasing SDOM loading due to the steric hindrance of hydrophobic compounds. This study highlighted the importance of corona composition in assessing the potential mobility of Cr (hydr)oxides and the stability of immobilized Cr species.
研究领域:
环境科学
·
分析化学
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DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2025
·
IF 11.3
Bingliang Zhang,Qiyi Wang,Ling Zhou,Xinqi Li,Fuyao Tong,Xiaomeng Wang,Yueke Wang,Chang Xu,Xifeng Shi,Bo Tang
Disinfection byproducts (DBPs) inevitably form during municipal wastewater disinfection, posing potential threats to human and ecological health. While UV-based advanced oxidation/reduction processes (UV-AOPs/ARPs) show promise in eliminating DBP precursors, their efficacy and mechanisms for controlling both known and unknown DBPs remain unclear. This study systemically investigated dissolved organic matter (DOM) transformation and DBP mitigation during pre-treatments of actual municipal wastewater using UV, UV/Peroxydisulfate (UV/PS), UV/H 2 O 2 , and UV/Sulfite. Combining spectroscopy, chromatography, and Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR-MS) analyses, the results demonstrated that UV/PS and UV/H 2 O 2 were more effective than UV/Sulfite at degrading aromatic and fluorescent compounds. All pre-treatments significantly reduced total organic chlorine and known DBPs versus direct chlorination, with UV/Sulfite achieving the highest reduction (80.42% and 60.98%). Unknown DBP molecules decreased by 31.54–53.04% (UV < UV/Sulfite < UV/PS < UV/H 2 O 2 ). Specifically, UV/PS and UV/H 2 O 2 preferentially controlled CHOSCl and CHONCl compounds, and 1Cl-DBPs, whereas UV/Sulfite excelled at reducing multi-chlorinated DBPs. Additionally, all pre-treatments reduced the calculated cytotoxicity of known DBPs by 49.89–81.25%, most notably for UV/Sulfite. These findings demonstrate the effectiveness of UV-AOPs/ARPs for comprehensive DBP control and provide practical guidance for selecting an optimal pre-treatment strategy based on target DBP profiles in wastewater applications.
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产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）