Ten series of aromatic hydrocarbon compounds (biphenyl, naphthalene, phenanthrene, anthracene, retene, chrysene, benzoanthracene, dibenzofuran, fluorene, dibenzothiophene) isolated from seven Triassic and Jurassic lac...Ten series of aromatic hydrocarbon compounds (biphenyl, naphthalene, phenanthrene, anthracene, retene, chrysene, benzoanthracene, dibenzofuran, fluorene, dibenzothiophene) isolated from seven Triassic and Jurassic lacustrine mudstone samples and three swamp coal samples, as well as five crude oil samples collected in the Kuche depression of the Tarim Basin, NW China, have been analysed by GC-MS techniques. It is found that the relative abundances of dibenzofuran series are higher in the three swamp coal samples than those in the lacustrine mudstone samples. Based on the similar relative abundances of dibenzofuran series, especially dibenzofuran compound, in the TICs of aromatic hydrocarbons, crude oils from wells SA3 (K), YTK5 (E, K) and QL1 (E) are thought to have been derived predominantly from the coals of the Lower Jurassic Yangxia Formation or Middle Jurassic Kezilenuer Formation, whereas those from wells YM7 (O) and YH1 (E) were derived mainly from Triassic and Jurassic lacustrine mudstones in the Kuche depression. This is the first report about how to distinguish coal-generated oils from lacustrine mudstone-generated oils in the Kuche depression in terms of the dibenzofuran series. The present paper has enlightening and directive significance for further oil-source rock correlations and oil and/or gas exploration in the Kuche depression of the Tarim Basin.展开更多
The adsorption of dibenzofuran on three commercial granular activated carbons (ACs) was investigated by dynamic experiment to correlate the adsorption equilibrium and kinetics with the structure of activated carbons.P...The adsorption of dibenzofuran on three commercial granular activated carbons (ACs) was investigated by dynamic experiment to correlate the adsorption equilibrium and kinetics with the structure of activated carbons.Physical properties including surface area, average pore diameter, micropore area and micropore volume of the activated carbons were characterized by N2 adsorption experiment on ASAP2010. To calculate the adsorption parameters, adsorption isotherm data were fitted to the Langmuir equation, and adsorption kinetic data were fitted to the linear driving force (LDF) diffusion model. From the correlation results, it is concluded that the adsorption equilibrium and diffusion coefficient of dibenzofuran on activated carbon are controlled respectively by the total adsorbent surface area and the adsorbent pore diameter.展开更多
The quantitative structure activity relationship(QSAR) of 32 polychlorinated dibenzo-p-furans toxicity is set up with some quantum-chemical parameters calculated by HyperChem7.0 and self-designed structure descriptor ...The quantitative structure activity relationship(QSAR) of 32 polychlorinated dibenzo-p-furans toxicity is set up with some quantum-chemical parameters calculated by HyperChem7.0 and self-designed structure descriptor codes.The quantum-chemical parameters(Ehomo,Ehomo1,Elumo,logP),the structure descriptor codes(R1,R9) are selected by stepwise regression.The predicting model has a correlation coefficient(R) of 0.9451 and standard error(s) of 0.5172.The performance of the QSAR equation is tested by leave-one-out procedure(LOO),and the correlation coefficient R and standard error(s) are 0.9381 and 0.5448 respectively.It shows that the QSAR model has good stability and predictability.The study indicates that the quantum-chemical parameters(Ehomo,Ehomo1,Elumo,logP) are important factors that can influence the compound toxicity.The toxicity of the compound would reduce when R1and R9 exist.展开更多
Phosphorus-containing compounds are considered as the potential alternatives of traditional inhibitors for suppressing the formation of polychlorinated dibenzo-p-dioxins and dibenzofurans(PCDD/Fs),but the suppression ...Phosphorus-containing compounds are considered as the potential alternatives of traditional inhibitors for suppressing the formation of polychlorinated dibenzo-p-dioxins and dibenzofurans(PCDD/Fs),but the suppression characteristics are scarcely studied.In this study,ammonium dihydrogen phosphate(ADP)was selected as the inhibitor to inhibit the PCDD/F formation via de novo synthesis at 350℃.The influence of oxygen content and addition method on PCDD/F inhibition was systematically investigated by means of statistical analysis and morphological characterization.The results showed that oxygen enhanced the formation of PCDD/Fs from 1470 ng g^(−1)(9.78 ng I-TEQ g^(−1))to 2110 ng g^(−1)(14.8 ng I-TEQ g^(−1)).ADP significantly inhibited the PCDD/F formation,with inhibition efficiencies ranging from 82.0%to 97.7%.Herein,a higher oxygen content and the premixed way intensified the suppression effect.Dibenzo-p-dioxin(DD)/dibenzofuran(DF)chlorination was proven to be effectively suppressed while chlorophenol(CP)route was not obviously influenced.With the addition of ADP,Cl source was significantly reduced and the formation of organic Cl was effectively inhibited.Also,it decreased the proportion of C–O/C=N and C=O,revealing the efficient inhibition of carbon oxidation.Meanwhile,the formation of copper phosphate and copper pyrophosphate was observed in XPS(X-ray photoelectron spectroscopy)spectra,indicating that the catalytic metal Cu was chelated and passivated by ADP.The premixed way had a better effect on reducing Cl resources,inhibiting oxidation and chelating metals,due to the direct contact with inhibitor.However,the separation method could only depend on the decomposed gases,resulting in a lower inhibition efficiency.展开更多
The thermodynamic properties of dibenzofurans （DFs）, xanthones （XTs） and an-thraquinones （AQs） with one and two positions substituted with hydroxyls in the ideal gas state at 298.15 K and 1.013×10^5 pa were...The thermodynamic properties of dibenzofurans （DFs）, xanthones （XTs） and an-thraquinones （AQs） with one and two positions substituted with hydroxyls in the ideal gas state at 298.15 K and 1.013×10^5 pa were calculated at the B3LYP/6-311G^＊ level using Gaussian 03 program. The isodesmic reactions were designed to calculate the standard free energy of formation （△fG^θ）. Three types of hydrogen bonds exist in the three kinds of chemicals and their bond energies were ascertained as 7-15, 15-23 and 49-58 kJ·mo1^-1 respectively by comparing the △fG^θ values. Electronic density topology analysis was applied to validate the strength of bond.展开更多
文摘Ten series of aromatic hydrocarbon compounds (biphenyl, naphthalene, phenanthrene, anthracene, retene, chrysene, benzoanthracene, dibenzofuran, fluorene, dibenzothiophene) isolated from seven Triassic and Jurassic lacustrine mudstone samples and three swamp coal samples, as well as five crude oil samples collected in the Kuche depression of the Tarim Basin, NW China, have been analysed by GC-MS techniques. It is found that the relative abundances of dibenzofuran series are higher in the three swamp coal samples than those in the lacustrine mudstone samples. Based on the similar relative abundances of dibenzofuran series, especially dibenzofuran compound, in the TICs of aromatic hydrocarbons, crude oils from wells SA3 (K), YTK5 (E, K) and QL1 (E) are thought to have been derived predominantly from the coals of the Lower Jurassic Yangxia Formation or Middle Jurassic Kezilenuer Formation, whereas those from wells YM7 (O) and YH1 (E) were derived mainly from Triassic and Jurassic lacustrine mudstones in the Kuche depression. This is the first report about how to distinguish coal-generated oils from lacustrine mudstone-generated oils in the Kuche depression in terms of the dibenzofuran series. The present paper has enlightening and directive significance for further oil-source rock correlations and oil and/or gas exploration in the Kuche depression of the Tarim Basin.
文摘The adsorption of dibenzofuran on three commercial granular activated carbons (ACs) was investigated by dynamic experiment to correlate the adsorption equilibrium and kinetics with the structure of activated carbons.Physical properties including surface area, average pore diameter, micropore area and micropore volume of the activated carbons were characterized by N2 adsorption experiment on ASAP2010. To calculate the adsorption parameters, adsorption isotherm data were fitted to the Langmuir equation, and adsorption kinetic data were fitted to the linear driving force (LDF) diffusion model. From the correlation results, it is concluded that the adsorption equilibrium and diffusion coefficient of dibenzofuran on activated carbon are controlled respectively by the total adsorbent surface area and the adsorbent pore diameter.
文摘The quantitative structure activity relationship(QSAR) of 32 polychlorinated dibenzo-p-furans toxicity is set up with some quantum-chemical parameters calculated by HyperChem7.0 and self-designed structure descriptor codes.The quantum-chemical parameters(Ehomo,Ehomo1,Elumo,logP),the structure descriptor codes(R1,R9) are selected by stepwise regression.The predicting model has a correlation coefficient(R) of 0.9451 and standard error(s) of 0.5172.The performance of the QSAR equation is tested by leave-one-out procedure(LOO),and the correlation coefficient R and standard error(s) are 0.9381 and 0.5448 respectively.It shows that the QSAR model has good stability and predictability.The study indicates that the quantum-chemical parameters(Ehomo,Ehomo1,Elumo,logP) are important factors that can influence the compound toxicity.The toxicity of the compound would reduce when R1and R9 exist.
基金supported by the Fundamental Research Funds for the Central Universities(No.K20220145).
文摘Phosphorus-containing compounds are considered as the potential alternatives of traditional inhibitors for suppressing the formation of polychlorinated dibenzo-p-dioxins and dibenzofurans(PCDD/Fs),but the suppression characteristics are scarcely studied.In this study,ammonium dihydrogen phosphate(ADP)was selected as the inhibitor to inhibit the PCDD/F formation via de novo synthesis at 350℃.The influence of oxygen content and addition method on PCDD/F inhibition was systematically investigated by means of statistical analysis and morphological characterization.The results showed that oxygen enhanced the formation of PCDD/Fs from 1470 ng g^(−1)(9.78 ng I-TEQ g^(−1))to 2110 ng g^(−1)(14.8 ng I-TEQ g^(−1)).ADP significantly inhibited the PCDD/F formation,with inhibition efficiencies ranging from 82.0%to 97.7%.Herein,a higher oxygen content and the premixed way intensified the suppression effect.Dibenzo-p-dioxin(DD)/dibenzofuran(DF)chlorination was proven to be effectively suppressed while chlorophenol(CP)route was not obviously influenced.With the addition of ADP,Cl source was significantly reduced and the formation of organic Cl was effectively inhibited.Also,it decreased the proportion of C–O/C=N and C=O,revealing the efficient inhibition of carbon oxidation.Meanwhile,the formation of copper phosphate and copper pyrophosphate was observed in XPS(X-ray photoelectron spectroscopy)spectra,indicating that the catalytic metal Cu was chelated and passivated by ADP.The premixed way had a better effect on reducing Cl resources,inhibiting oxidation and chelating metals,due to the direct contact with inhibitor.However,the separation method could only depend on the decomposed gases,resulting in a lower inhibition efficiency.
文摘The thermodynamic properties of dibenzofurans （DFs）, xanthones （XTs） and an-thraquinones （AQs） with one and two positions substituted with hydroxyls in the ideal gas state at 298.15 K and 1.013×10^5 pa were calculated at the B3LYP/6-311G^＊ level using Gaussian 03 program. The isodesmic reactions were designed to calculate the standard free energy of formation （△fG^θ）. Three types of hydrogen bonds exist in the three kinds of chemicals and their bond energies were ascertained as 7-15, 15-23 and 49-58 kJ·mo1^-1 respectively by comparing the △fG^θ values. Electronic density topology analysis was applied to validate the strength of bond.
