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strong> PYR-1 endowed with an enhanced activity of dihydroxylation of high-molecular-weight polyaromatic hydrocarbons

Yiquan Wu, Ying Xu, Ningyi Zhou

《环境科学与工程前沿（英文）》 2020年 第14卷 第1期 doi: 10.1007/s11783-019-1193-5

摘要： • Mycobacterium vanbaalenii PYR-1 utilizes PAHs at different rates. • Both NidA3B3 and FNidA3B3 catalyze high-molecular-weight PAHs dihydroxylation. • NidA3B3 shows an enhanced activity with an endogenous electron transport chain. • FNidA3B3 has an enhanced activity by 50% approximately compared with NidA3B3. • FNidA3B3/NidA3B3 and NidAB in the same strain come from different ancestors. NidA3B3 is a terminal dioxygenase whose favorable substrates are high-molecular-weight polyaromatic hydrocarbons (PAHs) from Mycobacterium vanbaalenii PYR-1, a powerful PAHs degradation strain. NidA3B3 was reported to incorporate a dioxygen into the benzene ring of PAHs when equipped with an exogenous electron transport chain components PhdCD from Nocardioides sp. strain KP7 by biotransformation, but this enzyme system was not particularly efficient. In this study, strain PYR-1 was confirmed to utilize four different PAHs at different growth rates. When PhtAcAd, an endogenous electron transport chain of a phthalate dioxygenase system, was substituted for PhdCD to couple with NidA3B3, the specific activity to convert phenanthrene by strain BL21(DE3) [pNidA3B3-PhAcAd] was 0.15±0.03 U/mg, but the specific activity of strain BL21(DE3) [pNidA3B3-PhdCD] was only 0.025±0.006 U/mg. In addition, FNidA3, encoded by a newly defined ORF, has a prolonged 19-amino acid sequence at the N-terminal compared with NidA3. FNidA3B3 increased the activity by 50% approximately than NidA3B3 when using PhtAcAd. Components of the electron transport chain PhtAc and PhtAd were purified and characterized. The Km, kcat, kcat/Km values of the PhtAd were 123±26.9 M, 503±49.9 min−1, 4.1 M−1·min−1, respectively. And the Km, kcat, kcat/Km values of the ferredoxin PhtAc were 52.5±9.7 M, 3.8±0.19 min−1 and 0.07 M−1·min−1, respectively. Basing on the phylogenetic analysis, NidA3/FNidA3 were far from its isoenzyme NidA from the same strain. Combining their primary differences of transcriptional pattern in vivo, it indicated that the functionally similar Rieske dioxygenases NidA3B3/FNidA3B3 and NidAB might originate from different ancestors.

关键词： Biodegradation     polyaromatic hydrocarbons     biotransformation     ring-hydroxylating dioxygenase system    

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Migration and fate of polycyclic aromatic hydrocarbons in bioretention systems with different media:

《环境科学与工程前沿（英文）》 2023年 第18卷 第4期 doi: 10.1007/s11783-024-1802-9

摘要：

● Bioretention systems showed > 92% load reduction rates of PAHs.

关键词： Bioretention     Polycyclic aromatic hydrocarbons     HYDRUS-1D     Model simulation     Migration    

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Enrichment and transfer of polycyclic aromatic hydrocarbons (PAHs) through dust aerosol generation from

《环境科学与工程前沿（英文）》 2023年 第17卷 第1期 doi: 10.1007/s11783-023-1610-7

摘要：

● Compositional patterns of PAHs in dust aerosol vary from soil during dust generation.

关键词： Dust aerosols     Enrichment factors (EFs)     Polycyclic aromatic hydrocarbons (PAHs)    

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Effect of ambient polycyclic aromatic hydrocarbons and nicotine on the structure of Aβ protein

《环境科学与工程前沿（英文）》 2023年 第17卷 第2期 doi: 10.1007/s11783-023-1615-2

摘要：

● B[a]P, nicotine and phenanthrene molecules altered the secondary structure of Aβ42.

关键词： Polycyclic aromatic hydrocarbons     Nicotine     toxicology     Aβ42 peptide     Alzheimer’s disease     Molecular dynamics simulations     Environmental pollution    

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Electrochemical reduction characteristics and the mechanism of chlorinated hydrocarbons at the copper

XU Wenying, GAO Tingyao, ZHOU Rongfeng, MA Lumin

《环境科学与工程前沿（英文）》 2007年 第1卷 第2期   页码 207-212 doi: 10.1007/s11783-007-0036-y

摘要： The electrochemical reduction characteristics of chlorinated hydrocarbons were investigated by cyclic voltammetry technique. The reduction mechanism and activity of the chlorinated hydrocarbons at the copper electrode were explored. The relationship between the structure of chlorinated hydrocarbons and their reductive activity were discussed. The experimental results showed that chlorinated alkanes and a portion of chlorinated aromatic hydrocarbons could be reduced directly at the copper electrode. However, chlorinated aromatic hydrocarbons were not easy to reduce at the copper electrode. The results provided a theoretical basis for the catalyzed iron inner electrolysis method.

关键词： electrolysis     chlorinated     relationship     mechanism     voltammetry technique    

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Transmembrane transport of polycyclic aromatic hydrocarbons by bacteria and functional regulation of

Hongqi Wang, Ruhan Jiang, Dekang Kong, Zili Liu, Xiaoxiong Wu, Jie Xu, Yi Li

《环境科学与工程前沿（英文）》 2020年 第14卷 第1期 doi: 10.1007/s11783-019-1188-2

摘要： Explaintheadsorption, uptake and transmembrane transport of PAHs by bacteria. Analyze functional regulation of membrane proteins inthe transmembrane transport. Proteomics technology such as iTRAQ labeling was used to access expressed proteins. Single cell analysis technology wereused to study the morphological structure. In recent years, increasing research has been conducted on transmembrane transport processes and the mechanisms behind the microbial breakdown of polycyclic aromatic hydrocarbons (PAHs), including the role of membrane proteins in transmembrane transport and the mode of transmission. This article explains the adsorption, uptake and transmembrane transport of PAHs by bacteria, the regulation of membrane protein function during the transmembrane transport. There are three different regulation mechanisms for uptake, depending on the state and size of the oil droplets relative to the size of the microbial cells, which are (i) direct adhesion, (ii) emulsification and pseudosolubilization, and (iii) interfacial uptake. Furthermore, two main transmembrane transport modes are introduced, which are (i) active transport and (ii) passive uptake and active efflux mechanism. Meanwhile, introduce the proteomics and single cell analysis technology used to address these areas of research, such as Isobaric tags for relative and absolute quantitation (iTRAQ) technology and Nano Secondary ion mass spectrometry (Nano-SIMS). Additionally, analyze the changes in morphology and structure and the characteristics of microbial cell membranes in the process of transmembrane transport. Finally, recognize the microscopic mechanism of PAHs biodegradation in terms of cell and membrane proteins are of great theoretical and practical significance for understanding the factors that influence the efficient degradation of PAHs contaminants in soil and for remediating the PAHs contamination in this area with biotechnology.

关键词： Polycyclic aromatic hydrocarbons     Transmembrane transport     Adsorption and uptake of hydrocarbons     Proteomics     Functional regulation of membrane protein     Single cell analysis technology    

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Progress in hydrogen enriched hydrocarbons combustion and engine applications

Zuohua HUANG, Jinhua WANG, Erjiang HU, Chenglong TANG, Yingjia ZHANG

《能源前沿（英文）》 2014年 第8卷 第1期   页码 73-80 doi: 10.1007/s11708-013-0287-1

摘要： The paper summarized the work on hydrogen enriched hydrocarbons combustion and its application in engines. The progress and understanding on laminar burning velocity, flame instability, flame structure flame and chemical kinetics were presented. Based on fundamental combustion, both homogeneous spark-ignition engine and direct-injection spark-ignition engine fueled with natural gas-hydrogen blends were conducted and the technical route of natural gas-hydrogen combined with exhaust gas recirculation was proposed which experimentally demonstrated benefits on both thermal efficiency improvement and emissions reduction.

关键词： hydrogen enriched hydrocarbon combustion     fundamental study     engine application    

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High-precision standard enthalpy of formation for polycyclic aromatic hydrocarbons predicting from general

《化学科学与工程前沿（英文）》 2022年 第16卷 第12期   页码 1743-1750 doi: 10.1007/s11705-022-2184-9

摘要： The standard enthalpy of formation is an important predictor of the reaction heat of a chemical reaction. In this work, a high-precision method was developed to calculate accurate standard enthalpies of formation for polycyclic aromatic hydrocarbons based on the general connectivity based hierarchy (CBH) with the discrete correction of atomization energy. Through a comparison with available experimental findings and other high-precision computational results, it was found that the present method can give a good description of enthalpy of formation for polycyclic aromatic hydrocarbons. Since CBH schemes can broaden the scope of application, this method can be used to investigate the energetic properties of larger polycyclic aromatic hydrocarbons to achieve a high-precision calculation at the CCSD(T)/CBS level. In addition, the energetic properties of CBH fragments can be accurately calculated and integrated into a database for future use, which will increase computational efficiency. We hope this work can give new insights into the energetic properties of larger systems.

关键词： standard enthalpy of formation     polycyclic aromatic hydrocarbons     connectivity based hierarchy     high-precision calculation    

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Multiphase redistribution differences of polycyclic aromatic hydrocarbons (PAHs) between two successive

Rufeng LI,Chenghong FENG,Dongxin WANG,Baohua LI,Zhenyao SHEN

《环境科学与工程前沿（英文）》 2016年 第10卷 第2期   页码 381-389 doi: 10.1007/s11783-015-0817-7

摘要： Successive sediment suspensions often happen in estuary, yet little research has probed into the difference in the release behaviors of organic compounds among different suspensions. This study took polycyclic aromatic hydrocarbons (PAHs) as typical organic contaminants and investigated the release behaviors between two successive suspensions with a particle entrainment simulator (PES). Results showed that successive sediment suspensions lowered the concentration of dissolved PAHs in the overlying water via facilitating the re-adsorption of dissolved PAHs onto the suspended particles. Fast-release and slow-release periods of PAHs were successively observed in the both suspensions. The concentration changes of dissolved PAHs in the second suspension were generally similar with but hysteretic to those in the first suspension. More vigorous desorption and re-absorption of PAHs were induced in the second suspension. Successive sediment suspensions obviously decreased the concentrations of mineral composition and organic matters in the overlying water, which significantly affects multiphase distribution of PAHs.

关键词： sediment suspension     PAHs     multiphase distribution     distribution coefficients    

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Removal of high concentrations of polycyclic aromatic hydrocarbons from contaminated soil by biodiesel

Jinbao WU, Zongqiang GONG, Liyan ZHENG, Yanli YI, Jinghua JIN, Xiaojun LI, Peijun LI

《环境科学与工程前沿（英文）》 2010年 第4卷 第4期   页码 387-394 doi: 10.1007/s11783-010-0269-z

摘要： Solubilizing experiments were carried out to evaluate the ability of biodiesel to remove polycyclic aromatic hydrocarbons (PAHs) from highly contaminated manufactured gas plant (MGP) and PAHs spiked soils with hydroxypropyl-β-cyclodextrin (HPCD) and tween 80 as comparisons. Biodiesel displayed the highest solubilities of phenanthrene (420.7 mg·L ), pyrene (541.0 mg·L ), and benzo(a)pyrene (436.3 mg·L ). These corresponded to several fold increases relative to 10% HPCD and tween 80. Biodiesel showed a good efficiency for PAH removal from the spiked and MGP soils for both low molecular weight and high molecular weight PAHs at high concentrations. Biodiesel was the best agent for PAH removal from the spiked soils as compared with HPCD and tween 80; as over 77.9% of individual PAH were removed by biodiesel. Tween 80 also showed comparable capability with biodiesel for PAH solubilization at a concentration of 10% for the spiked soils. Biodiesel solubilized a wider range of PAHs as compared to HPCD and tween 80 for the MPG soils. At PAH concentrations of 229.6 and 996.9 mg·kg , biodiesel showed obvious advantage over the 10% HPCD and tween 80, because it removed higher than 80% of total PAH. In this study, a significant difference between PAH removals from the spiked and field MGP soils was observed; PAH removals from the MGP soil by HPCD and tween 80 were much lower than those from the spiked soil. These results demonstrate that the potential for utilizing biodiesel for remediation of highly PAH-contaminated soil has been established.

关键词： polycyclic aromatic hydrocarbons (PAHs)     biodiesel     soil     removal     solubilization    

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Measurement of activity coefficients at infinite dilution for hydrocarbons in imidazolium-based ionic

ZHU Jiqin, YU Yanmei, CHEN Jian, FEI Weiyang

《化学科学与工程前沿（英文）》 2007年 第1卷 第2期   页码 190-194 doi: 10.1007/s11705-007-0035-3

摘要： The separations of olefin/paraffin, aromatic/aliphatic hydrocarbons or olefin isomers using ionic liquids instead of volatile solvents have interested many researchers. Activity coefficients γ at infinite dilution of a solute in ionic liquid are generally used in the selection of solvents for extraction or extractive distillation. In fact, the measurement of γ by gas-liquid chromatography is a speedy and cost-saving method. Activity coefficients at infinite dilution of hydrocarbon solutes, such as alkanes, hexenes, alkylbenzenes, styrene, in 1-allyl-3-methylimidazolium tetrafluoroborate ([AMIM][BF]) and 1-butyl-3-methyl imidazolium hexafluorophosphate ([BMIM][PF6]), 1-isobutenyl-3-methylimidazolium tetrafluoroborate ([MPMIM][BF]) and [MPMIM][BF]-AgBF have been determined by gas-liquid chromatography using ionic liquids as stationary phase. The measurements were carried out at different temperatures from 298 to 318 K. The separating effects of these ionic liquids for alkanes/hexane, aliphatic hydrocarbons/benzene and hexene isomers have been discussed. The hydrophobic parameter, dipole element, frontier molecular orbital energy gap and hydration energy of these hydrocarbons were calculated with the PM3 semi-empirical quantum chemistry method. The quantitative relations among the computed structure parameters and activity coefficients at infinite dilution were also developed. The experimental activity coefficient data are consistent with the correlated and predicted results using QSPR models.

关键词： cost-saving     consistent     coefficient     measurement     separating    

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Efficient hydrothermal deoxygenation of methyl palmitate to diesel-like hydrocarbons on carbon encapsulated

《化学科学与工程前沿（英文）》 2023年 第17卷 第2期   页码 139-155 doi: 10.1007/s11705-022-2217-4

摘要： Porous carbon-encapsulated Ni and Ni–Sn intermetallic compound catalysts were prepared by the one-pot extended Stöber method followed by carbonization and tested for in-situ hydrothermal deoxygenation of methyl palmitate with methanol as the hydrogen donor. During the catalyst preparation, Sn doping reduces the size of carbon spheres, and the formation of Ni–Sn intermetallic compounds restrain the graphitization, contributing to larger pore volume and pore diameter. Consequently, a more facile mass transfer occurs in carbon-encapsulated Ni–Sn intermetallic compound catalysts than in carbon-encapsulated Ni catalysts. During the in-situ hydrothermal deoxygenation, the synergism between Ni and Sn favors palmitic acid hydrogenation to a highly reactive hexadecanal that easily either decarbonylate to n-pentadecane or is hydrogenated to hexadecanol. At high reaction temperature, hexadecanol undergoes dehydrogenation–decarbonylation, generating n-pentadecane. Also, the C–C bond hydrolysis and methanation are suppressed on Ni–Sn intermetallic compounds, favorable for increasing the carbon yield and reducing the H2 consumption. The n-pentadecane and n-hexadecane yields reached 88.1% and 92.8% on carbon-encapsulated Ni3Sn2 intermetallic compound at 330 °C. After washing and H2 reduction, the carbon-encapsulated Ni3Sn2 intermetallic compound remains stable during three recycling cycles. This is ascribed to the carbon confinement that effectively suppresses the sintering and loss of metal particles under harsh hydrothermal conditions.

关键词： extended Stöber method     carbon encapsulated Ni–Sn intermetallic compounds     confinement     in-situ hydrothermal deoxygenation     hydrogenation     decarbonylation    

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Fenton process for degradation of selected chlorinated aliphatic hydrocarbons exemplified by trichloroethylene

QIANG Zhimin, BEN Weiwei, HUANG Chin-Pao

《环境科学与工程前沿（英文）》 2008年 第2卷 第4期   页码 397-409 doi: 10.1007/s11783-008-0074-0

摘要： The degradation of selected chlorinated aliphatic hydrocarbons (CAHs) exemplified by trichloroethylene (TCE), 1,1-dichloroethylene (DCE), and chloroform (CF) was investigated with Fenton oxidation process. The results indicate that the degradation rate was primarily affected by the chemical structures of organic contaminants. Hydroxyl radicals (OH) preferred to attack the organic contaminants with an electron-rich structure such as chlorinated alkenes (i.e., TCE and DCE). The dosing mode of Fenton’s reagent, particularly of Fe, significantly affected the degradation efficiency of studied organic compound. A new “time-squared” kinetic model, = exp(-), was developed to express the degradation kinetics of selected CAHs. This model was applicable to TCE and DCE, but inapplicable to CF due to their varied reaction rate constants towards OH. Chloride release was monitored to examine the degree of dechlorination during the oxidation of selected CAHs. TCE was more easily dechlorinated than DCE and CF. Dichloroacetic acid (DCAA) was identified as the major reaction intermediate in the oxidation of TCE, which could be completely removed as the reaction proceeded. No reaction intermediates or byproducts were identified in the oxidation of DCE and CF. Based on the identified intermediate, the reaction mechanism of TCE with Fenton’s reagent was proposed.

关键词： identified     1     1-dichloroethylene     kinetic     Dichloroacetic     Chloride    

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Particle-bound polycyclic aromatic hydrocarbons in typical urban of Yunnan-Guizhou Plateau: Characterization

《环境科学与工程前沿（英文）》 2022年 第16卷 第9期 doi: 10.1007/s11783-022-1535-6

摘要：

• The sampling was conducted in city on the Yunnan-Guizhou Plateau for one year.

关键词： Particle-associated PAHs     Fine particle     Source appointment     Group analysis     Risk assessment     Biomass burning    

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Opportunities and challenges for a Golden Age of chemical engineering

Phillip R. WESTMORELAND

《化学科学与工程前沿（英文）》 2014年 第8卷 第1期   页码 1-7 doi: 10.1007/s11705-014-1416-z

摘要： Chemical engineering is entering a new Golden Age of practice, thought, and impact, accompanied by great new opportunities and challenges. Five aspects mark this development: a new abundance of hydrocarbons; the evolution of biology into a molecular science; the ubiquity of powerful computational tools; the trend in manufacturing to be more process-oriented; and the systems approach that is part of ChE education from its first stages. There are important technical challenges, including technology creation and environmental impact, but just as important are new appreciation for and attention to challenges that require societal dialogues about complexity, uncertainty, and evolving and sometimes contradictory requirements. Crucial to all these impacts is enhancing the identity of what the profession is. That must be based on recognizing that the core of chemical engineering is applying molecular sciences to create value and advance the quality of life.

关键词： hydrocarbons     biotechnology     computation     cyberinfrastructure     manufacturing     environmental    

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标题 作者 时间 类型 操作

strong> PYR-1 endowed with an enhanced activity of dihydroxylation of high-molecular-weight polyaromatic hydrocarbons

Yiquan Wu, Ying Xu, Ningyi Zhou

期刊论文

Migration and fate of polycyclic aromatic hydrocarbons in bioretention systems with different media:

期刊论文

Enrichment and transfer of polycyclic aromatic hydrocarbons (PAHs) through dust aerosol generation from

期刊论文

Effect of ambient polycyclic aromatic hydrocarbons and nicotine on the structure of Aβ protein

期刊论文

Electrochemical reduction characteristics and the mechanism of chlorinated hydrocarbons at the copper

XU Wenying, GAO Tingyao, ZHOU Rongfeng, MA Lumin

期刊论文

Transmembrane transport of polycyclic aromatic hydrocarbons by bacteria and functional regulation of

Hongqi Wang, Ruhan Jiang, Dekang Kong, Zili Liu, Xiaoxiong Wu, Jie Xu, Yi Li

期刊论文

Progress in hydrogen enriched hydrocarbons combustion and engine applications

Zuohua HUANG, Jinhua WANG, Erjiang HU, Chenglong TANG, Yingjia ZHANG

期刊论文

High-precision standard enthalpy of formation for polycyclic aromatic hydrocarbons predicting from general

期刊论文

Multiphase redistribution differences of polycyclic aromatic hydrocarbons (PAHs) between two successive

Rufeng LI,Chenghong FENG,Dongxin WANG,Baohua LI,Zhenyao SHEN

期刊论文

Removal of high concentrations of polycyclic aromatic hydrocarbons from contaminated soil by biodiesel

Jinbao WU, Zongqiang GONG, Liyan ZHENG, Yanli YI, Jinghua JIN, Xiaojun LI, Peijun LI

期刊论文

Measurement of activity coefficients at infinite dilution for hydrocarbons in imidazolium-based ionic

ZHU Jiqin, YU Yanmei, CHEN Jian, FEI Weiyang

期刊论文

Efficient hydrothermal deoxygenation of methyl palmitate to diesel-like hydrocarbons on carbon encapsulated

期刊论文

Fenton process for degradation of selected chlorinated aliphatic hydrocarbons exemplified by trichloroethylene

QIANG Zhimin, BEN Weiwei, HUANG Chin-Pao

期刊论文

Particle-bound polycyclic aromatic hydrocarbons in typical urban of Yunnan-Guizhou Plateau: Characterization

期刊论文

Opportunities and challenges for a Golden Age of chemical engineering

Phillip R. WESTMORELAND

期刊论文