JOURNAL OF HAZARDOUS MATERIALS
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2020
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IF 9.038
Yunli Liu,Haiyang Hu,Giulio Zanaroli,Ping Xu,Hongzhi Tang
Polycyclic aromatic hydrocarbons (PAHs) and heterocyclic derivatives are organic pollutants that pose a serious health risk to human beings. In this study, a newly isolated Pseudomonas brassicacearum strain MPDS could effectively degrade PAHs and heterocyclic derivatives, including naphthalene , fluorene, dibenzofuran (DBF) and dibenzothiophene (DBT). Notably, strain MPDS is able to degrade fluorene, DBF and DBT uniquely via a lateral dioxygenation pathway, while most reported strains degrade fluorene, DBF and DBT via an angular dioxygenation pathway or co-metabolize them via a lateral dioxygenation pathway. Strain MPDS completely degraded 50 mg naphthalene (in 50 mL medium) in 84 h, and OD 600 reached 1.0–1.1; while, it stabilized at OD 600 0.5–0.6 with 5 mg fluorene or DBF or DBT. Meanwhile, 65.7% DBF and 32.1% DBT were degraded in 96 h, and 40.3% fluorene was degraded in 72 h, respectively. Through genomic and transcriptomic analyses, and comparative genomic analysis with another DBF degradation strain, relevant gene clusters were predicted, and a naphthalene-degrading gene cluster was identified. This study provides understanding of degradation of PAHs and their heterocyclic derivatives, as well as new insights into the lateral dioxygenation pathway of relevant contaminants.
研究领域:
环境微生物学
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生物修复
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基因组学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Hongyang Lv,Fengyu Tian,Xingxing Cui,Zhenkun Chen,Guangzheng Sun,Yuan Pan,Yichuan Li,Bin Dong,Bin Liu,Yongming Chai,Chenguang Liu
With the trend of heavy and inferior crude oil, the design of hydrodesulfurization (HDS) catalysts with excellent activity and high active metal utilization is an inevitable trend for the upgrading of refining technology. In this study, a highly dispersed Mo catalyst confined within nitrogen-doped porous carbon (xMo@NC) was prepared using an in situ encapsulation-pyrolysis approach and used in the HDS reaction of dibenzothiophene (DBT). The methods of XRD, HRTEM, HAADF-STEM, N 2 physisorption, FT-IR, Raman, and XPS were used to carry out thorough microstructural characterization. The results demonstrated that the Mo species in xMo@NC were highly dispersed, exhibiting superior intrinsic HDS activity compared to MoS 2 /NC* catalysts and conventional supported catalyst MoS 2 /Al 2 O 3 . The xMo@NC catalyst exhibited significant direct desulfurization (DDS) pathway in the HDS reaction of DBT. Differential charge density and bader charge suggested that significant electron transfer between the sulfur atom of DBT and the Mo species of xMo@NC, which weakened the C S bond and made it easier to remove sulfur via DDS pathway during the HDS reaction. This work presents a new catalytic material with high intrinsic activity and enhanced DDS desulfurization selectivity, providing fresh perspectives on the creation of high-performance HDS catalysts.
研究领域:
催化化学
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化学工程
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材料科学
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石油炼制
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表面化学
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2023
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IF 15.1
Hang Xu,Anqi Niu,Zihan Shang,Geng Li,Fengmin Wu,Xuefeng Wei,Jun Zhang
A heterogeneous catalyst was prepared by wrapping a poly 3-butyl vinylimidazole cobalt chloride ionic liquid (P[BVIM]CoCl 3 ) around the surface of Fe 3 O 4 @SiO 2 magnetic nanoballs. This catalyst was coupled with the oxidant peroxymonosulfate (PMS) for extraction catalytic oxidation desulfurization (ECODS). The prepared desulfurization catalyst had superparamagnetic properties, with a saturation magnetization of 32.5 emu/g. Moreover, this caalyst was multi-porous material, ans it had a specific surface area and pore volume of 8.14 m 2 /g and 0.018 cc/g, respectively. The average pore diameter of catalyst was 3.9 nm. The optimal experimental conditions were as follows: the initial sulfur content of the oil was 500 ppm, the catalyst dosage was 30 mg, PMS (20 wt%) dosage was 0.6 g, the ACN dosage was 2 g, and the oil sample size was 6 g. After 20 min, a sulfur removal rate of over 98 % was achieved at 20 °C. Furthermore, the unpurified catalyst still maintained high desulfurization activity after being used for 5 times, demonstrating good stability. The desulfurization mechanism was divided into two steps: first, DBT was oxidized to DBTO by SO 4 − free radicals, and second, the DBTO was further oxidized to DBTO 2 by OH free radicals in a tandem reaction. The reaction rates for the two steps at 20 °C were 0.0144 sec −1 and 0.00115 sec −1 , respectively. The activation energies associated with these steps were 65.65 kJ/mol and 105.22 kJ/mol, respectively. The quencher t-butanol had no effect on the first step but significantly inhibited the second step, meaning that DBTO became the main oxidation product. One potential application of this study is the utilization of t-butanol to regulate the oxygen content in organic sulfide oxidation products.
研究领域:
催化
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环境化学
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材料科学
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DOI
高影响因子
FUEL
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2022
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IF 8.035
Feng Li,Wending Zhou,Wanliang Yang,Meili Chen,Chun Wang,Rui Cao,Chengliang Zhou
The design and synthesis of hierarchical self-assembled 2D-channel silica (2D-CS) with mesoscopicshape control and developing of their application in catalysis has remained a challenge. Herein, we fabricated a series of 2D-CSx materials through the hierarchical self-assembly of curved lamellar micelles along with their derivative 2D channel catalysts (2D-CS x -NH 2 -HPW) by grafting amino groups and immobilizing phosphotungstic acid. These catalysts exhibit highly effective oxidative-adsorptive desulfurization (OADS) performance owing to their accessible open-transport channels. A novel theory that the stacking of curved lamellar micelles is similar to that of wrinkled-papers was proposed to explain the hierarchical self-assembly mechanism of the 2D-CS materials, which follows the “short-range order, long-range disorder” rule. Systematic characterizations and experiments indicated that the size and specific surface area of 2D-channel catalysts jointly determine their OADS performance. Most importantly, the 2D-channel catalysts show the highest removal efficiency of DBT when compared with 0D and 1D materials, which was ascribed to their facilitation of molecular diffusion owing to their accessible open-transport channels. The optimal 2D-channel catalysts (2D-CS 4 -NH 2 -HPW) exhibited excellent desulfurization performance despite omitting the extraction step, and the removal efficiency of DBT reached 99.72% in 5 min at 60 °C, much faster than previously reported mesoporous-catalyst-supported heteropoly acids. In addition, the OADS activity of typical sulfur compounds in the presence of the 2D-CS x -NH 2 -HPW catalyst was investigated, and the sulfur removal efficiency was found to decreases in the following order: DBT > 4,6-DMDBT > BT > n-DDM. The 2D-channel catalyst also exhibits excellent recyclability without significant loss of OADS activity after 10 cycles of reactions. This work provides a strategy for constructing 2D-channel catalysts for efficient desulfurization, demonstrating the potential of 2D-channel materials in catalytic applications.
研究领域:
材料科学
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催化
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化学工程
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
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