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Few-layered hexagonal boron nitride nanosheets stabilized Pt NPs for oxidation promoted adsorptive desulfurization of fuel oil

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Green Energy & Environment 2024年第3期9卷 495-506页

作者： Peiwen Wu Xin Song Linlin Chen Lianwen He Yingcheng Wu Duanjian Tao Jing He Chang Deng Linjie Lu Yanhong Chao Mingqing Hua Wenshuai Zhu School of Chemistry and Chemical Engineering Jiangsu UniversityZhenjiang212013China College of Chemical Engineering and Environment State Key Laboratory of Heavy Oil ProcessingChina University of Petroleum-BeijingBeijing102249China College of Chemistry and Chemical Engineering Jiangxi Normal UniversityNanchang330022China College of Science State Key Laboratory of Heavy Oil ProcessingChina University of Petroleum-BeijingBeijing102249China

A few-layered hexagonal boron nitride nanosheets stabilized platinum nanoparticles(Pt/h-BNNS)is engineered for oxidation-promoted adsorptive desulfurization(OPADS)of fuel oil.It was found that the few-layered structure and the defective sites of h-BNNS not only are beneficial to the stabilization of Pt NPs but also favor the adsorption of aromatic sulfides.By employing Pt/h-BNNS with a Pt loading amount of 1.19 wt%as the active adsorbent and air as an oxidant,a 98.0%sulfur removal over dibenzothiophene(DBT)is achieved along with a total conversion of the DBT to the corresponding sulfones(DBTO_(2)).Detailed experiments show that the excellent desulfurization activity originates from the few-layered structure of h-BNNS and the high catalytic activity of Pt NPs.In addition,the OPADS system with Pt/h-BNNS as the active adsorbent shows remarkable stability in desulfurization performance with the existence of different interferents such as olefin,and aromatic hydrocarbons.Besides,the Pt/h-BNNS can be recycled 12 times without a significant decrease in desulfurization performance.Also,a process flow diagram is proposed for deep desulfurization of fuel oil and recovery of high value-added products,which would promote the industrial application of such OPADS strategy.

关键词： Desulfurization Adsorption Catalytic oxidation Active adsorbent dibenzothiophene

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MoO_(x) nanoclusters on Mo-doped TiO_(2) nanosheets with enhanced singlet oxygen generation and sulfide conversion abilities for photocatalytic aerobic oxidative desulfurization

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Science China Chemistry 2024年第1期67卷 408-414页

作者： Suting Xie Xinyu Zhao Dongxiao Wang Huawei Yang Lixia Yang Liangjiu Bai Donglei Wei Wenxiang Wang Ying Liang Hou Chen Shaojun Guo College of Chemistry and Materials Science Ludong UniversityYantai 264025China College of Materials Science and Engineering Peking UniversityBeijing 100871China

Photocatalytic aerobic oxidation desulfurization(PAODS)is a promising and sustainable alternative to conventional,energyintensive desulfurization techniques for petroleum products.However,its development is greatly plagued by the low capability in generating highly reactive oxygen species and sluggish kinetics of sulfide oxidation of reported photocatalysts.Here we report a class of MoO_(x)nanocluster decorated on ultrathin Mo-doped TiO_(2)nanosheet(MoO_(x)/MoTiO)catalyst for efficiently facilitating the photocatalytic aerobic oxidation of sulfides.We demonstrate that MoO_(x)/MoTiO can not only promote the generation of highly reactive singlet oxygen(^(1)O_(2))but also enhance the aerobic conversion of sulfides,which leads to a record dibenzothiophene oxidation activity of 3.90 mmol g^(-1)h^(-1).The multiple experimental characterizations and density functional theory calculations collectively reveal that the doped-Mo sites can interact with the photogenerated excitons,enabling directly energy transfer generation of^(1)O_(2)through a new exciton modulation mechanism,and the coordination unsaturated MoO_(x)clusters play the role of co-catalyst to enhance the separation of charge carriers,and effectively catalyze the reaction between sulfides and1O_(2)to form sulfones.

关键词： titanium dioxide photocatalytic aerobic oxidation desulfurization dibenzothiophene singlet oxygen

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A universal polymer-assisted route to fabricate Zr-doped TiO2 nanocomposite: boosting reactive desulfurization

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Tungsten 2024年第3期6卷 596-609页

作者： Yue Du Ping Li Zhi-Yi Zhong Wen-Xue Chen Yi-Si Liu Yun-Long Xie Li-Na Zhou Kai Wang Hubei Key Laboratory of Photoelectric Materials and Devices College of Material Science and Engineering Hubei Normal University National Laboratory of Solid State Microstructures Nanjing University College of Urban and Environmental Sciences Huangshi Key Laboratory of Prevention and Control of Soil Pollution Hubei Normal University School of Chemistry Chemical Engineering and Biotechnology Nanyang Technological University

A series of transition metal ion-doped TiO2composites were prepared by polyethyleneimine-assisted solvent-free selfassembly.Due to the similar electronegativity and ionic radius of Ti and Zr ions,the introduction of Zr element to TiO2can effectively improve its surface acidity and introduce more defect sites on the TiO2framework.As-fabricated Zr-doped TiO2nanocomposite exhibits the formation of Zr-Ti bond,strong surface acidity,connected mesoporous channels,and relatively high crystallinity.These remarkable properties contribute to its adsorption-oxidation-desulfurization capacity toward thiophene-type sulfides,which can remove 500 ×10-6dibenzothiophene from the model fuel within 100 min at low reaction temperatures.The polymer-induced self-assembly method can reduce organic solvent usage,pollutant emissions,and energy consumption,which provides an efficient and practical way to prepare porous metal oxide-based catalysts in future.

关键词： Oxidative desulfurization Transition metal ion-doped TiO 2 nanocomposite dibenzothiophene Solvent-free self-assembly method

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Effects of nicotinamide and riboflavin on the biodesulfurization activity of dibenzothiophene by Rhodococcus erythropolis USTB-03

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Journal of Environmental Sciences 2008年第5期20卷 613-618页

作者： YAN Hai SUN Xudong XU Qianqian MA Zhao XIAO Chengbin Ning Jun Department of Biological Science and Technology School of Applied Science University of Science and Technology Beijing Beijing 100083 China Research Center for Eco-environmental Science Chinese Academy of Sciences Beijing 100085 China

Rhodococcus erythropolis USTB-03 is a promising bacterial strain for the biodesulfurization of dibenzothiophene （DBT） via a sulfurspecific pathway in which DBT is converted to 2-hydroxybiphenyl （2HBP） as an end product. The effects of nicotinamide and riboflavin on the sulfur specific activity （SA） of DBT biodesulfurization by R. erythropolis USTB-03 were investigated. Both nicotinamide and riboflavin were found to enhance the expression of SA, which was not previously reported. When R. erythropolis USTB-03 was grown on a medium containing nicotinamide of 10.0 mmol or riboflavin of 50.0 μmol, SA was raised from 68.0 or so to more than 130 mmol 2HBP/（kg dry cells.h）. When R. erythropolis USTB-03 was grown in the presence of both nicotinamide of 5.0 mmol and riboflavin of 25.0 μmol, SA was further increased to 159.0 mmol 2HBP/（kg dry cells.h）. It is suggested that the biological synthesis of reduced form of flavin mononucleotide （FMNH2）, an essential coenzyme for the activities of biodesulfurization enzyme Dsz C and A, might be enhanced by nicotinamide and riboflavin, which was responsible for the increased SA of R. erythropolis USTB-03.

关键词： biodesulfurization dibenzothiophene nicotinamide Rhodococcus erythropolis USTB-03 riboflavin

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N-butyl-pyridinium tetrafluoroborate as a highly efficient ionic liquid for removal of dibenzothiophene from organic solutions

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燃料化学学报 2015年第2期43卷 195-201页

作者： Maedeh Enayati Hossein Faghihian Department of Chemistry Shahreza BranchIslamic Azad University

In this research,1-butyl-pyridinium tetrafluoroborate([C4Py][BF4]-)was prepared by ion exchange method and was characterized by1H-NM R,13C-NM R,and FT-IR techniques.The synthesized ionic liquid w as used for removal of dibenzothiophene as a typical organosulfur pollutant from organic medium.The effect of different parameters on the extraction efficiency w as studied and optimized.At the optimized conditions,97.68%of dibenzothiophene w as extracted from 1 000 mg/L n-hexane solution.The extraction efficiency obtained in this w ork w as higher than the previous reported values.The desulfurization reaction w as kinetically follow ed the second order mechanism.The ionic liquid w as reusable and after four regeneration cycles 97%of its original extraction efficiency w as retained.

关键词：抽取 desulfurization 离子的液体 dibenzothiophene

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Desulfurization of dibenzothiophene by a newly isolated Corynebacterium sp. ZD-1 in aqueous phase

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Journal of Environmental Sciences 2004年第6期16卷 1011-1015页

作者： WANGMiao-dong LIWei WANGDa-hui SHIYao DepartmentofEnvironmentalEngineering ZhejiangUniversityHangzhou310027China

Sulfur emission through fuel combustion is a global problem because it is a major cause of acid rain. Crud oil contains many heterocyclic organic sulfur compounds, among which dibenzothiophene(DBT) and DBTs bearing alkyl substitutions usually are representative compounds. A strain was isolated from refinery sludge and identified as Corynebacterium ZD-1. The behavior of DBT degradation by ZD-1 in aqueous phase was investigated. Corynebacterium ZD-1 could metabolize DBT to 2-hydroxybiphenyl(2-HBP) as the dead-end metabolite through a sulfur-specific pathway. In shake flask culture, ZD-1 had its maximal desulfurization activity in the late exponential growth phase and the specific production rate of 2-HBP was about 0.14(mmol·kg dry cell -1·min -1, mmol·KDC -1·min -1). Active resting cells for desulfurization should be prepared only in this period. 2-HBP inhibited the growth of strain ZD-1, the production of DBT degradation enzymes, and the activity of enzymes. Sulfate inhibited the production of dibenzothiophene(DBT) degradation enzymes but had no effect on the enzymes' activity. The production rates of 2-HBP at lower cell densities were higher and the maximum amount conversion of DBT to 2-HBP(0.067 mmol/L) after 8 h was gained at 9.2 g dry cell/L rather higher cell density. The results indicated that this newly isolated strain could be a promising biocatalyst for DBT desulfurization.

关键词： biodesulfurization dibenzothiophene Corynebacterium

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Amorphous TiO_2-supported Keggin-type ionic liquid catalyst catalytic oxidation of dibenzothiophene in diesel

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Petroleum Science 2018年第4期15卷 870-881页

作者： Zhendong Yu Donghui Wang Suhang Xun Minqiang He Ruliang Ma Wei Jiang Hongping Li Wenshuai Zhu Huaming Li School of Chemistry and Chemical Engineering Jiangsu University School of Environment and Safety Engineering Institute of Environmental Health and Ecological SecurityJiangsu University Institute for Energy Research Jiangsu University

Supported ionic liquid(IL) catalysts [Cmim]PMoO/Am TiO(amorphous TiO) were synthesized through a one-step method for extraction coupled catalytic oxidative desulfurization(ECODS) system. Characterizations such as FTIR, DRS,wide-angle XRD, Nadsorption–desorption and XPS were applied to analyze the morphology and Keggin structure of the catalysts. In ECODS with hydrogen peroxide as the oxidant, it was found that ILs with longer alkyl chains in the cationic moiety had a better effect on the removal of dibenzothiophene. The desulfurization could reach 100% under optimal conditions, and GC–MS analysis was employed to detect the oxidized product after the reaction. Factors affecting the desulfurization efficiencies were discussed, and a possible mechanism was proposed. In addition, cyclic experiments were also conducted to investigate the recyclability of the supported catalyst. The catalytic activity of [Cmim]PMoO/Am TiOonly dropped from 100% to 92.9% after ten cycles, demonstrating the good recycling performance of the catalyst and its potential industrial application.

关键词： Supported ionic liquid catalyst Polyoxometallate Oxidative desulfurization Amorphous TiO_2 dibenzothiophene

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End-capped Thiophene Modulated Molecular Packing in 2,8-dibenzothiophene-based Materials:from Face-to-face to Edge-to-face Stacking

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Chinese Journal of Structural Chemistry 2012年第1期31卷 45-50页

作者：李业新陈志 School of Chemistry and Chemical Engineering University of Jinan 250022China

Two new organic crystals of 2,8-bisthienyldibenzothiophene（BTDT） and 2,8-bis-dithienyldibenzothiophene（BDTDT） compounds were successfully obtained.The change of end-capped group from thiophene to dithiophene causes big differences in molecular packing and carrier-transport property.The adjacent molecules of compound BTDT adopt face-to-face π stacking and exhibit two-dimensional interchain interactions.On the contrary,BDTDT molecules are arranged in an edge-to-face motif and show mainly one-dimensional interacting character.The packing mode exerts dramatic effect on the carrier-transport property.The crystal of BTDT belongs to the orthorhombic system,space group P21212 with a = 20.1427（11）,b = 4.6016（3）,c = 8.6340（5） ,V = 800.27（8） 3,Z = 2,Dc = 1.446 g/cm3,F（000） = 360,S = 1.019,the final R = 0.0491 and wR = 0.0960 for 1605 reflections with I 2σ（I）.The crystal of BDTDT belongs to the orthorhombic system,space group P212121 with a = 7.2636（15）,b = 25.359（5）,c = 25.359 ？,V = 4670.9（14）？3,Z = 8,Dc = 1.458 g/cm3,F（000） = 2112,S = 0.880,the final R = 0.0597 and wR = 0.1318 for 8047 reflections with I 2σ（I）.

关键词： dibenzothiophene crystal structure molecular packing organic field-effect transistor

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Macroporous 3D carbon-nitrogen(CN)confined MoO_(x) catalyst for enhanced oxidative desulfurization of dibenzothiophene

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Chinese Chemical Letters 2020年第10期31卷 2819-2824页

作者： Jinmei Ye Jie Wen Dongdong Zhao Peilun Zhang Airong Li Lianhong Zhang Hui Zhang Mengqi Wu Center for Computational Chemistry and Molecular Simulation College of Chemistry and Chemical EngineeringSouthwest Petroleum UniversityChengdu 610500China Department of Chemical and Biological Engineering Case Western Reserve UniversityClevelandOH 44120United States

Macroporous 3D carbon doped with nitrogen confined Mo catalyst(MoO_(x)@CN)had been prepared by a facile one-step pyrolysis technique using silica as a template and was employed for oxidative desulfurization(ODS)of dibenzothiophene(DBT)in model fuel with H2O_(2) as oxidant.The effect of different ope rating conditions(i.e.,reaction te mperature and time,catalyst dosage,H2O_(2)/DBT(O/S)molar ratio)were also systematic investigated.Under the optimal reaction condition,MoO_(x)@CN catalyst exhibited highly excellent ODS performance toward DBT,the highest sulfur removal efficiency can be up to 99.9%and sulfur content was wiped out from 800 ppm to 10 ppm.Due to the robust 3D structure promoting rapid transfer,in addition to the increased number of active sites induced by the Mo vacancies,the catalyst,prepared using chitosan and ammonium heptamolybdate in a mass ratio of 1:0.5,displayed rapid kinetics and low activation energy in the oxidation of dibenzothiophene.Moreover,it exhibited excellent recyclability after five cycles without any obvious decrease in catalytic activity for the oxidative desulfurization reaction.

关键词： O_(x)idation desulfurization Carbon-nitrogen confined MoO_(x) Mo vacancies dibenzothiophene Nanoparticles

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Sulfur-Selective Desulfurization of dibenzothiophene and Diesel Oil by Newly Isolated Rhodococcus erythropolis NCC-1

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Chinese Journal of Chemistry 2007年第3期25卷 400-405页

作者：李玉光马洁张倩倩王长水陈倩 Department of Chemistry Capital Normal University Beijing 100037 China Beijing Center for Disease Prevention and Control Beijing 100013 China

A dibenzothiophene （DBT）-desulfurizing bacteria strain was isolated from oil-contaminated soils and identified as Rhodococcus erythropolis NCC-1. Strain NCC-1 was found to convert DBT to hydroxybiphenyl （2-HBP） via the 4S pathway and also be able to use organic sulfur compounds other than DBT as a sole sulfur source. The strain could desulfurize 4,6-dimethyldibenzothiophene （4,6-DMDBT）, which is one of the most recalcitrant dibenzothiophene derivatives to hydrodesulfurization. When two type of oils, a model oil [n-hexadecane （n-C16） containing DBT] and a hydrodesulfurized diesel oil with various organic sulfur compounds, were treated with Rhodococcus erythropolis NCC-1 cells, the total sulfur content significantly decreased, from 150 to 20 mg/L for n-C16 and from 554 to 274 mg/L for diesel oil. The newly isolated strain NCC-1 is considered to have good potential for application in the biodesulfurization of fossil fuels.

关键词： biodesulfurization Rhodococcus erythropolis dibenzothiophene diesel oil

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