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Effect of Different Loadings on the Performance of Ni2P/Al2O3 Catalysts for Low-Temperature Thioethering and Selective Hydrogenation of Diolefins in Liquefied Petroleum gas

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China Petroleum processing & Petrochemical Technology 2023年第1期25卷 79-90页

作者： Xiao Han Sun Jinru Song Guoliang Xie Xianna Ke Ming Tong Yanbing Zhao Zhiping Wang Zijian Li Jiahan CNOOC CenerTech Tianjin Chemical Research and Design Institute Co LtdTianjin 300131China State Key Laboratory of Heavy Oil Processing and Beijing Key Lab of Oil&Gas Pollution Control China University of PetroleumBeijing 102249China

In this study,different loadings of x%Ni_(2)P/γ-Al_(2)O_(3)(x=6%,9%,12%,15%,18%)catalysts with aluminum oxide(Al_(2)O_(3))as the carrier,nickel chloride(NiCl2)as the nickel(Ni)source,and ammonium hypophosphite(NH_(4)H_(2)PO_(2))as the phosphorus(P)source were prepared by the equal volume impregnation method to investigate the effects of different loadings on the performance of the selective hydrogenation of diolefins and thiol etherification in *** physicochemical properties of the catalysts were characterized by XRD,BET,SEM,TEM,H_(2)-TPR,and XPS,and the catalytic activity of the catalysts was evaluated in a fixed-bed *** results showed that a change in the loading affected the catalyst crystalline phase structure and size,specific surface area,P coverage,active phase dispersion,and catalytic *** 6%,9%,and 12%loadings the catalysts had an Ni phase but there was no obvious Ni_(2)P phase in the nickel phosphide;at 15%loading a single Ni_(2)P phase was obtained,and at 18%loading both Ni_(2)P and Ni1_(2)P_(5) phases *** was a P enrichment on the catalyst surface,and the higher the loading the more P species were enriched on the surface,but some of the P was lost during the catalyst reduction process due to the production of phosphine(PH3)*** 15%Ni_(2)P/γ-Al_(2)O_(3) catalyst had the largest Ni/Al ratio and the best *** Ni_(2)P active phase size was small at about 4.25 nm and Ni_(2)P was uniformly dispersed on the catalyst surface without *** 15%Ni_(2)P/γ-Al_(2)O_(3) catalyst had the best catalytic activity at a pressure of 2.0 MPa,a liquid hourly space velocity(LHSV)of 3.0 h-1,and a hydrogen to hydrocarbon ratio of *** 1,3-butadiene conversion was 97.45%and the methanethiol removal was 100%at a temperature of 140℃.

关键词： Ni_(2)P dispersion low-temperature thioethering selective hydrogenation of diolefins

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Quantifying functional groups in the active layer of polyamide nanofiltration membranes via the dye adsorption method

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Frontiers of Materials Science 2024年第4期18卷 59-69页

作者： Li-ping Yue Fan-xin Kong Jin-fu Chen Ai-guo Zhou Guang-dong Sun State Key Laboratory of Heavy Oil Processing Beijing Key Laboratory of Oil&Gas Pollution ControlChina University of PetroleumBeijing 102249China Research Center for Urban&Rural Water Environmental Technology China Urban and Rural Holding Group Co.Ltd.Beijing 102249China

Ionized amine group(R-NH_(2))and carboxyl group(R-COOH)within the active layer of polyamide(PA)nanofiltration membranes result in the formation of positive(R-NH_(3)^(+))and negative(R-COO^(-))functional groups,respectively,which determines membrane performance and is essential for membrane fabrication and ***,a facile dye adsorption/desorption method using Orange II and Toluidine Blue O dyes was developed to measure the densities of R-NH2,R-,R-COOH,or R-COO^(-)on surfaces of six PA membranes,and the correlation between the density of such groups and the zeta potential was *** dye adsorption method was proven reliable due to its lower standard deviation,detection limit,and quantification limit ***,the densities of R-or R-COO^(-)under different pH values were measured,fitting well with results calculated from the acid-base equilibrium ***,a correlation was established between the net surface density([R-NH_(3)^(+)]-[R-COO^(-)])and the surface charge density(σ)calculated via the Gouy-Chapman model based on zeta potential *** resulted correlation(σ/(mC·m^(-2))=(3.67±0.08)×([R-NH_(3)^(+)]−[R-COO^(-)])/(nmol·cm^(-2))+(0.295±0.08))effectively predicts theσvalue of the *** study provides a facile and reliable dye adsorption method for measuring the density of R-NH2,R-NH_(3)^(+),R-COOH,or R-COO^(-),enabling an in-depth understanding of membrane charge properties.

关键词： carboxyl group amine group dye-adsorption method charge property

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Molecular transformation of dissolved organic matter in refinery wastewaters: Characterized by FT-ICR MS coupled with electrospray ionization and atmospheric pressure photoionization

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Petroleum Science 2023年第1期20卷 590-599页

作者： Chen He Wei-Ming Chen Chun-Mao Chen Quan Shi State Key Laboratory of Heavy Oil Processing Beijing Key Laboratory of Oil and Gas Pollution ControlChina University of PetroleumBeijing 102249China Faculty of Geosciences and Environmental Engineering Southwest Jiaotong UniversityChengduSichuan 611756China

Dissolved organic matter(DOM)in refinery wastewater is an extremely complex mixture of various organic *** mass spectrometry,it is impossible to characterize all of the DOM molecules with only one ionization *** this study,negative-ion,electrospray ionization(ESI),positive-ion ESI,and positive-ion atmospheric pressure photoionization(APPI)were coupled with Fourier transform ion cyclotron resonance mass spectrometry(FT-ICR MS)to analyze the molecular composition of DOM in a refinery wastewater stream during the treatment *** were obvious differences in the heteroatom composition,number of DOM constituents,and chemical properties in refinery wastewater under the three ionization *** CHO and CHOS compounds detected by(+)ESI,basic CHN and CHON compounds detected by(þ)ESI,and hydrocarbons detected by(+)APPI were analyzed to determine the molecular transformations that occurred during *** an anaerobic biological treatment process,acidic CHO and CHOS compounds with a high oxygen content were preferentially removed,and acidic CHO and CHOS compounds with a low oxygen content were *** an aerobic biological process,acidic CHO and CHOS compounds with a low oxygen content were preferentially removed,and acidic CHO and CHOS compounds with a high oxygen content were *** whole biological treatment process has a poor removal efficiency for CHN and CHON compounds,and *** activated carbon(AC)adsorption process removed different heteroatom compounds mainly with a low oxygen content for acidic and basic *** transformation mechanism of CHO and CHOS compounds in the biological treatment process was analyzed by the Kendrick mass defect(KMD)theory and a mass difference network *** the anaerobic process,large amounts of oxygenated CHO and CHOS compounds were degraded by decarboxylation,deoxydation,demethoxylation,and dehydration reactions,and converted to lower oxygen content *** the aerobic

关键词： Refinery wastewater DOM Molecular transformation ESI APPI FT-ICR MS

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Active phase morphology engineering of NiMo/Al2O3 through La introduction for boosting hydrodesulfurization of 4,6-DMDBT

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Petroleum Science 2023年第2期20卷 1231-1237页

作者： Ji-Xing Liu Xiang-Qi Liu Ri-Xin Yan Ling-Feng Ji Hui-Fang Cheng Hui Liu Yan Huang Ming-Qing Hua Hua-Ming Li Wen-Shuai Zhu School of Chemistry and Chemical Engineering and Institute for Energy Research Jiangsu UniversityZhenjiangJiangsu 212013China State Key Laboratory of Heavy Oil Processing and Beijing Key Lab of Oil&Gas Pollution Control China University of PetroleumBeijing 102249China State Key Laboratory of Fine Chemicals Dalian University of TechnologyDalianLiaoning 116024China

Herein,we designed and constructed a mesoporous LaAlOx via a solvent evaporation induced self-assembly *** structure and physicochemical property of the corresponding NiMo supported catalyst was analyzed by a set of characterizations,and its catalytic activity was investigated for hydrodesulfurization(HDS)of 4,*** has confirmed that the incorporation of La profoundly facilitate the generation of“Type II”NiMoS phase by weakening the interaction of Mo–O–Al leakage and promoting the sulfidation of both Ni and Mo oxides as well as changing the morphology of Ni promoted MoS2 slabs,thereafter boosting the HDS performance *** finding here may contribute to the fundamental understanding of structure-activity in ultra-deep desulfurization and inspire the advancement of highly-efficient HDS catalyst in future.

关键词： NiMo supported Catalyst LaAlOx composites Hydrodesulfurization Morphology Reaction kinetics

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The role and potential of attapulgite in catalytic pyrolysis of refinery waste activated sludge

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Petroleum Science 2022年第1期19卷 354-362页

作者： Qinghong Wang Kanghong Hao Chelsea Benally Yue Kou Zhexuan An Mohamed Gamal El-Din Chunmao Chen State Key Laboratory of Heavy Oil Processing Beijing Key Laboratory of Oil and Gas Pollution ControlChina University of Petroleum-BeijingBeijing102249China Department of Civil and Environmental Engineering University of AlbertaEdmontonAlbertaT6G 1H9Canada

Pyrolysis is a promising technology for the treatment of refinery waste activated sludge(rWAS).In this study,attapulgite as a natural clay was used to enhance the pyrolysis of *** yields,characteristics of pyrolytic products,pyrolytic kinetics and mechanisms were *** attapulgite improved the conversion of rWAS into non-condensable gases and pyrolytic *** bio-oil quality improved and the biochar yield *** average activation energy of Stage Ⅰ(230-400℃)and Stage Ⅱ(400-500℃)decreased by 36.5%and 49.7%,respectively,compared to rWAS ***_(2)O_(3)and Fe_(2)O_(3)in attapulgite enhanced the dealkylation reaction and cracking of C-C *** content of the gasoline(oil doubled relative to rWAS *** promoted the deoxygenation,dehydroxylation and dehydrogenation reactions of O-containing compounds,and the content of CO and CO_(2) in non-condensable gases *** of attapulgite(rWAS:attapulgite ratio of 1:1)decreased the O mobility from 14.6%to 12.8%relative to rWAS ***,the content of saturates in bio-oil increased from 38.5 wt%to 47.2 wt%and the lower heating value(LHV)increased from 6.8 kcal/kg to 8.4 kcal/*** heavy metals originally in rWAS were fixed into the pyrolytic residue and the environmental risks are *** study demonstrates the role and potential of attapulgite in catalytic pyrolysis of rWAS with an added advantage of increased cost-effectiveness.

关键词： Catalytic pyrolysis Attapulgite Kinetics Product characteristics

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Sorption and attenuation of petroleum VOCs in five unsaturated soils: Microcosms and column experiments

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Chemosphere 2024年 361卷 142551页

作者： Sun, Yue Cao, Jinhui Ma, Jie State Key Laboratory of Heavy Oil Processing Beijing Key Lab of Oil & Gas Pollution Control China University of Petroleum-Beijing Beijing102249 China

The fate of volatile organic compounds (VOC) vapors in the unsaturated zone is the basis for evaluating the natural attenuation potential and vapor intrusion risk. Microcosm and column experiments were conducted to study the effects chemical speciation and soil types/properties on the fate of petroleum VOCs in unsaturated zone. The biodegradation and total attenuation rates of the seven VOCs obtained by microcosm experiments in black soil and yellow earth were also generally higher than those in floodplain soil, lateritic red earth, and quartz sand. The VOC vapors in floodplain soil, lateritic red earth, and quartz sand showed slow total attenuation rates (−1). N-pentane, methylcyclopentane, and methylcyclohexane showed lower biodegradation rates than octane and three monoaromatic hydrocarbons. Volatilization into the atmosphere and biodegradation are two important natural attenuation paths for VOCs in unsaturated soil columns. The volatilization loss fractions of different volatile hydrocarbons in all five unsaturated soils were generally in the order: n-pentane (93.5%–97.8%) > methylcyclopentane (77.2%–85.5%) > methylcyclohexane (53.5%–69.2%) > benzene (17.1%–73.3%) > toluene (0–45.7%) > octane (1.9%–34.2%) > m-xylene (0–5.7%). The fractions by volatilization into the atmosphere of all seven hydrocarbons in quartz sand, lateritic red earth, and floodplain soil were close and higher compared to the yellow earth and black soil. Overall, this study illustrated the important roles chemical speciation and soil properties in determining the vapor-phase transport and natural attenuation of VOCs in the unsaturated zone. © 2024

关键词： Volatile organic compounds

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Simultaneous electrocoagulation and E-peroxone coupled with ultrafiltration membrane for shale gas produced water treatment

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Chemosphere 2024年 355卷 141834页

作者： Kong, Fan-xin Chen, Yu-Xuan Wang, Yu-kun Chen, Jin-fu State Key Laboratory of Heavy Oil Processing Beijing Key Laboratory of Oil & Gas Pollution Control China University of Petroleum Beijing102249 China

Membrane fouling caused by the organics-coated particles was the main obstacle for the highly efficient shale gas produced water (SGPW) treatment and recycling. In this study, a novel hybrid electrocoagulation (EC) and E-peroxone process coupled with UF (ECP-UF) process was proposed to examine the efficacy and elucidate the mechanism for UF fouling mitigation in assisting SGPW reuse. Compared to the TMP (transmembrane pressure) increase of −15 kPa in the EC-UF process, TMP in ECP-UF system marginally increased to −1.4 kPa for 3 filtration cycles under the current density of 15 mA/cm2. Both the total fouling index and hydraulically irreversible fouling index of the ECP-UF process were significantly lower than those of EC-UF process. According to the extended Derjaguin-Landau-Verwey-Overbeek theory, the potential barriers was the highest for ECP-UF processes due to the substantial increase of the acid-base interaction energy in ECP-UF process, which was well consistent with the TMP and SEM results. Turbidity and TOC of ECP-UF process were 63.6% and 45.8% lower than those of EC-UF process, respectively. According to the MW distribution, the variations of compounds and their relative contents were probably due to the oxidation and decomposing products of the macromolecular organics. The number of aromatic compound decreased, while the number of open-chain compounds (i.e., alkenes, alkanes and alcohols) increased in the permeate of ECP-UF process. Notably, the substantial decrease in the relative abundance of di-phthalate compounds was attributed to the high reactivity of these compounds with ·OH. Mechanism study indicated that ECP could realize the simultaneous coagulation, H2O2 generation and activation by O3, facilitating the enhancement of ·OH and Alb production and therefore beneficial for the improved water quality and UF fouling mitigation. Therefore, the ECP-UF process emerges as a high-efficient and space-saving approach, yielding a synergistic effect in mitigat

关键词： Produced Water

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Vapor-phase biodegradation and natural attenuation of petroleum VOCs in the unsaturated zone: A microcosm study

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Chemosphere 2023年第1期336卷 139275页

作者： Sun, Yue Liu, Yanbo Yue, Gangsen Cao, Jinhui Li, Chong Ma, Jie State Key Laboratory of Heavy Oil Processing Beijing Key Lab of Oil & Gas Pollution Control China University of Petroleum-Beijing Beijing102249 China

Traditional natural attenuation studies focus on aqueous process in the saturated zone while vapor-phase biodegradation and natural attenuation in the unsaturated zone received much less attention. This study used microcosm experiments to explore the vapor-phase biodegradation and natural attenuation of 23 petroleum VOCs in the unsaturated zone including 7 monoaromatic hydrocarbons, 6 n-alkanes, 4 cycloalkanes, 3 alkylcycloalkanes and 3 fuel ethers. We found that monoaromatic hydrocarbon vapors were easily attenuated with significantly high first-order attenuation rates (9.48 d−1-43.20 d−1) in live yellow earth, of which toluene and benzene had the highest rates (43.20 d−1 and 28.32 d−1, respectively). The 13 aliphatic hydrocarbons and 3 fuel ethers all have relatively low attenuation rates (−1) in live soil and negligible biodegradation contribution. We explored the effects of soil types (black soil, yellow earth, lateritic red earth and quartz sand), soil moisture (2, 5, 10, and 17 wt%) contents and temperatures (4, 15, 25, 35 and 45 °C) on the vapor attenuation. Results showed that increasing soil organic matter (SOM) content, silt content, porosity and soil microorganism numbers enhanced contaminant attenuation and remediation efficiency. Increasing moisture content reduced the apparent first-order biodegradation rates of monoaromatic hydrocarbon vapors. The vapor-phase biodegradation had optimal temperature (∼25 °C in yellow earth) and increasing or decreasing temperature slowed down biodegradation rate. Overall, this study enhanced our understanding of vapor-phase biodegradation and natural attenuation of petroleum VOCs in the unsaturated zone, which is critical for the long-term management and remediation of petroleum contaminated site. © 2023 Elsevier Ltd

关键词： Biodegradation

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Abiotic natural attenuation of 1,2,3-trichloropropane by natural magnetite under O2 perturbation

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Chemosphere 2024年 357卷 142040页

作者： Gu, Chunyun Li, Jiabin Zhou, Wei An, Jiayi Tian, Liting Xiong, Feng Fei, Wenbo Feng, Yangfan Ma, Jie State Key Laboratory of Heavy Oil Processing Beijing Key Lab of Oil & Gas Pollution Control China University of Petroleum-Beijing Beijing102249 China Institute of Resources and Environment Beijing Academy of Science and Technology Beijing100089 China

1,2,3-Trichloropropane (TCP) is an emerging groundwater pollutant, but there is a lack of reported studies on the abiotic natural attenuation of TCP by iron minerals. Furthermore, perturbation by O2 is common in the shallow subsurface by both natural and artificial processes. In this study, natural magnetite was selected as the reactive iron mineral to investigate its role in the degradation of TCP under O2 perturbation. The results indicated that the mineral structural Fe(II) on magnetite reacted with dissolved oxygen to generate O2−· and HO·. Both O2−· and HO· contributed to TCP degradation, with O2−· playing a more important role. After 56 days of reaction, 66.7% of TCP was completely dechlorinated. This study revealed that higher magnetite concentrations, smaller magnetite particle sizes, and lower initial TCP concentrations favored TCP degradation. The presence of 2 perturbation, providing crucial insights for the study of natural attenuation. © 2024

关键词： Groundwater

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Enhanced Ozonation of Nitrobenzene in Water Using Natural Iron Ores: Efficiencies, Mechanisms and Stability

SSRN

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SSRN 2024年

作者： Hu, Jingze Wang, Qingji Wang, Yuxian Wang, Qinghong Li, Zhuoyu Chen, Chunmao CNPC Research Institute of Safety and Environment Technology Beijing102206 China State Key Laboratory of Heavy Oil Processing Beijing Key Laboratory of Oil and Gas Pollution Control China University of Petroleum-Beijing Beijing102249 China

Natural minerals show potential for catalytic ozonation in industrial wastewater treatment. In this study, the efficiencies and mechanisms of two natural iron ores in catalytic ozonation process (COP) for aqueous nitrobenzene degradation were initially investigated. Compared with single O3, the removal of TOC increased by about 60% and 35% in COP with natural magnetite and pyrite, respectively. Both natural magnetite and pyrite could promote O3 decomposition to form hydroxyl radicals and 1O2. But the inner reaction pathways were different. The natural magnetite facilitated O3 decomposition through the Lewis acids and the electron transfer between Fe2+/Fe3+ on the catalyst surface, while electron transfer was the only pathway for O3 decomposition by natural pyrite. Continuous flow fixed-bed reactor was adopted to provide better simulation of the practical operation conditions, so that the potential of engineering application could be evaluated. The natural magnetite exhibited excellent catalytic activity and stability during long period continuous operation in fixed-bed reactor. The removal of TOC maintained at 81.9% under the optimized operating parameters of hydraulic retention time (2.84 h), O3 velocity (0.25 L min-1) and O3 concentration (30 mg L-1). HCO3- and PO43- obviously inhibited the removal of TOC through radical scavenging and surface -OH occupying. While low concentration of Cl- and SO42- showed negligible effect on the mineralization of aqueous nitrobenzene. After a long period operation for 672 h, the TOC removal of nitrobenzene solution in the magnetite-COP system was still stable at about 80%. The present study demonstrated the engineering application prospect of the natural iron ores in COP treatment of recalcitrant chemical wastewaters. © 2024, The Authors. All rights reserved.

关键词： Efficiency

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