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Photo-switchable Cu^(+)sites in metal-organic frameworks for adsorptive desulfurization

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Nano Research 2023年第2期16卷 3333-3338页

作者： Yu-Yang Gu Guoliang Liu Shi-Chao Qi Chen Gu Tao Yang Xiao-Qin Liu Lin-Bing Sun State Key Laboratory of Materials-Oriented Chemical Engineering Jiangsu National Synergetic Innovation Center for Advanced Material(SICAM)College of Chemical EngineeringNanjing Tech UniversityNanjing 211816China

Photo-switchable metal-organic frameworks(PMOFs)as energy-saving adsorbents for tailorable guest capture show admirable potentials for various applications like adsorptive ***,the regulation behavior of most reported PMOFs is based on weak physical interaction,and it is highly desired to introduce specific active sites to satisfy the demand of higher adsorption capacity and ***,for the first time,we prepared the PMOFs,azobenzene-functionalized HKUST-1(HK-Azo),simultaneously decorated with Cu_(2)O active sites that possess strong interaction with guest *** toπ-complexation interaction of Cu^(+)with aromatic sulfur compounds,the obtained HK-Azo shows obviously higher adsorption capacity on benzothiophene compared with *** ultraviolet(UV)and visible irradiation,azobenzene moieties in the PMOFs can transform their configuration freely and *** trans/cis isomerization of azobenzene causes exposure/shelter of Cu_(2)O active sites,leading to controllable benzothiophene *** HK-Azo exhibits the change of benzothiophene uptake up to 29.7%upon trans and cis isomerization,which is obviously higher than HKUST-1 with negligible *** work may inspire the development of new adsorption process regulated by light for adsorptive desulfurization that is impossible to realize by conventional PMOFs.

关键词： Cu+active sites metal-organic frameworks photo-switchable property azobenzene adsorptive desulfurization

Engineering Dual Oxygen Simultaneously Modified Boron Nitride for Boosting adsorptive desulfurization of Fuel

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Engineering 2022年第7期8卷 86-93页

作者： Jing Luo Yanchen Wei Yanhong Chao Chao Wang Hongping Li Jun Xiong Mingqing Hua Huaming Li Wenshuai Zhu School of Chemistry and Chemical Engineering&Institute for Energy Research Jiangsu UniversityZhenjiang 212013China State Key Laboratory of Heavy Oil Processing College of Chemical Engineering and EnvironmentChina University of Petroleum(Beijing)Beijing 102249China School of Materials Science and Engineering Jiangsu UniversityZhenjiang 212013China School of Pharmacy Jiangsu UniversityZhenjiang 212013China

Oxygen atoms usually co-exist in the lattice of hexagonal boron nitride(h-BN). The understanding of interactions between the oxygen atoms and the adsorbate, however, is still ambiguous on improving adsorptive desulfurization performance. Herein, simultaneously oxygen atom-scale interior substitution and edge hydroxylation in BN structure were constructed via a polymer-based synthetic *** results indicated that the dual oxygen modified BN(BN–2O) exhibited an impressively increased adsorptive capacity about 12% higher than that of the edge hydroxylated BN(BN–OH) fabricated via a traditional method. The dibenzothiophene(DBT) was investigated to undergo multimolecular layer type coverage on the BN–2O uneven surface via π–π interaction, which was enhanced by the increased oxygen doping at the edges of BN–2O. The density functional theory calculations also unveiled that the oxygen atoms confined in BN interior structure could polarize the adsorbate, thereby resulting in a dipole interaction between the adsorbate and BN–2O. This effect endowed BN–2O with the ability to selectively adsorb DBT from the aromatic-rich fuel, thereafter leading to an impressive prospect for the adsorptive desulfurization performance of the fuel. The adsorptive result was in good accordance with Freundlich and pseudo-second-order adsorption kinetics model results. Therefore, the designing of a polymer-based strategy could be also extended to other heteroatom doping systems to enhance adsorptive performance.

关键词： Polymer-based synthetic strategy Interior substitution BN Oxygen doping adsorptive desulfurization

Efficient desulfurization of gasoline fuel using ionic liquid extraction as a complementary process to adsorptive desulfurization

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Petroleum Science 2015年第2期12卷 330-339页

作者： N.Farzin Nejad A.A.Miran Beigi Petroleum Refining Technology Development Division Research Institute of Petroleum Industry

The extractive desulfurization of a model gaso- line containing several alkyl thiols and aromatic thiophenic compounds was investigated using two imidazolium-based ionic liquids （ILs）, 1-butyl-3-methylimidazolium tetrachloroaluminate, and 1-octyl-3-methylimidazolium te- trafluoroborate, as extractants. A fractional factorial design of experiments was employed to evaluate the effects and possible interactions of several process variables. Analysis of variance tests indicated that the number of extraction steps and the IL/gasoline volume ratio were of statistically highly significant, but none of the interactions were significant. The results showed that the desulfurization efficiency of the model gasoline by the ILs could reach 95.2 % under the optimal conditions. The optimized conditions were applied to study the extraction of thiophenic compounds in model gasoline and several real gasoline samples; the following order was observed in their separation： benzothio- phenc 〉 thiophcne 〉 3-methylthiophene 〉 2-methylthiophene, with 96.1% removal efficiency for benzothiophene. The IL extraction was successfully applied as a complementary process to the adsorptive desulfurization with acti- vated Raney nickel and acetonitrile solvent. The results indicated that the adsorptive process combined with IL extraction could provide high efficiency and selectivity, which can be regarded as a promising energy efficient desulfurization strategy for production of low-sulfur gasoline.

关键词： Liquid-liquid extraction Experimentaldesign adsorptive desulfurization Gasoline Thiopheniccompounds

Investigation on Modification of NaY Zeolite and Its Behaviors in Selective adsorptive desulfurization of FCC gasoline

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China Petroleum Processing & Petrochemical Technology 2009年第1期11卷 58-62页

作者： Zhu Heli Song Lijuan Gao Xiang Wang Hongguo Zhang Xiaotong Sun Zhaolin (Liaoning Key Laboratory of Petrochemical Engineering, Liaoning University of Petroleum and Chemical Technology, Fushun 113001) Liaoning Key Laboratory of Petrochemical Engineering Liaoning University of Petroleum and Chemical Technology Fushun 113001 China

NaY zeolite was modified with oxalic acid, and Ce(IV)Y(1) zeolite was obtained via liquid phase ion exchange between the modified NaY zeolite and cerium nitrate. The Ce(IV)Y(2) zeolite was obtained via liquid phase ion exchange between NaY zeolite and cerium nitrate. The performance of two Y zeolites [Ce(IV)Y(1) and Ce(IV)Y(2)] was compared through static selective adsorptive desulfurization of FCC gasoline at room temperature and normal pressure. The sulfur compounds and contents of the FCC gasoline were analyzed by microcoulometry and GC-SCD chromatogram. The results showed that the effect of adsorptive desulfurization of FCC gasoline achieved by Ce(IV)Y(1) zeolite was better than that of Ce(IV)Y(2) zeolite. The rate for adsorptive desulfurization of FCC gasoline by Ce(IV)Y(1) zeolite and Ce(IV)Y(2) zeolite was 85.0% and 62.4%, respectively. The Ce(IV)Y(1) zeolite could adsorb DMTs, which could not be adsorbed by Ce(IV)Y(2) zeolite. The rate of regeneration of extruded Ce(IV)Y(1)zeolite was 95.5%.

关键词： zeolite ion exchange FCC gasoline adsorptive desulfurization DMTs

Study on Modified Y Zeolites and Their Behaviors in Selective adsorptive desulfurization of FCC Gasoline (Ⅰ)

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China Petroleum Processing & Petrochemical Technology 2009年第4期11卷 18-22页

作者： Zhu Heli~(1,2) Liu Daosheng~2 Song Lijuan~2 Sun Zhaolin~2 (1.PetroChina Jinxi Petrochemical Company,Huludao 125001 2.Liaoning Key Laboratory of Petrochemical Engineering,Liaoning University of Petroleum and Chemical Technology) PetroChina Jinxi Petrochemical Company Huludao 125001 China Liaoning Key Laboratory of Petrochemical Engineering Liaoning University of Petroleum and Chemical Technology China

NaY zeolite was modified through dealumination with oxalic acid,and the HY zeolite was obtained by calcination of the modified NaY *** zeolite molding process was carried out at ambient temperature(25℃),and the influence of solid/fuel mass ratio and adsorptive desulfurization time on the HY zeolite were investigated through tests on static selective adsorptive desulfurization of FCC gasoline containing organic sulfur compounds(with a S content=135 ppm).The sulfur content and sulphide types in the FCC gasoline were analyzed by a GC 2010 sulfur analyzer and a GC-SCD *** test results showed that the molded HY zeolite was better than the unmolded HY *** a static adsorptive desulfurization time on the molded HY zeolite equating to 6 hours,a solid/fuel mass ratio of 1:3,the sulfur content of FCC gasoline was decreased to 30 ppm,and the desulfurization rate was equal to 78%.When the breakthrough point of the molded HY was equal to 50 ppm,the molded HY zeolite was capable of adsorbing 4.86 mg of sulfur per gram of *** the regeneration rate of molded HY zeolite was equal to 98%.

关键词： dealumination zeolite FCC gasoline adsorptive desulfurization

Removal of Heteroaromatic Sulfur Compounds by a Non-noble Metal Fe Single-atom Adsorbent

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China Petroleum Processing & Petrochemical Technology 2022年第2期24卷 46-57页

作者： LüYanjun Wen Jie Gong Qinmei Zhang Lianhong Li Airong Arshid Mahmood Ali Zhang Hui College of Chemistry and Chemical Engineering Southwest Petroleum UniversityChengdu 610500

Sulfur-containing compounds(SCCs)must be removed from fuels before *** this study,a novel non-noble metal Fe single-atom adsorbent(SA-Fe/CN)was synthesized using a core-shell strategy and applied for the adsorptive removal of benzothiophene(BT)and dibenzothiophene(DBT).The adsorption isotherms,thermodynamics,kinetics,and adsorption-regeneration cycles of DBT and BT on SA-Fe/CN were ***-Fe/CN exhibited a significant capacity to adsorb DBT,and the isothermal equilibrium was well described by the Langmuir *** Gibbs free energy values were negative(ΔG^(0)<0),indicating that the adsorption of DBT and BT was favored and *** adsorption process conformed to the pseudo-second-order kinetic model with high R^(2) values(0.9994,0.9987).The adsorption capacity of SA-Fe/CN for DBT and BT reached 163.21 mg/g and 90.35 mg/g,respectively,due to the highly active sites of the single atom and electrostatic interaction with the ***,SA-Fe/CN may be a promising adsorbent for SCC removal.

关键词： single-atom adsorbent adsorptive desulfurization thermodynamics and kinetics heteroaromatic sulfur compounds

Mssbauer spectroscopic characterization of ferrites as adsorbents for reactive adsorption desulfurization

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Chinese Journal of Catalysis 2016年第5期37卷 727-734页

作者：陈霄朱凯新 M.A.Ahmed 王军虎梁长海大连理工大学化工学院先进材料与催化工程实验室辽宁大连116012 中国科学院大连化学物理研究所穆斯堡尔数据中心辽宁大连116023 中国科学院大学北京100049 艾资哈尔大学理学院物理系

Sulfur in transportation fuels is a major source of air pollution. New strategies for the desulfurization of fuels have been explored to meet the urgent need to produce cleaner gasoline. adsorptive desulfurization（ADS） is one of the most promising complementary and alternative methods. Herein,nanocrystalline ferrite adsorbents were synthesized from metal nitrates and urea using a microwave assisted combustion method. A series of ADS experiments were performed using a fixed‐bed reactor to evaluate the ADS reactivity over the ferrites, which was found to have the order MgFe2O4〉NiFe2O4〉CuZnFe2O4〉ZnFe2O4〉CoFe2O4. This effect is explained by the fact that the low degree of alloying of Mg‐Fe and the doped Mg increased the interaction between Fe and S compounds,leading to a significant improvement in the desulfurization capability of the ***, Mg can dramatically promote the decomposition of thiophene. X‐ray diffraction and Mosbauer spectroscopy were used to characterize the fresh, regenerated, and sulfided *** the ferrite adsorbents were partially sulfided to bimetallic sulfides during the adsorption process, they were successfully regenerated after calcining at 500 °C in air.

关键词： Ferrite adsorptive desulfurization Msbauer spectroscopy Regeneration