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Nano Research 2022年第8期15卷 7052-7062页

作者： Dongxu Wang Lei Wang Yanqing Jiao Aiping Wu Haijing Yan Xin Kang Chungui Tian Jiancong Liu Honggang Fu Key Laboratory of Functional Inorganic Material Chemistry Ministry of Education of the People’s Republic of ChinaHeilongjiang UniversityHarbin 150080China

Hydrodesulfurization(HDS)is an essential process in clean fuel oil production,however,the huge challenge is the synthesis of the catalyst with plentiful active sites.Here,we have shown the design of few-layered,ultrashort Ni-Mo-S slabs dispersed on reduced graphene oxide(Ni-Mo-S/rGO-A)based on anchoring[PMo_(12)O_(40)]3−clusters and Ni^(2+)on polyethyleneimine(PEI)-modified graphite oxide.Structural characterizations(transmission electron microscopy(TEM),X-ray absorption fine structure(XAFS),etc.)show that Ni-Mo-S slabs with predominant monolayer and partial substitution of edge Mo atoms by isolated Ni atoms have rich accessible edge Ni-Mo-S sites and high sulfurization degree.All virtues endow it with plentiful edge-active sites,and consequently,the enhanced performance for Hydrodesulfurization of dibenzothiophene(DBT).The Hydrodesulfurization proceeds via a more-favorable direct desulfurization(DDS)route with a reaction rate constant(kHDS)of 48.6×10^(−7)mol·g^(−1)·s^(−1)over Ni-Mo-S/rGO-A catalyst,which is 4.3 times greater than that over traditional Ni-Mo-S/Al_(2)O_(3)catalyst and at the forefront of reported catalysts.

关键词： few-layered Ni-promoted MoS_(2) confined growth reduced graphene oxide high sulfurization degree Hydrodesulfurization

Study on the mechanism of Hydrodesulfurization of tetrahydrothiophene catalyzed by nickel phosphide

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Petroleum Science 2022年第3期19卷 1390-1400页

作者： Chuan-Tao Zhu Li-Qiang Zhang Mei-Ling Zhou Xin-Wei Wang Zheng-Da Yang Ri-Yi Lin De-Wei Yang College of New Energy China University of PetroleumQingdao266580China

Hydrodesulfurization(HDS)reaction can significantly reduce the viscosity and sulfur content of heavy oil,while the HDS reaction mechanism of tetrahydrothiophene as the main sulfide in heavy oil is still unclear.The HDS experiment of tetrahydrothiophene catalyzed by nickel phosphide(Ni_(2)P)is carried out at 200-300°C.The results indicate that the H_(2)S production under the catalysis of Ni_(2)P increases obviously within 200-250°C.The main gas products of HDS reaction are butane,butene and H_(2)S.Meanwhile,the mechanism of tetrahydrothiophene catalyzed by Ni_(2)P is analyzed based on Density Functional Theory(DFT).It is revealed that the adsorption model is most stable when tetrahydrothiophene is vertically adsorbed on the V-Ni-Hcp1 site of Ni_(2)P(001).The C-S bond is elongated and the C-C bond is shortened after adsorption.Hydrogenation(HYD)is the most possible reaction route of tetrahydrothiophene on Ni_(2)P(001)surface.There are two routes with the lowest activation energy,which are C_(4)H_(8)S→C_(4)H_(8)SH^(*)→C_(4)H_(9)SH^(*)→C_(4)H_(10)+H_(2)S and C_(4)H_(8)S→C_(4)H9S^(*)→C_(4)H_(9)^(*)+SH^(*)→C_(4)H_(10)+H_(2)S.Butane and H_(2)S are produced in the reaction,corresponding to the experimental results.This study provides a basis for understanding of the HDS mechanism of tetrahydrothiophene catalyzed by Ni_(2)P.

关键词： Tetrahydrothiophene Nickel phosphide Hydrodesulfurization Hydrogen sulfide DFT

Tuning active sites in MoS_(2)-based catalysts via H_(2)O_(2)etching to enhance Hydrodesulfurization performance

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Petroleum Science 2023年第6期20卷 3875-3886页

作者： Shui-Sen He Ting-Ting Huang Chao Chen Yu Fan State Key Laboratory of Heavy Oil Processing China University of PetroleumBeijing102249China State Key Laboratory Base for Eco-Chemical Engineering in College of Chemical Engineering Qingdao University of Science and TechnologyZhengzhou Road 53Qingdao266042ShandongChina

A H_(2)O_(2)etching strategy was adopted to introduce coordinatively unsaturated sites(CUS)on MoS_(2)-based catalysts for dibenzothiophene(DBT)Hydrodesulfurization(HDS).The CUS concentrations on MoS_(2) slabs were finely regulated by changing the concentrations of H_(2)O_(2)solution.With the increasing H_(2)O_(2)concentrations(0.1–0.3 mol/L),The CUS concentrations on MoS_(2) slabs increased gradually.However,the high-concentration H_(2)O_(2)etching(0.5 mol/L)increased the MoOxSy and MoO_(3) contents on MoS_(2) slabs compared to etching with the H_(2)O_(2)concentration of 0.3 mol/L,which led to the less CUS concentration in the sulfided Mo–H-0.5 catalyst than in the sulfided Mo–H-0.3 catalyst.A microstructure-activity correlation indicated that the CUS introduced by H_(2)O_(2)etching on MoS_(2) slabs significantly enhanced DBT HDS.Different Co loadings were further introduced into Mo–H-0.3,which had the most CUS concentration,and the corresponding 0.2-CoMo catalyst with the highest CoMoS content(3.853 wt%)exhibited the highest reaction rate constant of 6.95×10^(−6)mol g^(−1)s^(−1)among these CoMo catalysts.

关键词： H_(2)O_(2)etching Coordinatively unsaturated site concentrations CoMoS Hydrodesulfurization

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 protocol.The 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 4,6-dimethyldibenzothiophene.It 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 substantially.The 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

Hierarchically porous Beta/SBA-16 with different silica-alumina ratios and the Hydrodesulfurization performances of DBT and 4,6-DMDBT

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Petroleum Science 2022年第1期19卷 375-386页

作者： Jin-Lin Mei Yu Shi Cheng-Kun Xiao Ao-Cheng Wang Ai-Jun Duan Xi-Long Wang State Key Laboratory of Heavy Oil Processing China University of Petroleum(Beijing)Beijing 102249PR China

Hierarchically porous Beta/SBA-16(BS)composite materials,combining the characteristics of the acidity from the Beta zeolite and the three-dimensional structure from SBA-16,were synthesized successfully through a two-step in-situ assembly hydrothermal crystallization method.A series of Ni Mo catalysts supported on BS with different silica-alumina ratios were prepared.The supports and the corresponding catalysts were characterized by XRD,N_(2) physisorption,^(27)Al MAS NMR,TEM,pyridine-FTIR,Raman,XPS and HRTEM.The activities of series catalysts were evaluated by the Hydrodesulfurization(HDS)performances of dibenzothiophene(DBT)and 4,6-dimethyldibenzothiophene(4,6-DMDBT).It was found that the Beta crystallites were embedded into SBA-16 through silanols accompanied by dealumination on the T3-T9 sites of Beta crystallites.Ni Mo/BS-3 with a silica-alumina ratio of 100 exhibited the highest DBT and 4,6-DMDBT HDS activities at the WHSV value of 10 h^(-1),with the conversions of 95.9%and 86.9%respectively,due to the synergistic effects of the suitable specific surface areas,the relatively large pore size,appropriate acidity,the relatively high sulfidation degree,moderate dispersity and good stacking degree of Mo S;active phases.

关键词： Beta/SBA-16 Dibenzothiophene 4,6-Dimethyldibenzothiophene Hydrodesulfurization

The effect of chelating agent on Hydrodesulfurization reaction of ordered mesoporous alumina supported Ni Mo catalysts

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Petroleum Science 2022年第1期19卷 321-328页

作者： Di Hu Hui-Ping Li Jin-Lin Mei Cheng-Kun Xiao En-Hua Wang Xi-Yue Chen Wen-Xin Zhang Ai-Jun Duan State Key Laboratory of Heavy Oil Processing China University of Petroleum-BeijingBeijing102249China

In this paper,ordered mesoporous alumina(OMA)support with the high surface area(328 m^(2)g^(-1))and the large pore volume 0.74(cm^(3)·g^(-1))was synthesized by homogeneous precipitation method.And the influence of EDTA on the physical and chemical properties of the modified catalysts was also studied.The characteristic results showed that the addition of EDTA could adjust the metal-support interaction and improved the acidity of the corresponding catalyst.Combined with the catalytic performance results,the EDTA-modified Ni Mo E(1.0)/OMA catalyst displays the highest DBT Hydrodesulfurization conversion(97.7%).

关键词： Chelating agent Hydrodesulfurization Ordered mesoporous alumina

Highly Active Sulfided NiPMo Hydrodesulfurization Catalyst Prepared from Keggin-type Phosphomolybdic Acid

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China Petroleum Processing & Petrochemical Technology 2023年第1期25卷 133-143页

作者： Zhu Tianhan Li Wenxu Wang Haiyong Wang Chenguang Yang Bin Guangzhou Institute of Energy Conversion Chinese Academy of SciencesGuangzhou 510640China

A highly active sulfided NiPMo/MCM-41(NiPMo-S/M41)Hydrodesulfurization(HDS)catalyst was successfully synthesized using Keggin-type phosphomolybdic acid as the phosphorus and molybdenum source and thioacetamide as the sulfur source.The supported catalysts NiPMo/M41,Ni_(2)P-Mo/M41,and Ni_(2)P/M41 were also prepared to investigate the effects of Mo,S,and the Keggin structure on the HDS performance.The HDS activities of NiPMo/M41 and NiPMo-S/M41 toward dibenzothiophene were much higher than that of Ni_(2)P-Mo/M41,demonstrating that the active phases in the Keggin-structured catalysts were significantly superior to the Mo-modified Ni_(2)P phase.The HDS activities of the catalysts followed the order NiPMo-S/M41(96.7%)>NiPMo/M41(89.9%)>Ni_(2)P-Mo/M41(53.5%)>Ni_(2)P/M41(48.9%).For Ni_(2)P/M41,Ni_(2)P-Mo/M41,and NiPMo/M41,cyclohexylbenzene(CHB)was formed in low concentrations(<21.0%),indicating that direct desulfurization was the favored reaction route and that this did not change for Keggin-structured NiPMo/M41.By contrast,the CHB selectivity of NiPMo-S/M41 increased to 44.6%,much higher than that of NiPMo/M41(17.6%),demonstrating that sulfidation enhanced the hydrogenation ability,which was ascribed to a metal-acid synergistic effect.

关键词： Keggin-type phosphomolybdic acid Hydrodesulfurization dibenzothiophene

Effect of Reduction Temperature on the Hydrodesulfurization Performance of Carbon-doped Alumina-supported Nickel Phosphide Catalyst

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China Petroleum Processing & Petrochemical Technology 2022年第3期24卷 44-51页

作者： Jiang Nan Wang Shuai Jiang Bolong Innovation Institute for Sustainable Maritime Architecture Research and Technology Qingdao University of TechnologyQingdao266000China Provincial Key Laboratory of Oil&Gas Chemical Technology College of Chemistry&Chemical EngineeringNortheast Petroleum UniversityDaqing163318China

Nickel phosphide-carbon-doped alumina(Ni_(2)P/Al_(2)O_(3)-C)catalysts with 10 wt.%Ni_(2)P loading were successfully prepared via a hydrothermal reduction process and the effect of reduction temperature on the Hydrodesulfurization(HDS)performance of the as-prepared Ni_(2)P/Al_(2)O_(3)-C catalysts was investigated.The properties of the support(Al_(2)O_(3)-C)and Ni_(2)P/Al_(2)O_(3)-C catalysts were characterized by transmission electron microscopy,scanning electron microscopy,Brunauer-Emmett-Teller measurements,X-ray diffractometry,and X-ray photoelectron spectroscopy.The results indicated that the incorporation of carbon in the support aided the reduction of Ni_(2)P.With an increase in the reduction temperature,Ni and Ni_(12)P_(5) were first generated and then converted into crystalline Ni_(2)P.Furthermore,a higher reduction temperature enhanced the HDS performance of the catalyst by generating more well-dispersed active-phase crystalline Ni_(2)P.

关键词： Hydrodesulfurization carbon doped alumina Ni_(2)P

Coupling non-isothermal trickle-bed reactor with catalyst pellet models to understand the reaction and diffusion in gas oil Hydrodesulfurization

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Chinese Journal of Chemical Engineering 2020年第4期28卷 1095-1106页

作者： Xingqiang Zhao Changfeng Yang Mengke Lu Yao Shi Gang Qian Xinggui Zhou Xuezhi Duan State Key Laboratory of Chemical Engineering East China University of Science and Technology130 Meilong RoadShanghai 200237China

In this work,a trickle-bed reactor coupled with catalyst pellet model is employed to understand the effects of the temperature and catalyst pellet structures on the reaction-diffusion behaviors in gas oil Hydrodesulfurization(HDS).The non-isothermal reactor model is determined to be reasonable due to non-negligible temperature variation caused by the reaction heat.The reaction rate along the reactor is mainly dominated by the temperature,and the sulfur concentration gradient in the catalyst pellet decreases gradually along the reactor,leading to the increased internal effectiveness factor.For the fixed catalyst bed volume,there exists a compromise between the catalyst reaction rate and effectiveness factor.Under commonly studied catalyst pellet size of 0.8-3 mm and porosity of 0.4-0.8,an optimization of the temperature and catalyst pellet structures is carried out,and the optimized outlet sulfur content decreases to 7.6 wppm better than the commercial level at 0.96 mm of the catalyst pellet size and 0.40 of the catalyst porosity.

关键词： Hydrodesulfurization Catalyst pellet Trickle-bed reactor Coupling model Reaction-diffusion behavior

Experimental and theoretical study of microwave enhanced catalytic Hydrodesulfurization of thiophene in a continuous-flow reactor

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Frontiers of Chemical Science and Engineering 2019年第4期13卷 744-758页

作者： Hui Shang Pengfei Ye Yude Yue Tianye Wang Wenhui Zhang Sainab Omar Jiawei Wang State Key Laboratoiy of Heavy Oil Processing China University of Petroleum(Beijing)Beijing 102249China European Biocncrgy Research Institute Aston UniversityBirminghamB47ETUK

Hydrodesulfiirization(HDS)of thiophene,as a gasoline model oil,over an industrial Ni-Mo/Al2O3 catalyst was investigated in a continuous system under microwave irradiation.The HDS efficiency was much higher(5%-14%)under microwave irradiation than conventional heating.It was proved that the reaction was enhanced by both microwave thermal and non-thermal effects.Microwave selective heating caused hot spots inside the catalyst,thus improved the reaction rate.From the analysis of the non-thermal effect,the molecular collisions were significantly increased under microwave irradiation.However,instead of being reduced,the apparent activation energy increased.This may be due to the microwave treatment hindering the adsorption though upright S-bind(η1)and enhancing the parallel adsorption(η5),both adsorptions were considered to favor to the direct desulfurization route and the hydrogenation route respectively.Therefore,the HDS process was considered to proceed along the hydrogenation route under microwave irradiation.

关键词： thiophene microwave irradiation Hydrodesulfurization non-thermal microwave effect