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Al-modified yolk-shell silica particle-supported NiMo catalysts for ultradeep hydrodesulfurization of dibenzothiophene and 4,6-dimethyldibenzothiophene:Efficient accessibility of active sites and suitable acidity

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Petroleum Science 2024年第1期21卷 654-666页

作者： Ke Yu Wei-Min Kong Zhen Zhao Ai-Jun Duan Lian Kong Xi-Long Wang State Key Laboratory of Heavy Oil Processing China University of PetroleumBeijing102249China Institute of Catalysis for Energy and Environment College of Chemistry and Chemical EngineeringShenyang Normal UniversityShenyang 110034LiaoningChina

Yolk-shell SiO2 particles(YP)with center-radial meso-channels were fabricated through a simple and effective method.Al-containing YP-supported NiMo catalysts with different Al amounts(NiMo/AYP-x,x=Si/Al molar proportion)were prepared and dibenzothiophene(DBT)and 4,6-dimethyl-dibenzothiophene(4,6-DMDBT)were employed as the probes to evaluate the hydrodesulfurization(HDS)catalytic performance.The as-prepared AYP-x carriers and corresponding catalysts were characterized by some advanced characterizations to obtain deeper correlations between physicochemical properties and the HDS performance.The average pore sizes of series AYP-x supports are above 6.0 nm,which favors the mass transfer of organic sulfides.The cavity between the yolk and the shell is beneficial for the enrichment of S-containing compounds and the accessibility between reactants and active metals.Aluminum embedded into the silica framework could facilitate the formation of Lewis(L)and Brønsted(B)acid sites and adjust the metal-support interaction(MSI).Among all the as-synthesized catalysts,NiMo/AYP-20 catalyst shows the highest HDS activities.The improved HDS activity of NiMo/AYP-20 catalyst is attributed to the perfect combination of excellent structural properties of the yolk-shell mesoporous silica,enhanced acidity,moderate MSI,and good accessibility/dispersion of active components.

关键词： Al-containing yolk-shell silica particles Accessibility Acidity Metal-support interaction hydrodesulfurization

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Combined Promoting Effects of Specific Organic Functional Groups and Alumina Surface Characteristics for the Design of a Highly Efficient NiMo/Al_(2)O_(3) hydrodesulfurization Catalyst

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China Petroleum Processing & Petrochemical Technology 2024年第1期26卷 1-11页

作者： Li Huifeng Li Mingfeng Zhang Le Wang Wei Nie Hong National Energy R&D Center of Petroleum Refining Technology SINOPEC Research Institute of Petroleum Processing Co.Ltd.Beijing 100083China

To prepare a highly efficient NiMo/Al_(2)O_(3) hydrodesulfurization catalyst,the combined effects of specific organic functional groups and alumina surface characteristics were investigated.First,the correlation between the surface characteristics of four different alumina and the existing Mo species states was established.It was found that the Mo equilibrium adsorption capacity can be used as a specific descriptor to quantitatively evaluate the changes in surface characteristics of different alumina.A lower Mo equilibrium adsorption capacity for alumina means weaker metal-support interaction and the loaded Mo species are easier to transform into MoS2.However,the Mo-O-Al bonds still exist at the metal-support interface.The introduction of cationic surfactant hecadecyl trimethyl ammonium bromide(CTAB)can further improve Mo species dispersion through electrostatic attraction with Mo anions and interaction of its alkyl chain with the alumina surface;meanwhile,the introduction of ethylenediamine tetraacetic acid(EDTA)can complex with Ni ions to enhance the Ni-promoting effect on Mo.Therefore,the NiMo catalyst designed using alumina with lower Mo equilibrium adsorption capacity and the simultaneous addition of EDTA and CTAB exhibits the highest hydrodesulfurization activity for 4,6-dimethyl dibenzothiophene because of its proper metal-support interaction and more well-dispersed Ni-Mo-S active phases.

关键词： alumina Mo equilibrium adsorption capacity organic functional groups metal-support interaction hydrodesulfurization

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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

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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

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The confined growth of few-layered and ultrashort-slab Ni-promoted MoS_(2)on reduced graphene oxide for deep-degree hydrodesulfurization

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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

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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

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Optimization of dendritic TS-1/Silica micro–mesoporous composites for efficient hydrodesulfurization of dibenzothiophene and 4,6-dimethyldibenzothiophene

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Petroleum Science 2023年第4期20卷 2521-2530页

作者： Cheng-Kun Xiao Yu-Tong Zou Dong-Ze Li En-Hua Wang Ao-Cheng Wang Dao-Wei Gao Ai-Jun Duan Peng Zheng Xi-Long Wang State Key Laboratory of Heavy Oil Processing China University of PetroleumBeijing102249China School of Chemistry and Chemical Engineering University of JinanJinanShandong250022China

A novel composite material(TD)composed of TS-1 microcrystalline and dendritic mesoporous silica nanospheres(DMSNs)was successfully prepared.The TD composite material had open pore structure and large specific surface area,which was conducive to the mass transfer of reactants and products.The Ti element in TS-1 could be used as an electron assistant,and the spillover d-electrons were conducive to the improvement of the sulfidation and dispersion of MoS_(2),thereby forming more type II MoS_(2) active phases.The incorporation of Ti could bring more Brønsted(B)and Lewis(L)acid,which was conducive to the hydrogenation pathway(HYD)selectivity(41.2%)of dibenzothiophene(DBT)hydrodesulfurization(HDS)and isomerization(ISO)route selectivity(21.9%)of 4,6-dimethyldibenzothiophene(4,6-DMDBT)HDS,thus improve the HDS activity of DBT and 4,6-DMDBT.NiMo/TD-70(Aging temperature=70℃)had the best HDS activities of DBT(99.0%)and 4,6-DMDBT(93.7%)due to its large open pore structure,good acidity,suitable metal-support interaction(MSI)and perfect dispersion of the metallic active sites.

关键词： Dendritic TS-1-DMSNs composites NiMo/TD catalysts Dibenzothiophene4,6-Dimethyldibenzothiophene hydrodesulfurization

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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 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

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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

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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

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