Preparation of highly active hydrodesulfurization catalysts is extremely meaningful for the sulfur removal from thiophene substances.In this work,commercial nano-Al_(2)O_(3)with mesoporous structure supported monometa...Preparation of highly active hydrodesulfurization catalysts is extremely meaningful for the sulfur removal from thiophene substances.In this work,commercial nano-Al_(2)O_(3)with mesoporous structure supported monometallic phosphide(NiP/Al_(2)O_(3)and MoP/Al_(2)O_(3))and bimetallic phosphide(NiMoP/Al_(2)O_(3)with various Ni/Mo molar ratio)catalysts are successfully prepared by temperature-programmed reduction.X-ray diffraction(XRD)result shows the Ni/Mo molar ratio affect the crystal phase in catalysts.Scanning electron microscopy(SEM),transmission electron microscopy(TEM)and X-ray photoelectron spectroscopy(XPS)characterizations co-confirm the interact between Ni and Mo elements in bimetallic phosphide.Catalyst evaluation in hydrodesulfurization of dibenzothiophene shows that bimetallic phosphide samples exhibit better catalytic performance than monometallic phosphide.62.1%conversion and 86.3%biphenyl selectivity with 30 h stability are achieved over NiMoP/Al_(2)O_(3)(Ni/Mo=1∶1)catalyst at 400℃under 3 MPa H_(2).All characterization results demonstrate that the improved activity of bimetallic phosphide owes to the Ni-Mo synergistic effect in NiMoP/Al_(2)O_(3)(Ni/Mo=1∶1)catalyst.This finding provides a guide to the design of bimetallic catalyst with synergistic effect.展开更多
In the current study simultaneous reactions of hydrodesulfurization(HDS) of dibenzothiophene(DBT) and reforming of methanol in a micro-autoclave reactor were studied over bi-metallic(Co-Mo/Al2O3 and Ni-Mo/Al2O3) and t...In the current study simultaneous reactions of hydrodesulfurization(HDS) of dibenzothiophene(DBT) and reforming of methanol in a micro-autoclave reactor were studied over bi-metallic(Co-Mo/Al2O3 and Ni-Mo/Al2O3) and tri-metallic(Pd-Co-Mo/Al2O3 and Pd-Ni-Mo/Al2O3) catalyst systems which were prepared by incipient impregnation method.In situ hydrogen utilization and low Pd loadings were the major targets of this study.For comparison purpose,catalytic activity was separately determined for both the methanol reforming and HDS of DBT reactions as well.Ni based catalysts were confirmed with better activity than Co ones for both the reactions with Pd promoted ones ranking at the top i.e.Pd-Ni-Mo/Al2O3 > Ni-Mo/Al2O3 > Pd-Co-Mo/Al2O3 > Co-Mo/Al2O3 where Pd-Ni-Mo/Al2O3 showed 91% DBT conversion at 380 ℃ and 12 h reaction time.Some of the selected organic additives on catalytic activity were tested for their effect toward HDS reaction which was unique with close relation to their chemical nature.Reaction products were quantitatively and qualitatively analyzed via HPLC and GC-MS techniques respectively which helped in elucidating reaction mechanism.展开更多
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 o...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.展开更多
基金supported by National Natural Science Foundation of China(22202093)the Scientific and Technological Innovation Youth Talent Team of Shanxi Province(202204051001005)。
文摘Preparation of highly active hydrodesulfurization catalysts is extremely meaningful for the sulfur removal from thiophene substances.In this work,commercial nano-Al_(2)O_(3)with mesoporous structure supported monometallic phosphide(NiP/Al_(2)O_(3)and MoP/Al_(2)O_(3))and bimetallic phosphide(NiMoP/Al_(2)O_(3)with various Ni/Mo molar ratio)catalysts are successfully prepared by temperature-programmed reduction.X-ray diffraction(XRD)result shows the Ni/Mo molar ratio affect the crystal phase in catalysts.Scanning electron microscopy(SEM),transmission electron microscopy(TEM)and X-ray photoelectron spectroscopy(XPS)characterizations co-confirm the interact between Ni and Mo elements in bimetallic phosphide.Catalyst evaluation in hydrodesulfurization of dibenzothiophene shows that bimetallic phosphide samples exhibit better catalytic performance than monometallic phosphide.62.1%conversion and 86.3%biphenyl selectivity with 30 h stability are achieved over NiMoP/Al_(2)O_(3)(Ni/Mo=1∶1)catalyst at 400℃under 3 MPa H_(2).All characterization results demonstrate that the improved activity of bimetallic phosphide owes to the Ni-Mo synergistic effect in NiMoP/Al_(2)O_(3)(Ni/Mo=1∶1)catalyst.This finding provides a guide to the design of bimetallic catalyst with synergistic effect.
基金Fundamental Research Foundation of Sinopec(X505015)
文摘In the current study simultaneous reactions of hydrodesulfurization(HDS) of dibenzothiophene(DBT) and reforming of methanol in a micro-autoclave reactor were studied over bi-metallic(Co-Mo/Al2O3 and Ni-Mo/Al2O3) and tri-metallic(Pd-Co-Mo/Al2O3 and Pd-Ni-Mo/Al2O3) catalyst systems which were prepared by incipient impregnation method.In situ hydrogen utilization and low Pd loadings were the major targets of this study.For comparison purpose,catalytic activity was separately determined for both the methanol reforming and HDS of DBT reactions as well.Ni based catalysts were confirmed with better activity than Co ones for both the reactions with Pd promoted ones ranking at the top i.e.Pd-Ni-Mo/Al2O3 > Ni-Mo/Al2O3 > Pd-Co-Mo/Al2O3 > Co-Mo/Al2O3 where Pd-Ni-Mo/Al2O3 showed 91% DBT conversion at 380 ℃ and 12 h reaction time.Some of the selected organic additives on catalytic activity were tested for their effect toward HDS reaction which was unique with close relation to their chemical nature.Reaction products were quantitatively and qualitatively analyzed via HPLC and GC-MS techniques respectively which helped in elucidating reaction mechanism.
文摘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.
基金Beijing Natural Science Foundation(2052009)Funding Project for Academic Human Resources Development in Institutions of Higher Learning Under the Jurisdiction of Beijing Municipality(PHR200907129)
