More stringent environmental legislation imposes severe requirements to reduce the sulfur content in diesel to ultra-low levels with high efficient catalysts.In this paper,a series of CoMo/NDC@alumina catalysts were s...More stringent environmental legislation imposes severe requirements to reduce the sulfur content in diesel to ultra-low levels with high efficient catalysts.In this paper,a series of CoMo/NDC@alumina catalysts were synthesized by combination of the chemical vapor deposition of nitrogen-doped carbon(NDC)using 1,10-phenanthroline and co-impregnation of Mo and Co active components.The optimal catalyst with additive of 25%1,10-phenanthroline was screened by a series of property characterization and the hydrodesulfrization(HDS)active test.The amount of“CoMoS”active phase of the optimal CoMo/C3 catalyst increased 5.3%as compared with the CoMo/c-Al_(2)O_(3).The introduction of NDC improved the sulfidation degree of Mo by 21.8%as compared to the CoMo/c-Al_(2)O_(3) catalyst,which was beneficial to form more active sites.The HDS conversion of the NDC supported catalysts are higher than CoMo/c-Al_(2)O_(3) whether for the dibenzothiophene(DBT)or 4,6-dimethyl dibenzothiophene(4,6-DMDBT).Further hydroprocessing evaluation with Dagang diesel revealed that the CoMo/C3 catalyst possessed higher HDS property and the removal rate of DBTs in the diesel increased by 4%–11%as compared to the CoMo/c-Al_(2)O_(3) catalyst.展开更多
Higher alcohol synthesis(HAS)from syngas could efficiently alleviate the dependence on the traditional fossil resources.However,it is still challenging to construct high-performance HAS catalysts with satisfying selec...Higher alcohol synthesis(HAS)from syngas could efficiently alleviate the dependence on the traditional fossil resources.However,it is still challenging to construct high-performance HAS catalysts with satisfying selectivity,space–time yield(STY),and stability.Herein,we designed a diatomic catalyst by anchoring Co and Cu sites onto a hierarchical porous N-doped carbon matrix(Co/Cu–N–C).The Co/Cu–N–C is efficient for HAS and is among the best catalysts reported.With a COconversion of 81.7%,C2+OHselectivity could reach 58.5%with an outstanding C2+OH STY of 851.8 mg/g·h.We found that the N4–Co1 and Cu1–N4 showed an excellent synergistic effect.The adsorption of CO occurred on the Co site,and the surrounding nitrogen sites served as a hydrogen reservoir for the CO reduction reactions to form CHxCo.Meanwhile,the Cu sites stabilized a CHOCu species to interact with CHxCo,facilitating a barrier-free formation of C2 species,which is responsible for the high selectivity of higher alcohols.展开更多
基金supports by National Natural Science Foundation of China(NSFC)(Nos.21878329 and 21476257)the National Key Research and Development Program Nanotechnology Specific Project(No.2020YFA0210900)Science Foundation of China University of Petroleum,Beijing(No.2462018QZDX04).
文摘More stringent environmental legislation imposes severe requirements to reduce the sulfur content in diesel to ultra-low levels with high efficient catalysts.In this paper,a series of CoMo/NDC@alumina catalysts were synthesized by combination of the chemical vapor deposition of nitrogen-doped carbon(NDC)using 1,10-phenanthroline and co-impregnation of Mo and Co active components.The optimal catalyst with additive of 25%1,10-phenanthroline was screened by a series of property characterization and the hydrodesulfrization(HDS)active test.The amount of“CoMoS”active phase of the optimal CoMo/C3 catalyst increased 5.3%as compared with the CoMo/c-Al_(2)O_(3).The introduction of NDC improved the sulfidation degree of Mo by 21.8%as compared to the CoMo/c-Al_(2)O_(3) catalyst,which was beneficial to form more active sites.The HDS conversion of the NDC supported catalysts are higher than CoMo/c-Al_(2)O_(3) whether for the dibenzothiophene(DBT)or 4,6-dimethyl dibenzothiophene(4,6-DMDBT).Further hydroprocessing evaluation with Dagang diesel revealed that the CoMo/C3 catalyst possessed higher HDS property and the removal rate of DBTs in the diesel increased by 4%–11%as compared to the CoMo/c-Al_(2)O_(3) catalyst.
基金the National Key Research and Development Program of China(grant nos.2019YFB1503903,2019YFB1503904,and 2018YFB1501403)The Natural Science Foundation of Fujian Province of China(grant no.2019J06005).
文摘Higher alcohol synthesis(HAS)from syngas could efficiently alleviate the dependence on the traditional fossil resources.However,it is still challenging to construct high-performance HAS catalysts with satisfying selectivity,space–time yield(STY),and stability.Herein,we designed a diatomic catalyst by anchoring Co and Cu sites onto a hierarchical porous N-doped carbon matrix(Co/Cu–N–C).The Co/Cu–N–C is efficient for HAS and is among the best catalysts reported.With a COconversion of 81.7%,C2+OHselectivity could reach 58.5%with an outstanding C2+OH STY of 851.8 mg/g·h.We found that the N4–Co1 and Cu1–N4 showed an excellent synergistic effect.The adsorption of CO occurred on the Co site,and the surrounding nitrogen sites served as a hydrogen reservoir for the CO reduction reactions to form CHxCo.Meanwhile,the Cu sites stabilized a CHOCu species to interact with CHxCo,facilitating a barrier-free formation of C2 species,which is responsible for the high selectivity of higher alcohols.
