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,ultras...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.展开更多
基金the National Key Research and Development Program of China(No.2018YFE0201704)the National Natural Science Foundation of China(Nos.U20A20250,91961111,21901064,and 22171074)+1 种基金the Natural Science Foundation of Heilongjiang Province(No.ZD2021b003)University Nursing Program for Young Scholars with Creative Talents in Heilongjiang Province(No.UNPYSCT-2018013)。
文摘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.
