This paper reports a sustainable,water-assisted,solid-state method for synthesizing ammonium nickel molybdate((NH4)HNi2(OH)2(MoO4)2,ANM),a precursor for an unsupported hydrodesulfurization(HDS) catalyst.The ...This paper reports a sustainable,water-assisted,solid-state method for synthesizing ammonium nickel molybdate((NH4)HNi2(OH)2(MoO4)2,ANM),a precursor for an unsupported hydrodesulfurization(HDS) catalyst.The associated ANM formation mechanism is also discussed.The synthesis route consists of physical mixing of the raw materials,water-assisted grinding and heating.The formation mechanism involves replacement of a Mo atom by a Ni atom,generating the metastable intermediate(NH4)4(NiH6Mo6O(24))·5H2O.Heating of this intermediate at 120 ℃ removes the added water and produces ANM.Catalysts prepared by this method exhibit almost the same physicochemical properties and catalytic performance during the HDS of dibenzothiophene as materials made from ANM synthesized by a chemical precipitation procedure.Compared with traditional hydrothermal or chemical precipitation methods,this water-assisted,solid-state synthesis provides several significant advantages,including simplifying the synthetic procedure,reducing waste and energy costs and increasing product yields.These features will be highly important with regard to allowing the application of ANM in industrial-scale processes involving HDS reactions.This water-assisted,solid-state strategy can also be extended to the synthesis of isomorphous compounds such as ammonium cobalt(zinc and copper) molybdate.展开更多
Electron-hole separation is a critical step to achieving efficient photocatalysis, towards which use of co-catalysts has become a widely used strategy. Despite the tremendous efforts and demonstrated functions of nobl...Electron-hole separation is a critical step to achieving efficient photocatalysis, towards which use of co-catalysts has become a widely used strategy. Despite the tremendous efforts and demonstrated functions of noble metal co-catalysts, seeking noble metal-free co-catalysts will always be the goal when designing cost- effective, high-performance hybrid photocatalysts. In this work, we demonstrate that MoS~ nanosheets with 1T phase (i.e., octahedral phase) can function as a co-catalyst with multiple merits: (1) Noble-metal-free; (2) high mobility for charge transport; (3) high density of active sites for H2 evolution on basal planes; (4) good performance stability; (5) high light transparency. As demonstrated in both photocatalytic hydrogen production and Rhodamine B degradation, the developed hybrid structure with TiO2 exhibits excellent performance, in sharp contrast to bare TiO2 and the hybrid counterpart with 2H-MoS2.展开更多
基金supported by the National Natural Science Fundation of China(U1162203,21106185)the Fundamental Research Funds for the Central Universities(15CX02023A,15CX06051A)Financial support from Petro China Corporation Limited~~
文摘This paper reports a sustainable,water-assisted,solid-state method for synthesizing ammonium nickel molybdate((NH4)HNi2(OH)2(MoO4)2,ANM),a precursor for an unsupported hydrodesulfurization(HDS) catalyst.The associated ANM formation mechanism is also discussed.The synthesis route consists of physical mixing of the raw materials,water-assisted grinding and heating.The formation mechanism involves replacement of a Mo atom by a Ni atom,generating the metastable intermediate(NH4)4(NiH6Mo6O(24))·5H2O.Heating of this intermediate at 120 ℃ removes the added water and produces ANM.Catalysts prepared by this method exhibit almost the same physicochemical properties and catalytic performance during the HDS of dibenzothiophene as materials made from ANM synthesized by a chemical precipitation procedure.Compared with traditional hydrothermal or chemical precipitation methods,this water-assisted,solid-state synthesis provides several significant advantages,including simplifying the synthetic procedure,reducing waste and energy costs and increasing product yields.These features will be highly important with regard to allowing the application of ANM in industrial-scale processes involving HDS reactions.This water-assisted,solid-state strategy can also be extended to the synthesis of isomorphous compounds such as ammonium cobalt(zinc and copper) molybdate.
文摘Electron-hole separation is a critical step to achieving efficient photocatalysis, towards which use of co-catalysts has become a widely used strategy. Despite the tremendous efforts and demonstrated functions of noble metal co-catalysts, seeking noble metal-free co-catalysts will always be the goal when designing cost- effective, high-performance hybrid photocatalysts. In this work, we demonstrate that MoS~ nanosheets with 1T phase (i.e., octahedral phase) can function as a co-catalyst with multiple merits: (1) Noble-metal-free; (2) high mobility for charge transport; (3) high density of active sites for H2 evolution on basal planes; (4) good performance stability; (5) high light transparency. As demonstrated in both photocatalytic hydrogen production and Rhodamine B degradation, the developed hybrid structure with TiO2 exhibits excellent performance, in sharp contrast to bare TiO2 and the hybrid counterpart with 2H-MoS2.