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Plasmonic Heating-Promoted Photothermal Synthesis of α-Cyanoacrylonitriles Over Au/h-BN Catalysts.

ABSTRACT: Plasmonic nanoparticle-involved materials play an essential role in the field of photothermal conversion. Herein, we report the application of photothermal heterogeneous catalysts consisting of gold nanoparticles decorated on defect-rich h-BN sheets (Au/h-BN) for the photocatalytic synthesis of α-cyanoacrylonitriles under mild conditions. It has been demonstrated the-NH₂ groups present in the defect-rich h-BN act as the catalytically active sites, while plasmonic heating from the gold nanoparticles can drive the reaction by providing local heat. Au/h-BN catalyst can work for a broad substrate scope in the synthesis of α-cyanoacrylonitriles, and a plausible -NH₂ group-involved reaction mechanism has been proposed. This work may open up new avenues in photothermal catalysis by combining plasmonic materials and catalytic sites in one system.

SUBMITTER: Liang C

PROVIDER: S-EPMC8455885 | biostudies-literature | 2021

REPOSITORIES: biostudies-literature

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Plasmonic Heating-Promoted Photothermal Synthesis of α-Cyanoacrylonitriles Over Au/h-BN Catalysts.

Liang Ce C Zhang Yuanyuan Y Zhang Bin B Liu Xin-Miao XM Gao Guo-Lin GL Cao Jingyan J Xu Ping P

Frontiers in chemistry 20210908

Plasmonic nanoparticle-involved materials play an essential role in the field of photothermal conversion. Herein, we report the application of photothermal heterogeneous catalysts consisting of gold nanoparticles decorated on defect-rich h-BN sheets (Au/h-BN) for the photocatalytic synthesis of α-cyanoacrylonitriles under mild conditions. It has been demonstrated the-NH<sub>2</sub> groups present in the defect-rich h-BN act as the catalytically active sites, while plasmonic heating from the gold ...[more]

PMID: 34568280

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Project description:The production of linear alpha-olefins (α-olefins) is a practical way to increase the economic potential of the Fischer-Tropsch synthesis (FTS) because of their importance as chemical intermediates. Our study aimed to optimize Na-promoted Fe1Zn1.2O x catalysts such that they selectively converted syngas to linear α-olefins via FTS at 340 °C and 2.0 MPa. The Fe1Zn1.2O x catalysts were calcined at different temperatures from 350 to 700 °C before Na anchoring. The increase in the size of the ZnFe2O4 crystals comprising the catalyst had a negative effect on the reducibility of Fe oxides and the particle size of Fe5C2 during the reaction. The Na species in the catalyst restrained the reduction of Fe1Zn1.2O x but facilitated the formation of Fe5C2. When pure Fe1Zn1.2O x was calcined at 400 °C, the corresponding catalyst (i.e., Na0.2/Fe1Zn1.2O x (400)) exhibited higher catalytic activity and stability than the other catalysts for a 50 h reaction. Compared to the other catalysts, Na0.2/Fe1Zn1.2O x (400) enabled a higher number of active Fe carbides (Fe5C2) to intimately interact with the Na species, even though the catalyst had a lower total surface basicity based on surface area. The Na0.2/Fe1Zn1.2O x (400) showed a maximum hydrocarbon yield of 49.7% with a maximum olefin selectivity of 61.3% in the C1-C32 range. Examination of the reaction product mixture revealed that the Na0.2/Fe1Zn1.2O x catalysts converted α-olefins to branched paraffins (13.9-19.5%) via a series of isomerization, skeletal isomerization, and hydrogenation reactions. The Na0.2/Fe1Zn1.2O x (400) catalyst had a relatively low consumption rate of internal olefins compared to other catalysts, resulting in the lowest selectivity for branched paraffins. The Na0.2/Fe1Zn1.2O x (400) showed a maximum α-olefin yield (26.6%) in the range C2-C32, which was 27.9-50.0% higher than that of other catalysts. The α-olefin selectivity in the C5-C12 range for the Na0.2/Fe1Zn1.2O x (400) was 37.5% relative to the total α-olefins.

Dataset Information

Plasmonic Heating-Promoted Photothermal Synthesis of α-Cyanoacrylonitriles Over Au/h-BN Catalysts.

Publications

Plasmonic Heating-Promoted Photothermal Synthesis of α-Cyanoacrylonitriles Over Au/h-BN Catalysts.

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