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Active catalyst construction for CO₂ recycling via catalytic synthesis of N-doped carbon on supported Cu.

ABSTRACT: Bridging homogeneous and heterogeneous catalysis is a long-term pursuit in the field of catalysis. Herein, we report our results in integration of nano- and molecular catalysis via catalytic synthesis of nitrogen doped carbon layers on AlOx supported nano-Cu which can finely tune the catalytic performance of the supported copper catalyst. This synthetic catalytic material, which can be generated in situ by the reaction of CuAlOx and 1,10-Phen in the presence of hydrogen, could be used for controllable synthesis of N,N-dimethylformamide (DMF) from dimethylamine and CO₂/H₂ via blocking reaction pathways of further catalytic hydrogenation of DMF to N(CH₃)₃. Detailed characterizations and DFT calculations reveal that the presence of N-doped layered carbon on the surface of the nano-Cu particles results in higher activation energy barriers during the conversion of DMF to N(CH₃)₃. Our primary results could promote merging of homogeneous catalysis and heterogeneous catalysis and CO₂ recycling.

SUBMITTER: Wu Y

PROVIDER: S-EPMC6565717 | biostudies-literature | 2019 Jun

REPOSITORIES: biostudies-literature

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Active catalyst construction for CO<sub>2</sub> recycling via catalytic synthesis of N-doped carbon on supported Cu.

Wu Yajuan Y Wang Tao T Wang Hongli H Wang Xinzhi X Dai Xingchao X Shi Feng F

Nature communications 20190613 1

Bridging homogeneous and heterogeneous catalysis is a long-term pursuit in the field of catalysis. Herein, we report our results in integration of nano- and molecular catalysis via catalytic synthesis of nitrogen doped carbon layers on AlOx supported nano-Cu which can finely tune the catalytic performance of the supported copper catalyst. This synthetic catalytic material, which can be generated in situ by the reaction of CuAlOx and 1,10-Phen in the presence of hydrogen, could be used for contro ...[more]

PMID: 31197203

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Project description:Nitrogen-doped activated carbon (N-AC) obtained through the thermal treatment of a mixture of HNO₃-pretreated activated carbon (AC) and urea under N₂ atmosphere at 600 °C was used as the carrier of Pd catalyst for both liquid-phase hydrodechlorination of 2,4-dichlorophenol (2,4-DCP) and gas-phase hydrodechlorination of chloropentafluoroethane (R-115). The effects of nitrogen doping on the dispersion and stability of Pd, atomic ratio of Pd/Pd2+ on the surface of the catalyzer, the catalyst's hydrodechlorination activity, as well as the stability of N species in two different reaction systems were investigated. Our results suggest that, despite no improvement in the dispersion of Pd, nitrogen doping may significantly raise the atomic ratio of Pd/Pd2+ on the catalyst surface, with a value of 1.2 on Pd/AC but 2.2 on Pd/N-AC. Three types of N species, namely graphitic, pyridinic, and pyrrolic nitrogen, were observed on the surface of Pd/N-AC, and graphitic nitrogen was stable in both liquid-phase hydrodechlorination of 2,4-DCP and gas-phase hydrodechlorination of R-115, with pyridinic and pyrrolic nitrogen being unstable during gas-phase hydrodechlorination of R-115. As a result, the average size of Pd nanocrystals on Pd/N-AC was almost kept unchanged after liquid-phase hydrodechlorination of 2,4-DCP, whereas crystal growth of Pd was clearly observed on Pd/N-AC after gas-phase hydrodechlorination of R-115. The activity test revealed that Pd/N-AC exhibited a much better performance than Pd/AC in liquid-phase hydrodechlorination of 2,4-DCP, probably due to the enhanced stability of Pd exposed to the environment resulting from nitrogen doping as suggested by the higher atomic ratio of Pd/Pd2+ on the catalyst surface. In the gas-phase hydrodechlorination of R-115, however, a more rapid deactivation phenomenon occurred on Pd/N-AC than on Pd/AC despite a higher activity initially observed on Pd/N-AC, hinting that the stability of pyridinic and pyrrolic nitrogen plays an important role in the determination of catalytic performance of Pd/N-AC.

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Active catalyst construction for CO₂ recycling via catalytic synthesis of N-doped carbon on supported Cu.

Publications

Active catalyst construction for CO<sub>2</sub> recycling via catalytic synthesis of N-doped carbon on supported Cu.

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Active catalyst construction for CO2 recycling via catalytic synthesis of N-doped carbon on supported Cu.

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Active catalyst construction for CO<sub>2</sub> recycling via catalytic synthesis of N-doped carbon on supported Cu.

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OmicsDI is part of the ELIXIR infrastructure

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Active catalyst construction for CO₂ recycling via catalytic synthesis of N-doped carbon on supported Cu.