Methanol-to-olefins(MTO)process is one of the most critical pathways to produce low carbon olefins.Typically,the reaction is driven by thermal catalysis,which inevitably needs to consume large amounts of fossil fuel.D...Methanol-to-olefins(MTO)process is one of the most critical pathways to produce low carbon olefins.Typically,the reaction is driven by thermal catalysis,which inevitably needs to consume large amounts of fossil fuel.Developing a new technique to substitute for the fuel burning is urgent for MTO process to improve the industry prospects and sustainability.Herein,we report a novel W_(18)O_(49)/Au/SAPO-34(W/Au/S),a multifunctional photothermal catalyst for the MTO reaction.A high methanol conversion was achieved under xenonum(Xe)lamp irradiation,yielding methyl ether(ME)and ethylene as the main products.The optimized W/Au/S catalysts showed ethylene yield as high as 250μmol in 60 min,which was 2.5 times higher than that of Au/SAPO-34.The physiochemical characterization revealed that the SAPO-34 molecular sieves were surrounded by Au and W_(18)O_(49)nanoparticles,which exhibited a strong localized surface plasmon resonance excitation around 540 nm and light absorption beyond 500 nm.The multifunctional catalysts showed a strong photothermal effect,arising from the broadened light absorption of Au and W_(18)O_(49)nanoparticles,leading to a temperature as high as 250℃on the surface of the catalysts.Mechanism study showed that the superior ethylene selectivity of W/Au/S catalysts was attributed to the moderating acidic sites of W_(18)O_(49)for methanol dehydration to ethylene.This research may provide new insight for designing heterostructures to improve photo-to-chemical conversion performance and is expected to accelerate progress toward the excellent multifunctional photothermal catalysts with broad light absorption for methanol activation and C-C bond formation.展开更多
基金financially supported by the High-level Innovative Talent Cultivation Project of Guizhou Province(No.GZSQCC2019003)the Natural Science Research Project of Guizhou Provincial Department of Education(No.QJHKY Zi[2021]257)the Academic New Seedling Cultivation and Innovation Exploration Project of Guizhou Institute of Technology(No.GZLGXM-08)。
文摘Methanol-to-olefins(MTO)process is one of the most critical pathways to produce low carbon olefins.Typically,the reaction is driven by thermal catalysis,which inevitably needs to consume large amounts of fossil fuel.Developing a new technique to substitute for the fuel burning is urgent for MTO process to improve the industry prospects and sustainability.Herein,we report a novel W_(18)O_(49)/Au/SAPO-34(W/Au/S),a multifunctional photothermal catalyst for the MTO reaction.A high methanol conversion was achieved under xenonum(Xe)lamp irradiation,yielding methyl ether(ME)and ethylene as the main products.The optimized W/Au/S catalysts showed ethylene yield as high as 250μmol in 60 min,which was 2.5 times higher than that of Au/SAPO-34.The physiochemical characterization revealed that the SAPO-34 molecular sieves were surrounded by Au and W_(18)O_(49)nanoparticles,which exhibited a strong localized surface plasmon resonance excitation around 540 nm and light absorption beyond 500 nm.The multifunctional catalysts showed a strong photothermal effect,arising from the broadened light absorption of Au and W_(18)O_(49)nanoparticles,leading to a temperature as high as 250℃on the surface of the catalysts.Mechanism study showed that the superior ethylene selectivity of W/Au/S catalysts was attributed to the moderating acidic sites of W_(18)O_(49)for methanol dehydration to ethylene.This research may provide new insight for designing heterostructures to improve photo-to-chemical conversion performance and is expected to accelerate progress toward the excellent multifunctional photothermal catalysts with broad light absorption for methanol activation and C-C bond formation.
