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Thermocatalytic nonoxidative ethane dehydrogenation (EDH) is a promising strategy for ethene production but suffers from intense energy consumption and poor catalyst durability; exploring technology that permits efficient EDH by solar energy remains a giant challenge. Herein, we present that an oxygen vacancy (Ov)-rich LaVO4 (LaVO4-Ov) catalyst is highly active and stable for photocatalytic EDH, through a dynamic lattice oxygen (Olatt.) and Ov co-mediated mechanism. Irradiated by simulated sunlight at mild conditions, LaVO4-Ov effectively dehydrogenates undiluted ethane to produce C2H4 and CO with a conversion of 2.3%. By loading a small amount of Pt cocatalyst, the evolution and selectivity of C2H4 are enhanced to 275 mu mol h-1 g-1 and 96.8%. Of note, LaVO4-Ov appears nearly no carbon deposition after the reaction. The isotope tracked reactions reveal that the consumed Olatt. recuperates by exposing the used catalyst with O2, thus establishing a dynamic cycle of Olatt. and achieving a facile catalyst regeneration to preserve its intrinsic activity. The refreshed LaVO4-Ov exhibits superior reusability and delivers a turnover number of about 305. The Ov promotes photo absorption, boosts ethane adsorption/activation, and accelerates charge separation/transfer, thus improving the photocatalytic efficiency. The possible photocatalytic EDH mechanism is proposed, considering the key intermediates predicted by density functional theory (DFT) and monitored by in-situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS).(c) 2023 Published by Elsevier B.V. on behalf of Chinese Chemical Society and Institute of Materia Medica, Chinese Academy of Medical Sciences.
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CHINESE CHEMICAL LETTERS
ISSN: 1001-8417
CN: 11-2710/O6
Year: 2023
Issue: 3
Volume: 35
9 . 4
JCR@2023
9 . 4 0 0
JCR@2023
JCR Journal Grade:1
CAS Journal Grade:2
Cited Count:
WoS CC Cited Count: 11
SCOPUS Cited Count: 13
ESI Highly Cited Papers on the List: 0 Unfold All
WanFang Cited Count:
Chinese Cited Count:
30 Days PV: 0
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