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Abstract
We examined oxidative coupling of methane (OCM) over various Ce–W–O catalysts at 423 K in an electric field. Ce2(WO4)3/CeO2 catalyst showed high OCM activity. In a periodic operation test over Ce2(WO4)3/CeO2 catalyst, C2 selectivity exceeded 60% during three redox cycles. However, Ce2(WO4)3/CeO2 catalyst without the electric field showed low activity, even at 1073 K: CH4 Conv., 6.0%; C2 Sel., 2.1%. A synergetic effect between the Ce2(WO4)3 structure and electric field created the reactive oxygen species for selective oxidation of methane. Results of XAFS, in-situ Raman and periodic operation tests demonstrated that OCM occurred as the lattice oxygen in Ce2(WO4)3 (short W–O bonds in distorted WO4 unit) was consumed. The consumed oxygen was reproduced by a redox mechanism in the electric field.
Highlights
OCM occurred as the lattice oxygen in Ce2(WO4)[3] was consumed
We reported that OCM proceeded at a low temperature (423 K) in the electric field over Sr-La2O3 (Sr/La = 1/20) catalyst[11,12]
We evaluated the effects of an electric field on OCM activity over various catalysts including TBA-PW12O40/CeO2 catalyst (Supplementary Information Tables S2 and S3)
Summary
OCM occurred as the lattice oxygen in Ce2(WO4)[3] (short W–O bonds in distorted WO4 unit) was consumed. The state of natural gas, especially methane, at room temperature and atmospheric pressures is gaseous. To resolve the difficulties described above, we adopted a non-conventional catalytic system, a catalytic reaction in an electric field, in anticipation of methane activation at low temperatures. Results show that various low-temperature catalytic reactions such as methane steam reforming[6,7,8,9,10] can proceed in the electric field. We reported that OCM proceeded at a low temperature (423 K) in the electric field over Sr-La2O3 (Sr/La = 1/20) catalyst[11,12]. As described in this paper, we examined Ce–W–O system oxide catalysts, including Keggin-type heteropoly acids (HPAs) as catalysts, for improving OCM activity in the electric field. Moffat et al.[24,25,26,27] reported the partial oxidation of methane www.nature.com/scientificreports/
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