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Date of Publication:2015-01-01

Journal:催化学报

Volume:36

Issue:3

Page Number:274-282

ISSN No.:0253-9837

Abstract:The catalytic effect of H2 in the one‐step synthesis of ethylene glycol (EG) from methanol dehydro‐genation coupling reaction using dielectric barrier discharge (DBD) was studied by in‐situ optical emission spectroscopy and online chromatographic analysis. The influence of discharge frequency, methanol and H2 flow rates as well as reaction pressure was investigated systematically. Results show that, in the non‐equilibrium plasma produced by DBD, H2 dramatically improved not only the conversion of methanol but also the selectivity for EG. Using the reaction conditions of 300 °C, 0.1 MPa, input power 11 W, discharge frequency 12.0 kHz, methanol gas flow rate 11.0 mL/min, and H2 flow rate 80–180 mL/min, the reaction of the CH3OH/H2 DBD plasma gave a methanol conversion close to 30%and a selectivity for EG of more than 75%. The change of the EG yield correlated with the intensity of the Hαspectral line. H atoms appear to be the catalytically active species in the reac‐tion. In the DBD plasma, the stable ground state H2 molecule undergoes cumulative collision excita‐tion with electrons before transitioning from higher energy excited states to the first excited state. The spontaneous dissociation of the first excited state H2 molecules generates the catalytically ac‐tive H atom. The discharge reaction condition affects the catalytic performance of H2 by influencing the dissociation of H2 molecules into H atoms. The catalytic effect of H2 exhibited in the non‐equilibrium plasma may be a new opportunity for the synthesis of chemicals.

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