醋酸钯和四氯对苯醌催化氧化低浓度煤矿瓦斯制甲醇.pdf

第44卷第2期
燃料化学学报
Vol 44 No
2016年2月
Journal of Fuel Chemistry and Technology
Feb.2016
文章编号:0253-2409(2016)02-0239-05
Pd (OAC)> and chloranil-catalyzed oxidation of low-concentration coal
mine gases to methanol
XU Feng", LI Chuang, JIA Shao-yang, WU Yang, ZHU Li-hua
College of Safety Engineering, Heilongiang University of Science and Technology, Harbin 150022, China)
Abstract: A self-made experimental system was used to study the catalytic oxidation of low-concentration coal mine gases to
methanol in acetic acid solution. With Pd(OAC) as catalyst, addition of p-benzoquinone or chloranil in the reaction system
rovides a beneficial environment for activation of methane, and chloranil show a more positive effect. Chlorani amount and
reaction temperature and pressure are the key factors influencing the catalytic propertics. The target product yicld has a positiv
relationship with these three factors. CH, OH is formed from the reaction of generated H2 O2 and CH. CH, COOCH, is generated via
two routes: one is direct oxidation of Pd and CH,, the other is esterification of CH OH and CH COOH
Keywords: palladium acetate; chloranil; mine gases; methano
Although mine gases, as one of coal accessories
Micha]kiewicz e/ a)Ila) With the biological oxidation
may cause destructive disaster for coal mines and knowledge, An et al proposed an electron-transfer
clean energy and manufacture chemicais: 13)ve
evere air pollution, they can be used to serve as loop with Pd""as active site for oxidation of methane
in CF COOH. In this way, methane was selectively
mine gases explosion accident is often avoided by oxidized to methanol at 80C and 5. 5 Mpa. Yuan et
enhancing their extraction. However, this makes the al
ld that methane can also be selectively
extracted mine gases with low concentration of CH(< oxidized to methanol in CF; COOH with Pd( OAC)?/
30%), thus, majority of which are directly benzoquinone/H; PMO Ou as catalyst. Xu et
discharged into air due to lack of economic utilization
17-20
preliminarily studied the liquid-phase
technology. This not only le
oxidation of methane or mine
to methanol over
pollution, but also waste significant amounts of Pd(OAC )2 or Pd-cupc/Y catalyst in CH; COOH
carbon resource
Therefore, it is necessary and solution. However, the above studies center on the
important to utilize these low-concentration mine conversion of pure methane or mine gases with higl
gases. An interesting approach is to convert them into concentration of methane. Liquid-phase catalytic
methanol by liquid-phase catalytic oxidation . oxidation of mine gases having low content of
siquid-phase catalytic oxidation allows the reaction to methane has not been reported yet. Thus, catalytic
be conducted under mild conditions by means o
oxidation of mine gases with low concentration o
solvation. It has been shown that noble metal methane (20%, volume ratio) to methanol over
catalysts, such as Pt, Pd and Rh, give high methane palladium acetate and chloranil are studied here
conversion in acidic medium 6-1] Mukhopadhyay et
al synthesized CH, SO, H by reacting SO and CH
1 Materials and methods
in H2 SO solution in the presence of Pdcl, -Cucl2
1. 1 Materials
catalyst. Periana et al obtained a high yield
The model m