摘要
通过对CH4低温活化与CO2 加氢研究成果的分析 ,提出了在CO2 加氢催化剂上CH4表面吸附物种与CO2低温转化直接合成含氧化合物的可行性 ,并进行了热力学分析和实验验证 .实验结果表明 ,CH4表面吸附物种与CO2 在Cu Co基催化剂表面相互作用能生成醇、醛、酸、酮和两种环戊烷衍生物Ⅰ和Ⅱ ,产物分布随进料方式而有很大的变化 ,但无论哪种方式都有乙酸和环戊烷衍生物Ⅰ生成 .就乙酸收率而言 ,最佳反应条件为T =5 2 3K ,n(Cu) /n(Co) =5 .FT IR测试结果表明 ,反应后催化剂表面有CHx 和CHxO生成 .
The feasibility of direct conversion of CH4 and CO2 to oxygenated compounds by means of a two-step reaction sequence at low temperature was suggested. The thermodynamics of isothermal and nonisothermal two-step reaction was analyzed. The reactivity of CH4 adsorbed and CO2 was investigated with temperature programming surface reaction (TPSR) from 323 to 873 K and with a continuous fixed-bed flow micro-reactor from 443 to 573 K at normal pressure. The product was analyzed by means of GC-MS and IC. The preliminary experiment results showed that the interaction of CH4 adsorbed and CO2 over Cu-Co based catalysts can produce various kinds of compounds such as. alcohol, aldehyde, ketone, carboxylic acid and cyclopentane derivatives I and II. The product composition and distribution depend greatly on feeding methods, but the acetic acid and cyclopentane derivative I are always produced for the three kinds of feeding methods studied in this paper. The optimum temperature is 523 K and the Cu/Co molar ratio is 5 for acetic acid production. The FT-IR measurement results showed the formation of CHx and CHxO over the catalyst samples.
出处
《催化学报》
SCIE
EI
CAS
CSCD
北大核心
2001年第4期321-325,共5页
基金
山西省自然科学基金 ( 9610 13)
山西省归国留学基金资助项目
