球形氧化铝负载Ni-Co双金属催化剂上沼气重整制氢——操作条件的影响  

Biogas reforming for hydrogen production over Ni-Co bimetallic catalyst supported on spherical Al_2O_3——Effect of operating conditions

作　　者：李兆静[1,2] 周伟[2,3] 徐军科[2,4] 汪吉辉[1,2] 马建新[2,3] 

机构地区：[1]华东理工大学资源与环境工程学院,上海200237 [2]同济大学新能源汽车工程中心,上海201804 [3]同济大学汽车学院,上海201804 [4]同济大学环境科学与工程学院,上海200092

出　　处：《环境工程学报》2010年第12期2827-2832,共6页Chinese Journal of Environmental Engineering

基　　金：科技部国际合作重点项目(2007DFC61690);同济大学汉高基金教席(081591)

摘　　要：前期研究开发出了活性、稳定性和抗积碳性能都较好的沼气重整制氢Ni-Co/La2O3-Al2O3催化剂。在此基础上选用商业球形氧化铝作为载体（4~5 mm）并掺杂La2O3,用浸渍法制备了Ni-Co/La2O3-Al2O3球形催化剂,以CH4/CO2体积比为1的混合气模拟沼气,考察了操作条件对工业尺度催化剂沼气重整反应性能的影响。结果表明：负载活性组分的γ-Al2O3球形催化剂的沼气重整活性基本达到小试的水平。反应温度升高有利于提高催化剂的重整活性,850℃以上催化剂的活性趋于稳定。反应温度升高有利于减少催化剂的表面积碳,却加速了金属颗粒的团聚。随着空速的增加,催化剂的活性显著降低。较好的催化剂还原方式为用纯H2在700℃下还原2 h,用该方式还原的催化剂反应后金属粒径较小,平均积碳速率较低。Ni-Co/La2O3-Al2O3 catalyst of biogas reforming with better activity,stability and resistance to carbon deposition was developed in our previous work.In present paper,commercial Al2O3 pellets（4~5 mm） were selected as support and doped with La2O3.The spherical Ni-Co/La2O3-Al2O3 catalyst was prepared by conventional wetness incipient impregnation.Effect of operating conditions on the performance of the industrial scale catalyst was investigated,feeding with CH4/CO2 volume ratio of 1,which was similar with the composition of biogas.The results showed that low activity of biogas reforming was observed over commercial γ-Al2O3 pellet but very high activity over the spherical Ni-Co/La2O3-Al2O3 catalyst in the laboratory scale.Higher reaction temperature was beneficial to increase catalytic activity of reforming,but the increasing trend was slow above 800℃.Metal particles tended to aggregate and the deposition of carbon was suppressed at higher reaction temperature.Catalytic activity decreased with the increasing of gas hourly space velocity（GHSV）.It was proved that the catalyst reduced at 700℃ for 2 h in pure H2 flow showed smaller metal particle size and lower average coking rate.

关 键 词：沼气重整 制氢 球形氧化铝 镍钴双金属 操作条件 

分 类 号：X701.7[环境科学与工程—环境工程]