Abstract: The calcination process of the alumina industry usually produces nearly 10 000 mg/m3 CO in the flue gas during the combustion process due to low temperature or low excess air coefficient. Direct emissions not only causes energy waste but also causes harm to the local atmosphere. To explore the industrial application feasibility for catalytic elimination of CO from flue gas in alumina calcination, the manganese-cerium particulate industrial catalysts were prepared by co-precipitation method, and the pilot application study with flue gas volume of 1000 Nm3/h was carried out in an aluminum company of Shandong Province. The pilot test results showed that under the condition of low sulfur (<10 mg/m3), when the inlet temperature was 170℃, the CO removal rate was 80%~85%, and the removal rate was above 90% when the temperature was above 200℃. The catalyst was used in the pilot test to run continuously for 500 h at the inlet temperature of 190~200℃. It was found that there was no significant decrease in activity as a whole, indicating that the manganese-cerium catalyst had good stability in the purification of CO gas under actual working conditions. After 500 h of pilot-scale catalyst operation, the catalyst samples at different positions of the fixed bed were analyzed, and it was found that the catalyst performance at the flue gas inlet decreased slightly. The characterization results of typical samples such as XRD, TG, BET, SEM-EDS, and H2-TPR showed that the crystal diffraction peak of the catalyst sample at the flue gas inlet was enhanced, the specific surface area was decreased, and the sulfur deposition was increased, indicating that the local heating sintering and sulfur deposition were the main reasons for the partial deactivation of the catalyst.

Key words: CO removal, manganese-based catalyst, catalytic oxidation, pilot test

摘要： 氧化铝工业煅烧过程由于温度偏低或过量空气系数偏小，导致排放燃烧烟气含有约10 000 mg/m3的高浓度一氧化碳(CO)，不仅造成能源浪费，而且对局部大气环境造成污染。为探究锰铈基催化剂催化氧化脱除氧化铝煅烧烟气CO技术可行性，采用共沉淀法制备了锰铈颗粒体工业催化剂，并在山东某铝业公司进行了烟气量为1000 Nm3/h的中试应用研究。中试运行结果表明，在低硫条件下(<10 mg/m3)，当进气温度在170℃时，CO脱除率在80%~85%，而温度在200℃以上时，CO脱除率提升至90%以上；在190~200℃连续运行500 h后，整体CO脱除效率无明显下降。对反应器中不同位置催化剂进行取样分析，结果表明烟气入口处样品催化性能略有降低，典型样品XRD, TG, BET, SEM-EDS和H2-TPR等表征结果表明，烟气入口处催化剂样品晶体衍射峰增强、比表面积下降、硫沉积增多，表明局部升温烧结和硫沉积是造成催化剂部分失活的主要原因。

关键词: CO脱除, 锰基催化剂, 催化氧化, 中试