肖高1,
郭杰1,
刘明华1,
齐赛男1,
刘学虎2,
李军2,
华坚3,
王涛3,
李新4
1.福州大学环境与资源学院,福州 350108
2.中国人民解放军军事科学院防化研究院,北京 102205
3.四川大学轻纺与食品学院,成都 610065
4.成都国化环保科技有限公司,成都 610065
基金项目: 国家自然科学基金资助项目(21506036)
福建省自然科学基金资助项目(2017J01412)
福建省教育厅中青年教师教育科研项目(JA15099,JA14062)
中国人民解放军军事科学院防化研究院(823093)
福州大学国家级大学生创新训练计划项目(201610386021)
Effect of surface modification of coal based activated carbon on low temperature denitrification performance of rare-earth supported CeO2/AC
CHEN Wei1,,XIAO Gao1,
GUO Jie1,
LIU Minghua1,
QI Sainan1,
LIU Xuehu2,
LI Jun2,
HUA Jian3,
WANG Tao3,
LI Xin4
1.College of Environment and Resouces, Fuzhou University, Fuzhou 350108, China
2.Institute of Chemical Defense, Academy of Military Science of the Chinese People’s Liberation Army, Beijing 102205, China
3.College of Light Industry, Textile and Food Engineering, Sichuan University, Chengdu 610065, China
4.Chengdu Guohua Environmental Protection Technology Co.Ltd., Chengdu 610065, China
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摘要:以煤基活性炭(AC)为载体,在不同温度下分别采用空气热氧化和硝酸浸渍对其进行预氧化表面改性处理,然后将稀土金属Ce3+负载在预氧化改性后的活性炭载体上,经煅烧而制得改性CeO2/AC低温SCR脱硝剂。并采用N2等温吸附脱附测试、X 射线光电子能谱等表征手段考察了2种不同预氧化改性方式对基炭孔结构和表面物化性质的影响。同时研究了不同预氧化方式、稀土负载量、煅烧温度对脱硝剂的低温脱硝性能的影响。结果表明:空气热氧化预处理的AC相对于原炭而言,比表面积没有明显损失,且基炭表面官能团得到了明显丰富;而经硝酸氧化的活性炭,比表面积有明显下降。制备CeO2/AC低温脱硝剂的最佳工艺为:在350 ℃下,采用空气热氧化预处理,稀土负载量为5% (质量分数), 500 ℃ N2保护煅烧温度下,所得到的CeO2/AC脱硝剂具有最佳低温脱硝活性。该脱硝剂在脱硝温度为150 ℃即可达到100%的脱硝率。
关键词: 活性碳/
SCR脱硝剂/
稀土改性/
氧化
Abstract:This work presented the preparation process of modified activated carbon supported Ce3+ for SCR denitration. As the catalyst support, coal-based activated carbon was pretreated by two methods of thermal oxidation by air and wet chemical oxidation by dipping nitric acid. The pore structure and surface chemical properties of the modified activated carbon by different methods was investigated by N2 adsorption and X-ray photoelectron spectrometer (XPS). The results show that the BET surface of modified activated carbon by hot air presented no obvious loss and the surface functional groups of activated carbon was obviously enriched. However, the BET surface of modified activated carbon by dipping nitric acid showed significantly reduce. Moreover, we also discovered the optimum preparation process of Ce3+ supported modified activated carbon (CeO2/AC) as SCR denitration catalyst. When the temperature of hot air oxidation is 350 ℃, the loading amount of Ce is 5% (mass fraction) by dipping method, and the calcining temperature is 500 ℃ under the protection of nitrogen, the obtained denitration catalyst CeO2/AC has the optimum SCR catalytic activity and its denitration rate can reach 100% at 150 ℃.
Key words:activated carbon/
SCR denitration catalyst/
rare-earth modification/
oxidization.
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煤基活性炭表面改性对稀土负载型CeO2/AC低温脱硝性能的影响
陈薇1,,肖高1,
郭杰1,
刘明华1,
齐赛男1,
刘学虎2,
李军2,
华坚3,
王涛3,
李新4
1.福州大学环境与资源学院,福州 350108
2.中国人民解放军军事科学院防化研究院,北京 102205
3.四川大学轻纺与食品学院,成都 610065
4.成都国化环保科技有限公司,成都 610065
基金项目: 国家自然科学基金资助项目(21506036) 福建省自然科学基金资助项目(2017J01412) 福建省教育厅中青年教师教育科研项目(JA15099,JA14062) 中国人民解放军军事科学院防化研究院(823093) 福州大学国家级大学生创新训练计划项目(201610386021)
关键词: 活性碳/
SCR脱硝剂/
稀土改性/
氧化
摘要:以煤基活性炭(AC)为载体,在不同温度下分别采用空气热氧化和硝酸浸渍对其进行预氧化表面改性处理,然后将稀土金属Ce3+负载在预氧化改性后的活性炭载体上,经煅烧而制得改性CeO2/AC低温SCR脱硝剂。并采用N2等温吸附脱附测试、X 射线光电子能谱等表征手段考察了2种不同预氧化改性方式对基炭孔结构和表面物化性质的影响。同时研究了不同预氧化方式、稀土负载量、煅烧温度对脱硝剂的低温脱硝性能的影响。结果表明:空气热氧化预处理的AC相对于原炭而言,比表面积没有明显损失,且基炭表面官能团得到了明显丰富;而经硝酸氧化的活性炭,比表面积有明显下降。制备CeO2/AC低温脱硝剂的最佳工艺为:在350 ℃下,采用空气热氧化预处理,稀土负载量为5% (质量分数), 500 ℃ N2保护煅烧温度下,所得到的CeO2/AC脱硝剂具有最佳低温脱硝活性。该脱硝剂在脱硝温度为150 ℃即可达到100%的脱硝率。
English Abstract
Effect of surface modification of coal based activated carbon on low temperature denitrification performance of rare-earth supported CeO2/AC
CHEN Wei1,,XIAO Gao1,
GUO Jie1,
LIU Minghua1,
QI Sainan1,
LIU Xuehu2,
LI Jun2,
HUA Jian3,
WANG Tao3,
LI Xin4
1.College of Environment and Resouces, Fuzhou University, Fuzhou 350108, China
2.Institute of Chemical Defense, Academy of Military Science of the Chinese People’s Liberation Army, Beijing 102205, China
3.College of Light Industry, Textile and Food Engineering, Sichuan University, Chengdu 610065, China
4.Chengdu Guohua Environmental Protection Technology Co.Ltd., Chengdu 610065, China
Keywords: activated carbon/
SCR denitration catalyst/
rare-earth modification/
oxidization
Abstract:This work presented the preparation process of modified activated carbon supported Ce3+ for SCR denitration. As the catalyst support, coal-based activated carbon was pretreated by two methods of thermal oxidation by air and wet chemical oxidation by dipping nitric acid. The pore structure and surface chemical properties of the modified activated carbon by different methods was investigated by N2 adsorption and X-ray photoelectron spectrometer (XPS). The results show that the BET surface of modified activated carbon by hot air presented no obvious loss and the surface functional groups of activated carbon was obviously enriched. However, the BET surface of modified activated carbon by dipping nitric acid showed significantly reduce. Moreover, we also discovered the optimum preparation process of Ce3+ supported modified activated carbon (CeO2/AC) as SCR denitration catalyst. When the temperature of hot air oxidation is 350 ℃, the loading amount of Ce is 5% (mass fraction) by dipping method, and the calcining temperature is 500 ℃ under the protection of nitrogen, the obtained denitration catalyst CeO2/AC has the optimum SCR catalytic activity and its denitration rate can reach 100% at 150 ℃.