SCS法制备Co_(3)O_(4)催化氧化低浓度甲烷  

Catalytic Oxidation of Low Concentration Methane by Co_(3)O_(4)Prepared via SCS Method

作　　者：费轲 阳昌真 赵梦奇[1,3] 张亚新 郭皓[1,3] 廖银念 FEI Ke;YANG Changzhen;ZHAO Mengqi;ZHANG Yaxin;GUO Hao;LIAO Yinnian(School of Chemical Engineering and Technology,Xinjiang University,Urumqi 830017,China;School of Applied Chemistry and Materials,Zhuhai College of Science and Technology,Zhuhai 519041,China;Xinjiang Key Laboratory of Clean Coal Conversion&Chemical Engineering Process,Urumqi 830017,China)

机构地区：[1]新疆大学化工学院,新疆乌鲁木齐830017 [2]珠海科技学院应用化学与材料学院,广东珠海519041 [3]新疆煤炭清洁转化与化工过程自治区重点实验室,新疆乌鲁木齐830017

出　　处：《环境科学与技术》2023年第10期121-128,共8页Environmental Science & Technology

基　　金：新疆维吾尔自治区自然科学基金面上项目(2020D01C021);国家自然科学基金-新疆联合基金培育项目(U2003123);广东省普通高校重点科研平台和项目重点专项项目(2022ZDZX3039);广东省重点建设学科科研能力提升项目(2022ZDJS141)。

摘　　要：前驱物中氧化剂(硝酸钴)/燃料(柠檬酸)配比对溶液燃烧法制备的Co_(3)O_(4)催化氧化低浓度甲烷性能的影响极大。随着燃料占比的增多,Co_(3)O_(4)的比表面积逐渐增大,氧化还原性能逐渐增强。其中当氧化剂/燃料比为1∶2时所得的Co3O(4命名为Co1CA2)具有最小的晶体尺寸、较高的比表面积。此外,该催化剂不仅具有较好的氧化还原能力,同时表面有更丰富的Co^(2+)以及吸附氧物种,并且此时的Co-O键更容易断裂,意味着可以提供更多的活性氧物种。在低浓度甲烷的催化氧化测试中,Co1CA2表现出了最好的催化活性,其T90值为370℃,相较于直接煅烧硝酸钴得到的Co_(3)O_(4)降低68℃。在经过3次非连续的稳定性测试后,Co1CA2对甲烷的去除率仍旧稳定在90%以上,表现出良好的耐性。The ratio of oxidant(cobalt nitrate)to fuel(citric acid)in the precursor could exert great influence on the catalytic oxidation of low concentration methane of Co_(3)O_(4),which was prepared by solution combustion synthesis.With the increasing of fuel proportion,the specific surface area of Co_(3)O_(4)and the catalytic performance gradually increased.Among all of the obtained Co_(3)O_(4)samples,the one obtained by setting the oxidant/fuel ratio to be 1∶2(named as Co1CA2)showed the smallest crystal size and higher specific surface area.In addition,the Co1CA2 displayed not only better reducibility,but also a richer surface of Co^(2+)and Oads,and the Co-O bond in this catalyst is more likely to break,which means more reactive oxygen species can be provided and thus would bring benefit to the catalytic activity of Co_(3)O_(4)during the methane oxidation.Therefore,in the catalytic oxidation of low concentrations of methane,Co1CA2 performed the highest catalytic activity with a T90 value of 370℃,which is 68℃lower than the Co_(3)O_(4)obtained by calcining oxidant directly.After three discontinuous stability tests,the removal rate of methane by Co1CA2 was still above 90%,showing good water resistance,repeatability,and durability.

关 键 词：氧化剂/燃料配比 溶液燃烧法 Co_(3)O_(4) 催化氧化 低浓度甲烷 

分 类 号：X701[环境科学与工程—环境工程]