高等学校化学学报
高等學校化學學報
고등학교화학학보
CHEMICAL JOURNAL OF CHINESE UNIVERSITIES
2014年
12期
2598-2604
,共7页
张叶%周佳佳%吴贵升%毛东森%卢冠忠
張葉%週佳佳%吳貴升%毛東森%盧冠忠
장협%주가가%오귀승%모동삼%로관충
甲醛催化氧化%四氧化三钴%甲酸盐%程序升温脱附%原位漫反射红外光谱%表面氧
甲醛催化氧化%四氧化三鈷%甲痠鹽%程序升溫脫附%原位漫反射紅外光譜%錶麵氧
갑철최화양화%사양화삼고%갑산염%정서승온탈부%원위만반사홍외광보%표면양
Formaldehyde catalytic oxidation%Co3 O4%Formate%Temperature programmed desorption%In situ diffuse reflectance infrared Fourier transform spectroscopy%Surface oxygen species
采用沉淀法制备了Co3 O4催化剂,并将催化剂在流动的N2或O2气氛中于不同温度下进行预处理。通过X射线衍射( XRD)、热重-差示扫描量热分析( TG-DSC)、程序升温脱附( O2/CO2-TPD, HCHO-TPSR)和原位漫反射傅里叶变换红外光谱( in situ DRIFTS)等手段对催化剂表面物种进行了表征。结果表明, Co3 O4-N2-200催化剂表面存在Co3+不饱和配位中心和丰富的弱配位氧负离子,容易形成双配位的甲酸盐,并转化成单配位的甲酸盐,进一步分解为产物。
採用沉澱法製備瞭Co3 O4催化劑,併將催化劑在流動的N2或O2氣氛中于不同溫度下進行預處理。通過X射線衍射( XRD)、熱重-差示掃描量熱分析( TG-DSC)、程序升溫脫附( O2/CO2-TPD, HCHO-TPSR)和原位漫反射傅裏葉變換紅外光譜( in situ DRIFTS)等手段對催化劑錶麵物種進行瞭錶徵。結果錶明, Co3 O4-N2-200催化劑錶麵存在Co3+不飽和配位中心和豐富的弱配位氧負離子,容易形成雙配位的甲痠鹽,併轉化成單配位的甲痠鹽,進一步分解為產物。
채용침정법제비료Co3 O4최화제,병장최화제재류동적N2혹O2기분중우불동온도하진행예처리。통과X사선연사( XRD)、열중-차시소묘량열분석( TG-DSC)、정서승온탈부( O2/CO2-TPD, HCHO-TPSR)화원위만반사부리협변환홍외광보( in situ DRIFTS)등수단대최화제표면물충진행료표정。결과표명, Co3 O4-N2-200최화제표면존재Co3+불포화배위중심화봉부적약배위양부리자,용역형성쌍배위적갑산염,병전화성단배위적갑산염,진일보분해위산물。
The Co3 O4 catalysts were prepared via precipitation methods, and then were pretreated in N2 or O2 at different temperatures. Based on the study of formaldehyde catalytic oxidation, the catalytic performances were investigated with the detailed surface characterization via temperature programmed desorption ( O2/CO2-TPD, HCHO-TPSR) , thermogravimetric-differential scanning calorimetry( TG-DSC) and in situ diffuse reflec-tance infrared fourier transform spectroscopy ( in situ DRIFTS ) . The results presented that Co3 O4-N2-200 showed the optimal catalytic performance, because there were rich unsaturated coordination centers of Co3+and negative oxygen ions with weak bond strength on the surface of Co3 O4-N2-200, which was ready to adsorb formaldehyde to form bidentate formate, and then decompose to products via monodentate formate. With increasing pretreatment temperature, the amount of negative oxygen ions decreased, accordingly the catalytic activity for formaldehyde catalytic oxidation decreased due to slow decomposition rate of desorbed bidentate formate.