Cu-Fe composite oxides were prepared by co-precipitation method and tested for higher alcohol synthesis from syngas. The selectivity to C2＋OH and C6＋OH in alcohol distribution was very high while the methane product...Cu-Fe composite oxides were prepared by co-precipitation method and tested for higher alcohol synthesis from syngas. The selectivity to C2＋OH and C6＋OH in alcohol distribution was very high while the methane product fraction in hydrocarbon distribution was rather low, demonstrating a promising potential in higher alcohols synthesis from syngas. The distribution of alcohols and hydrocarbons approximately obeyed Anderson-Schulz-Flory distribution with similar chain growth probability, indicating alcohols and hydrocarbons derived from the same intermediates. The effects of Cu/Fe molar ratio, reaction temperature and gas hourly space velocity （GHSV） on catalytic performance were studied in detail. The sample with a Cu/Fe molar ratio of 10/1 exhibited the best catalytic performance. Higher reaction temperature accelerated water-gas-shift reaction and led to lower total alcohols selectivity. GHSV showed great effect on catalytic performance and higher GHSV increased the total alcohol selectivity, indicating there existed visible dehydration reaction of alcohol into hydrocarbon.展开更多
Boron-based metal-free catalysts for oxidative dehydrogenation of propane(ODHP)have drawn great attention in both academia and industry due to their impressive activity and olefin selectivity.Herein,the SiO2 and B2O3 ...Boron-based metal-free catalysts for oxidative dehydrogenation of propane(ODHP)have drawn great attention in both academia and industry due to their impressive activity and olefin selectivity.Herein,the SiO2 and B2O3 sequentially coated honeycomb cordierite catalyst is designed by a two-step wash-coat method with different B2O3 loadings(0.1%–10%)and calcination temperatures(600,700,800℃).SiO2 obtained by TEOS hydrolysis acts as a media layer to bridge the cordierite substrate and boron oxide via abundant Si\\OH groups.The welldeveloped straight channels of honeycomb cordierite make it possible to carry out the reactor under high gas hourly space velocity(GHSV)and the thin wash-coated B2O3 layer can effectively facilitate the pore diffusion on the catalyst.The prepared B2O3/SiO2@HC monolithic catalyst exhibits good catalytic performance at low boron oxide loading and achieves excellent propylene selectivity(86.0%),olefin selectivity(97.6%,propylene and ethylene)and negligible CO2(0.1%)at 16.9%propane conversion under high GHSV of 345,600 ml·(g B2O3)^-1·h^-1,leading to a high propylene space time yield of 15.7 g C3H6·(g B2O3)^-1·h^-1 by suppressing the overoxidation.The obtained results strongly indicate that the boron-based monolithic catalyst can be properly fabricated to warrant the high activity and high throughput with its high gas/surface ratio and straight channels.展开更多
利用溶胶-凝胶法制备Mn-Ce-O_x催化剂,考察了锰铈摩尔比和焙烧温度对催化剂催化氧化NO活性的影响,并对空速和稳定性进行了探究。结果表明,锰铈摩尔比为1,焙烧温度为300℃和400℃时,催化剂的NO氧化活性最佳。不同焙烧温度的催化剂中,400...利用溶胶-凝胶法制备Mn-Ce-O_x催化剂,考察了锰铈摩尔比和焙烧温度对催化剂催化氧化NO活性的影响,并对空速和稳定性进行了探究。结果表明,锰铈摩尔比为1,焙烧温度为300℃和400℃时,催化剂的NO氧化活性最佳。不同焙烧温度的催化剂中,400℃焙烧,催化剂呈片状结构,比表面积最大,可达113.8 m^2/g;其具有良好的稳定性,在NO体积分数为600μL/L,O_2的体积分数为4%,N2作平衡气,空速为480 000 m L/(g·h),反应温度为260℃时,NO催化氧化活性最高可达89%;进一步增大空速至960 000 m L/(g·h),相同反应条件下,NO催化活性最高可达69%。展开更多
基金the State Key Fundamental Research Program(Ministry of Science and Technology of China,No.2011CBA00501)Shanghai Municipal Science and Technology Commission,China(Grant No:11DZ1200300)the Foundation of State Key Laboratory of Coal Conversion(Grant No:1112610)
文摘Cu-Fe composite oxides were prepared by co-precipitation method and tested for higher alcohol synthesis from syngas. The selectivity to C2＋OH and C6＋OH in alcohol distribution was very high while the methane product fraction in hydrocarbon distribution was rather low, demonstrating a promising potential in higher alcohols synthesis from syngas. The distribution of alcohols and hydrocarbons approximately obeyed Anderson-Schulz-Flory distribution with similar chain growth probability, indicating alcohols and hydrocarbons derived from the same intermediates. The effects of Cu/Fe molar ratio, reaction temperature and gas hourly space velocity （GHSV） on catalytic performance were studied in detail. The sample with a Cu/Fe molar ratio of 10/1 exhibited the best catalytic performance. Higher reaction temperature accelerated water-gas-shift reaction and led to lower total alcohols selectivity. GHSV showed great effect on catalytic performance and higher GHSV increased the total alcohol selectivity, indicating there existed visible dehydration reaction of alcohol into hydrocarbon.
基金supported by State Key Program of National Natural Science Foundation of China(21733002)Joint Sino-German Research Project(21761132011)Cheung Kong Scholars Programme of China(T2015036)。
文摘Boron-based metal-free catalysts for oxidative dehydrogenation of propane(ODHP)have drawn great attention in both academia and industry due to their impressive activity and olefin selectivity.Herein,the SiO2 and B2O3 sequentially coated honeycomb cordierite catalyst is designed by a two-step wash-coat method with different B2O3 loadings(0.1%–10%)and calcination temperatures(600,700,800℃).SiO2 obtained by TEOS hydrolysis acts as a media layer to bridge the cordierite substrate and boron oxide via abundant Si\\OH groups.The welldeveloped straight channels of honeycomb cordierite make it possible to carry out the reactor under high gas hourly space velocity(GHSV)and the thin wash-coated B2O3 layer can effectively facilitate the pore diffusion on the catalyst.The prepared B2O3/SiO2@HC monolithic catalyst exhibits good catalytic performance at low boron oxide loading and achieves excellent propylene selectivity(86.0%),olefin selectivity(97.6%,propylene and ethylene)and negligible CO2(0.1%)at 16.9%propane conversion under high GHSV of 345,600 ml·(g B2O3)^-1·h^-1,leading to a high propylene space time yield of 15.7 g C3H6·(g B2O3)^-1·h^-1 by suppressing the overoxidation.The obtained results strongly indicate that the boron-based monolithic catalyst can be properly fabricated to warrant the high activity and high throughput with its high gas/surface ratio and straight channels.
文摘利用溶胶-凝胶法制备Mn-Ce-O_x催化剂,考察了锰铈摩尔比和焙烧温度对催化剂催化氧化NO活性的影响,并对空速和稳定性进行了探究。结果表明,锰铈摩尔比为1,焙烧温度为300℃和400℃时,催化剂的NO氧化活性最佳。不同焙烧温度的催化剂中,400℃焙烧,催化剂呈片状结构,比表面积最大,可达113.8 m^2/g;其具有良好的稳定性,在NO体积分数为600μL/L,O_2的体积分数为4%,N2作平衡气,空速为480 000 m L/(g·h),反应温度为260℃时,NO催化氧化活性最高可达89%;进一步增大空速至960 000 m L/(g·h),相同反应条件下,NO催化活性最高可达69%。
