合成气制低碳醇碳化钼催化剂的研究及其对生态环境的影响
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摘要
在化石能源日益枯竭和环境污染日趋严重的今天,寻找绿色、清洁的替代能源迫在眉睫。利用生物质能源,开发“绿色燃料”——低碳醇燃料是解决该问题的主要途径之一。由生物质制备合成气用于合成低碳醇燃料在经济和技术方面都具有潜在的优势,有巨大的应用前景。然而如何提高合成气制低碳醇反应活性、减少尾气中CH4和C02的排放以及降低反应过程中的能耗是未来合成气制低碳醇反应实现工业化需要解决的问题。因此合成具有高活性和高选择性的合成气制低碳醇催化剂就成为解决问题的首要因素。研究表明碳化钼催化剂在合成气制低碳醇反应中具有较高的C2+OH选择性,是一类非常有前景的催化剂。
本文制备了负载型碳化钼催化剂,对其合成气制低碳醇反应的催化活性、尾气中CH4和CO2的排放量进行综合评价。以具有三维笼状结构的介孔分子筛SBA-16为载体,通过等体积浸渍将活性组分负载到载体上,制备了一系列Ni-β-Mo2C-K/SBA-16催化剂。通过XRD、TEM及比表面积等测试手段,对催化剂物相、孔结构和活性成分等进行分析,重点讨论载体、助剂与催化剂结构、性能之间的关系,探讨影响催化剂反应性能的因素。
实验发现,反应温度对催化活性的影响最明显,升高反应温度可以提高CO转化率、C2+OH选择性和时空产率,但是总醇选择性会降低；反应压力对催化性能的影响最小,在一定范围内改变压力对反应活性几乎没有影响；空速对反应的影响介于温度和压力之间,提高空速可以增加总醇选择性,但CO转化率和C2+OH选择性会降低。助剂Ni含量过低会降低C2+OH选择性,而过高会生成烃类化合物,因此在负载型碳化钼催化剂中Ni/Mo的物质量之比在1/8时反应活性最好。K助剂对总醇选择性和C2+OH选择性有影响。在负载型碳化钼催化剂中K/Mo的摩尔比在3/10时CO转化率、总醇选择性和C2+OH选择性最高。增加Mo含量,CO转化率、总醇选择性、C2+OH选择性和时空产率都会提高。当Mo负载量30%、Ni/Mo=1/8、K/Mo=3/10时,负载型催化剂Ni-β-Mo2C-K/SBA-16的活性最佳。通过催化反应发现具有三维笼状孔道且含有较大孔径的SBA-16介孔材料能够促进催化反应、提高CO转化率、总醇选择性和C2+OH选择性。
将负载型双金属碳化钼催化剂应用于CH4/CO2催化重整反应,模拟了合成气制低碳醇反应装置与CH4/CO2催化重整反应装置耦合的生产模式,摸索合成气制低碳醇反应装置与CH4/CO2催化重整装置耦合的经验。
It is very urgent for looking green and clean alternative energy with the depletion of fossil energy and environmental pollution. Using biomass energy to developing "green fuel"—alcohol fuel is one of the main ways to solve the problem. It has potential advantage and great prospect on economic and technical aspects that synthesis gas preparation from biomass for alcohol fuel. How to improve the syngas to alcohol reaction activity, reduce exhaust of CH4and CO2as well as energy consumption in the process of syngas to alcohol are urgent problems for future industrialization. A key solution for solving the problem is to develop the syngas to alcohol catalyst with high activity and high selectivity. It is evident from the recent research that the β-Mo2C-based catalysts are with high C2+OH selectivity and thus the most promising catalysts for higher alcohol synthesis.
In this paper we prepared supported molybdenum carbide catalysts. The comprehensive evaluation of the catalysts such as syngas to alcohol activity, emissions of CH4and CO2is presented and discussed.3D cage-like structure of mesoporous molecular sieve SBA-16as the carrier, prepared a series of Ni-β-Mo2C-K/SBA-16catalysts by impregnation method. The N2adsorption-desorption isotherms, XRD, TEM measurements were used to characterize the phase, pore structure, element distribution and active sites of the catalysts.
We found that the influence of the reaction temperature on the catalytic activity is the most obvious, elevated reaction temperature may increase the rate of CO conversion, C2+OH selectivity and space time yield, but would reduce total alcohol selectivity at the same time. Reaction pressure is minimal effect on the catalytic performance; the pressure is changed within a certain range, almost no influence on the reaction activity. Space velocity range between temperature and pressure effect on the reaction, increasing the space velocity could promote the selectivity of the total alcohol with reducing the CO conversion and C2+OH selectivity. Low Ni content will reduce the C2+OH selectivity, and will generate the hydrocarbon compound with high contents. Therefore, the mass ratio of Ni/Mo=1/8in supported molybdenum carbide catalyst has the highest reactivity. Metal K affects the total alcohol selectivity and C2+OH selectivity. The CO conversion, total alcohol selectivity and C2+OH selectivity are high when K/Mo molar ratio of3/10. The CO conversion rate, the total alcohol selectivity, C2+OH selectivity and space-time yield improved with increasing the Mo content. When the the Mo loading amount30%, Ni/Mo=1/8, K/Mo=3/10, the activity of the supported catalyst Ni-β-Mo2C-K/SBA-16has the best performence. By catalytic reaction, having a3D cage-like pore and containing the larger aperture of the SBA-16mesoporous material can contribute to the catalytic reaction, which could enhance the rate of CO conversion, and total alcohol selectivity and C2+OH selectivity.
The supported bimetallic molybdenum carbide catalyst is applied in CH4/CO2reforming reaction, and a production mode was simulated by coupling of the alcohol from syngas device with CH4/CO2reforming unit.
本文制备了负载型碳化钼催化剂,对其合成气制低碳醇反应的催化活性、尾气中CH4和CO2的排放量进行综合评价。以具有三维笼状结构的介孔分子筛SBA-16为载体,通过等体积浸渍将活性组分负载到载体上,制备了一系列Ni-β-Mo2C-K/SBA-16催化剂。通过XRD、TEM及比表面积等测试手段,对催化剂物相、孔结构和活性成分等进行分析,重点讨论载体、助剂与催化剂结构、性能之间的关系,探讨影响催化剂反应性能的因素。
实验发现,反应温度对催化活性的影响最明显,升高反应温度可以提高CO转化率、C2+OH选择性和时空产率,但是总醇选择性会降低；反应压力对催化性能的影响最小,在一定范围内改变压力对反应活性几乎没有影响；空速对反应的影响介于温度和压力之间,提高空速可以增加总醇选择性,但CO转化率和C2+OH选择性会降低。助剂Ni含量过低会降低C2+OH选择性,而过高会生成烃类化合物,因此在负载型碳化钼催化剂中Ni/Mo的物质量之比在1/8时反应活性最好。K助剂对总醇选择性和C2+OH选择性有影响。在负载型碳化钼催化剂中K/Mo的摩尔比在3/10时CO转化率、总醇选择性和C2+OH选择性最高。增加Mo含量,CO转化率、总醇选择性、C2+OH选择性和时空产率都会提高。当Mo负载量30%、Ni/Mo=1/8、K/Mo=3/10时,负载型催化剂Ni-β-Mo2C-K/SBA-16的活性最佳。通过催化反应发现具有三维笼状孔道且含有较大孔径的SBA-16介孔材料能够促进催化反应、提高CO转化率、总醇选择性和C2+OH选择性。
将负载型双金属碳化钼催化剂应用于CH4/CO2催化重整反应,模拟了合成气制低碳醇反应装置与CH4/CO2催化重整反应装置耦合的生产模式,摸索合成气制低碳醇反应装置与CH4/CO2催化重整装置耦合的经验。
It is very urgent for looking green and clean alternative energy with the depletion of fossil energy and environmental pollution. Using biomass energy to developing "green fuel"—alcohol fuel is one of the main ways to solve the problem. It has potential advantage and great prospect on economic and technical aspects that synthesis gas preparation from biomass for alcohol fuel. How to improve the syngas to alcohol reaction activity, reduce exhaust of CH4and CO2as well as energy consumption in the process of syngas to alcohol are urgent problems for future industrialization. A key solution for solving the problem is to develop the syngas to alcohol catalyst with high activity and high selectivity. It is evident from the recent research that the β-Mo2C-based catalysts are with high C2+OH selectivity and thus the most promising catalysts for higher alcohol synthesis.
In this paper we prepared supported molybdenum carbide catalysts. The comprehensive evaluation of the catalysts such as syngas to alcohol activity, emissions of CH4and CO2is presented and discussed.3D cage-like structure of mesoporous molecular sieve SBA-16as the carrier, prepared a series of Ni-β-Mo2C-K/SBA-16catalysts by impregnation method. The N2adsorption-desorption isotherms, XRD, TEM measurements were used to characterize the phase, pore structure, element distribution and active sites of the catalysts.
We found that the influence of the reaction temperature on the catalytic activity is the most obvious, elevated reaction temperature may increase the rate of CO conversion, C2+OH selectivity and space time yield, but would reduce total alcohol selectivity at the same time. Reaction pressure is minimal effect on the catalytic performance; the pressure is changed within a certain range, almost no influence on the reaction activity. Space velocity range between temperature and pressure effect on the reaction, increasing the space velocity could promote the selectivity of the total alcohol with reducing the CO conversion and C2+OH selectivity. Low Ni content will reduce the C2+OH selectivity, and will generate the hydrocarbon compound with high contents. Therefore, the mass ratio of Ni/Mo=1/8in supported molybdenum carbide catalyst has the highest reactivity. Metal K affects the total alcohol selectivity and C2+OH selectivity. The CO conversion, total alcohol selectivity and C2+OH selectivity are high when K/Mo molar ratio of3/10. The CO conversion rate, the total alcohol selectivity, C2+OH selectivity and space-time yield improved with increasing the Mo content. When the the Mo loading amount30%, Ni/Mo=1/8, K/Mo=3/10, the activity of the supported catalyst Ni-β-Mo2C-K/SBA-16has the best performence. By catalytic reaction, having a3D cage-like pore and containing the larger aperture of the SBA-16mesoporous material can contribute to the catalytic reaction, which could enhance the rate of CO conversion, and total alcohol selectivity and C2+OH selectivity.
The supported bimetallic molybdenum carbide catalyst is applied in CH4/CO2reforming reaction, and a production mode was simulated by coupling of the alcohol from syngas device with CH4/CO2reforming unit.
引文
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