国产Ru/Al2O3甲烷化催化剂的工业应用与探讨

对国产Ru/Al2O3催化剂研制开发、侧线试验及工业化试用情况进行了探讨,为国产Ru/Al2O3催化剂的推广应用提供了依据.     

担载型含稀土三组份体系在二氧化碳甲烷化反应中的催化性能

用浸渍法制备了一系列氧化锆担载的含稀土Ⅷ族金属催化剂，对其在二氧化碳甲烷化过程中的催化活性作了研究，并用漫反射紫外可见光谱，ＦＴＩＲ等手段对催化剂作了表征。结果表明，含稀土新型催化剂具有催化活性高，目标产物选择性好等优点；稀土主要以氧化物形式存在于催化剂表面，参与对氢及表面含碳物种的吸附及活化；含稀土三组份催化剂的活性与所添加稀土三价离子的４ｆ电子数有关。     

煤加氢液化制取芳烃研究进展

芳烃化合物是一类主要有机化工原料，目前主要从石油化工中获得．我国石油资源紧缺已成为生产芳烃的瓶颈，而煤由于其特殊的芳香性，在一定条件下经加氢液化后得到主要富舍芳烃的液体产品，有望成为石油代替和减缓石油供需矛盾的有效途径之一．对煤加氢液化制取芳烃的可能性、加氢液化工艺进展、煤液化油的组成以及液化油如何制取芳烃的方法等进行了综述和讨论，为进一步开展这一领域的研究工作奠定了基础．     

Kinetics of the methanation of carbon dioxide over a supported Ni-La2O3 catalyst

The kinetics of the methanation of carbon dioxide was investigated using an alumina supported Ni-La₂O₂ catalyst in a differential and integral reactor. In the differential reactor the molar ratio of H₂ to CO₂ was varied from 0.6 to 30. In the integral reactor the rates were measured with up to 90% conversion. Both reactor tests were carried out at temperatures between 513 and 593 K. The experimental results were described by a Langmuir-Hinshelwood type equation. The kinetics can be explained by assuming equilibrium of dissociative carbon dioxide and hydrogen adsorption, and assuming hydrogenation of surface carbon as the rate determining step.     

15万t/a双甲氨合成联合装置设计

从工艺路线的比较、压力等级的选择、主要设备的选型等方面阐述了双甲氨合成联合装置的设计特点。结合生产运行实践,分析了双甲氨合成工艺路线的运行参数,与采用不同工艺的生产消耗和产品成本进行了对比。结果表明,该工艺吨氨节约成本80元,精醇成本为1112.6元/t,经济效益显著且生产运行稳定。     

Methanation of carbon dioxide over Ru/Titania at room temperature: explorations for a photoassisted catalytic reaction

The methanation of CO₂ has been investigated over a special Ru/TiO₂ catalyst suggested by Thampi, Kiwi and Graetzel [4]. This paper deals with the analysis of the material and the investigation of the reported photoenhancement of the activity. The catalyst is characterised by in situ UV-VIS spectroscopy and by XPS. Conversion experiments at atmospheric pressure were carried out with and without UV light irradiation. The irradiation increases the conversion significantly. From various experiments it can be shown, however, that this effect is due to a thermal effect and does not involve an intrinsic photochemical step. Localised Ti³⁺ states sensitise the support to convert visible light into heat resulting in the observed increase in conversion.     

Hydrocarbon synthesis over sulfide catalysts. Break-down of the Anderson-Schulz-Flory distribution

The kinetics of hydrocarbon synthesis over sulfide-based catalysts was studied. It appears that the formation of methane follows another reaction path than that of higher hydrocarbons. This might explain the very high selectivities for ethane and propane as compared with conventional Fischer-Tropsch catalysts. Reference is made to testing of the catalysts at industrial conditions.     

Materials for global carbon dioxide recycling

CO₂ emissions, which induce global warming, increase with the development of economic activity. It is impossible to decrease the CO₂ emissions by suppression of the economic activity. Global CO₂ recycling can solve this problem. The global CO₂ recycling consists of three district: The electricity is generated by solar cells on deserts. At desert coasts, the electricity is used for H₂ production by seawater electrolysis and H₂ is used for CH₄ production by the reaction with CO₂. CH₄ which is the main component of liquefied natural gas is liquefied and transported to energy consuming districts where CO₂ is recovered, liquefied and transported to the desert coasts. A CO₂ recycling plant for substantiation of our idea has been built on the roof of the Institute for Materials Research in 1996. Key materials necessary for the global CO₂ recycling are the anode and cathode for seawater electrolysis and the catalyst for CO₂ conversion. All of them have been tailored by us. They have very high activity and selectivity for necessary reactions in addition to excellent durability. A pilot plant consisting of minimum units in an industrial scale is going to be built in three years.     

合成气甲烷化过程热力学分析

以化学热力学为基础,利用FactSage软件对2种典型的煤气化合成气甲烷化反应过程进行了热力学计算和分析。研究了合成气的组分、氢气的配比、反应温度、压力等条件对甲烷化过程的影响,特别是氢气的配比研究,区别于常规对H_2/CO分析而是以氢气的理论配比H_2/(3CO+4CO_2)进行分析。结果表明:反应器操作压力对甲烷化过程的影响不明显,合成气的组分、氢气的配比、反应温度的选择对甲烷化过程的影响较大。得出:合成气甲烷化过程应采用多段反应器,最终控制温度为(300~350)℃;操作压力一般为(3.0~3.5)MPa;H_2的配比采用理论配比时生产出的CH_4浓度高。     

Highly efficient MOF-templated Ni catalyst towards CO selective methanation in hydrogen-rich reformate gases

Highly efficient and non-noble metal-based Ni/ZrO₂ catalyst templated with Ni/UiO-66 precursor was successfully prepared and applied to CO selective methanation in H₂-rich gases. This catalyst showed excellent activity and selectivity in an extremely wide temperature window of 215–350 °C, and it also had high stability with no deactivation during a long-term stability test (120 h). The increased specific surface area, smaller crystallite size (3.5 nm) and higher dispersion (15.3%) of Ni nanoparticles, and the enhanced chemisorption capability for CO might contribute to its excellent performance.