共查询到20条相似文献,搜索用时 31 毫秒
1.
Sunggyu Lee Vetkav R. Parameswaran Irving Wender Conrad J. Kulik 《Petroleum Science and Technology》1989,7(8):1021-1057
The roles played by carbon dioxide in the chemistry of methanol synthesis over CuO/ZnO/A12O3 catalysts have been experimentally investigated. It was concluded based on reaction rate measurements and thermodynamic considerations, that the two reactions that best describe the chemical system of methanol synthesis are the CO2-hydrogenation and water-gas shift reactions. It was also found experimentally that the presence of CO2 is vital for maintaining the catalytic activity. The significance of the study is enhanced by the fact that this was the first such investigation of the global chemistry of methanol synthesis to be based on the novel liquid phase process. It was also observed that the rates of methanol synthesis attained a maximum when the concentration of carbon dioxide in the reactor feed was controlled at a certain optimal value. The optimal CO2 content was found to be a function of the operating temperature and syngas composition. The experimental data are especially important because the apparatus and the operating conditions have been well-defined and carefully chosen to closely simulate industrial reactors. 相似文献
2.
Abstract The chemical equilibrium compositions and equilibrium constants of methanol synthesis reactions, starting from carbon monoxide, carbon dioxide and hydrogen, were studied experimentally at P=4.0-8. 6MPa and t = 220~260°C. It was found that lower temperatures and higher pressures are favourable to chemical equilibria In the interested range of the synthesis reactions using low-pressure process, but the influence of temperature on Kp Is much larger than that of pressure. 相似文献
3.
Vetkav R. Parameswaran Sunggyu Lee Irving Wender 《Petroleum Science and Technology》2013,31(7):899-918
Abstract This work focuses on the influence of water in determining the rate of methanol synthesis over CuO/ZnO/Al2O3 catalysts. The experimental investigations were conducted in a 1-L slurry reactor based on the novel liquid phase methanol synthesis process. The liquid medium used was a blend of paraffinic and naphthenic mineral oils with a mean molecular mass of 250. It was found that the methanol rates attained a maximum at an optimal water content which was dependent on the reaction temperature. The catalytic activity was found to decline with time at lower temperatures in the presence of a relatively large excess of water. The influence of water was also found to be firmly linked to the corresponding carbon dioxide content in the reactor feed. The experimental data bear additional significance because this was the first such study to be performed on the liquid phase process. Emphasis was therefore placed on the use of a CO-rich syngas in order to simulate anticipated process conditions. 相似文献
4.
ABSTRACT This work focuses on the investigation of the catalyst post-treatment in the liquid phase methanol synthesis process. The novel post-treatment process, using carbon dioxide, has been developed and experimentally proven to be effective not only in maintaining the initial catalytic activity over a long period of usage but also in improving the mechanical and chemical strength of the catalyst. It was also found that the role of ZnO in the catalytic reaction, if any, can be nicely replaced by ZnCO3. 相似文献
5.
Abstract Oil fields offer significant potential for storing carbon dioxide (CO2) and will most likely be the first large-scale geological targets for sequestration because the infrastructure, experience, and permitting procedures already exist. In addition, almost 40 years' experience in enhanced oil recovery (EOR) allows utilization of carbon capture and storage (CCS) and CO2 sequestration techniques in such a way as to improve recovery of petroleum fields and reduce the environmental issue of fossil fuel combustion gas products, particularly carbon dioxide. Carbon dioxide is one of the main greenhouse gases that causes global warming. As a response to global warming, geologic sequestration of CO2 in oil and gas reservoirs is one possibility to reduce the amount of CO2 released to the atmosphere. This simulation study presents a synthetic geologic model that is used to sequestrate carbon dioxide beside an EOR immiscible displacement process. 相似文献
6.
The chemical equilibrium compositions and equilibrium constants of methanol synthesis reactions, starting from carbon monoxide, carbon dioxide and hydrogen, were studied experimentally at P=4.0-8. 6MPa and t = 220∼260°C. It was found that lower temperatures and higher pressures are favourable to chemical equilibria In the interested range of the synthesis reactions using low-pressure process, but the influence of temperature on Kp Is much larger than that of pressure. 相似文献
7.
A. Djavidnia A. A. Izadpanah M. V. Sefti F. Varaminian 《Petroleum Science and Technology》2013,31(19):2013-2021
Equilibrium data for the novel formation of hydrates of carbon dioxide and mixtures of carbon dioxide and methane in 20 wt% aqueous methanol solution were measured by the constant-volume method. For CO2, these data were taken at the temperature and pressure ranges of 264.7–270.7 K and 1,470–3,160 kPa, respectively. For mixtures of carbon dioxide and methane, these data were taken at the temperature and pressure ranges of 262.9–273.7 K and 1,370–5,100 kPa, respectively. The data obtained for CO2 in 20 wt% aqueous methanol solution were in disagreement with previously published data, but there was good agreement between our data and the predictions of thermodynamic models. The Peng-Robinson equation of state (PR EOS) coupled with the Wong-Sandler (WS) mixing rule was used to obtain the fugacities of the components in the gas and aqueous liquid phases. The PR EOS was then coupled with van der Waals-Platteeuw (vdW-P) hydrate model and applied to predict hydrate-formation conditions in the system containing methanol. The model predictions demonstrated good agreement with the experimental data. 相似文献
8.
Makarand R. Gogate 《Petroleum Science and Technology》2019,37(5):603-610
One of the very long-standing controversies in CO/CO2 hydrogenation chemistry has been the following: What is the principal source of C in the methanol product, CO or CO2? In other words, do CO hydrogenation and CO2 hydrogenation proceed independently, in parallel, over the industrial Cu/ZnO/Al2O3 catalyst? Using state of the art experimental data and our analysis of prior studies and experimental techniques including isotopic labeling studies, including radioactive tracers, FTIR, XPS, and E-TEM, we discuss the experimental findings of the prior art and analyze the experimental and theoretical first-principles calculational data, to come up with a rational and cogent explanation for all controversial areas in methanol synthesis chemistry. 相似文献
9.
The formation of carbon dioxide in the Fischer-Tropsch synthesis performed in a three-phase system in the presence of a nanosized
catalyst was studied. The synthesis temperature was found the main parameter responsible for the yield of CO2. At a constant conversion of CO, pressure has almost no effect on selectivity for the formation of CO2, whereas a decrease in the H2/CO ratio and an increase in the contact time or the concentration of an active component in the reaction zone lead to a decrease
in the selectivity. 相似文献
10.
《Petroleum Science and Technology》2013,31(7-8):841-866
ABSTRACT Oil fields are likely to the first category of geologic formation where carbon dioxide (CO2) is injected for sequestration on a large scale, if geologic sequestration proves feasible. About 1.4 BCF per day (69 300 tonnes/day) of CO2 are currently injected for oil recovery in the U.S. Replacing this naturally occurring CO2 with anthropogenic CO2 would have a minor, but measurable, effect on overall CO2 emissions. However, CO2 is injected into only a small fraction of reservoirs and it is estimated that upwards of 80% of oil reservoirs worldwide might be suitable for CO2 injection based upon oil recovery criteria alone. These facts combined with the generally extensive geologic characterization of oil reservoirs and the maturity of CO2–oil recovery technology make oil reservoirs attractive first targets as CO2 sinks. This paper lays the groundwork necessary to evaluate whether an oil reservoir might be suitable for CO2 storage. As such, a series of criteria for injection into currently producing, depleted, or inactive reservoirs are proposed. Aspects considered include the reservoir depth, storage capacity, water and oil volumes in place, formation thickness, and permeability. Importantly, the effect of oil production on reservoir properties, especially fault movement and induced fractures must be gauged and included in assessments. It is demonstrated that CO2 density with depth alone is not a sufficient criterion for choosing candidate sites. It is necessary to consider also porosity and the amount of water and oil that are displaceable. The end result is a criteria table for rapid screening of candidate reservoirs. 相似文献
11.
大气中CO2含量不断增加对环境和社会的影响是目前全球面临的最重大挑战之一。作为减缓和适应气候变化的行之有效的手段,碳捕获、利用和封存已引起越来越多的关注。其中,CO2利用,即直接使用CO2或将其转化为更有价值的产品,已成为减少CO2排放广泛战略中的一个极其重要的组成部分,这一挑战的实现需要技术和政策变革的支撑。总结和讨论了近20年来国内外利用催化、合成技术,将CO2转化为高附加值特定化学品(如甲酸、甲醇、聚合物等)的工艺研究进展和存在的相关挑战,并从原子高效率利用和工业角度,提出一些以CO2为合成原料的具有一定工业应用前景的有机合成方法,如基于CO2的聚醚醇碳酸酯和聚碳酸酯的合成,并指出实现这一工业应用面临的难点和挑战。 相似文献
12.
Abstract Recently, there is a growing interest the in oil industry to utilize carbon dioxide (CO2) to enhance oil production from mature reservoirs. Conversely, there is a rising global attention to reduce CO2 emissions from burning fossil fuels due to environmental concerns. Synchronization between these two objectives is promising through CO2 Capture and Storage (CCS) projects where CO2 is captured from large emission sources and then storedin safe geological structures. Economical evaluation of CO2-EOR projects is a crucial measure in order to ensure a project's viability. In this study, an efficient model was developed to predict the economics of CO2-EOR projects. The developed model consists of five modules that are linked together to allow for fast prediction of CO2-EOR economics. The model was used to predict the economics of a case study where CO2-EOR application is considered for a Middle Eastern reservoir. Moreover, the case study was subjected to sensitivity analyses to evaluate the effects of several parameters on the various economical components of CO2-EOR projects. 相似文献
13.
P. Vijayaraghavan Conrad j. Kulik Sunggyu Lea 《Petroleum Science and Technology》2013,31(11):1577-1596
ABSTRACT The commercial reactor proposed for the liquid phase methanol synthesis process (LPMeCHTM) is a liquid entrained reactor (LER), since it possesses several operational advantages over a mechanically agitated slurry reactor (MASR). This paper discusses in detail the develocment of a correlation for the prediction of the overall gas-liquid mass transfer coefficient (KLiaB) in a LER. The overall mass transfer coefficient experimentally determined for the LER, is compared with the corresponding value obtained for the MASR under nominally identical operating conditions. It was observed that the overall gas-liquid mass transfer coefficient and hence the overall rate of methanol production per unit mass of catalyst, is significantly higher in the LER compared to the MASR at identical operating conditions. In the LER mode, the limitation posed on the system by chemical equilibrium, is alleviated by selective renewal of products thus making the process ideal for the once-through methanol (CIM) This justifies the proposed commercial mode of synthesis of methanol in the liquid entrained reactor. 相似文献
14.
M. V. Tsodikov A. S. Fedotov V. V. Zhmakin K. B. Golubev V. N. Korchak V. N. Bychkov N. Yu. Kozitsyna I. I. Moiseev 《Petroleum Chemistry》2011,51(7):568-576
The features of the carbon dioxide reforming of ethanol and an ethanol-glycerol mixture to synthesis gas in the presence of
porous membrane catalyst systems have been studied. It has been shown that the CO2 reforming of alcohols in open pores of ceramic membranes modified with nanosized active palladiumcontaining components proceeds
at a higher rate as compared to that in a conventional fixed-bed flow reactor charged with a catalyst of similar composition. 相似文献
15.
Abstract The intricate behavior of carbon dioxide at supercritical conditions is considered to influence the ultimate recovery of additional hydrocarbon reserves through the application of CO2-enhanced gas recovery projects. Mixing in such a system is a diffusion-like process, which definitely depends on the physical properties of the displacing and displaced phases and the heterogeneity of the medium. The authors' aim was to experimentally investigate the consequence of pore pressure on the recovery efficiency and multiphase gas flow in a reservoirs porous medium. The displacement tests were carried out at five different pore pressures ranging from 10.34 to 40.68 MPa, temperature of 433.15 K, and displacement rate of 10 cm/hr. Results determined that improved recovery by approximately 40% can be obtained by applying the highest pore pressure in comparison with the test conducted at low pore pressure. 相似文献
16.
Tianfu Xu Liange Zheng Hailong Tian 《Journal of Petroleum Science and Engineering》2011,78(3-4):765-777
One way to reduce carbon dioxide (CO2) releases to the atmosphere, is to capture it from power plants and then inject it into deep geological formations. Understanding water-gas-mineral reactions is the core of assessing the long term storage and risks in geological sequestration. Because of various limitations of laboratory and field tests, reactive transport modeling has been one important supplementary or independent tool to study the water–gas–mineral reactions at different components of geological sequestration. In this paper, we reviewed the applications of reactive transport modeling to three aspects of CO2 geological sequestration: the behavior of CO2 in storage formation, the storage security issues related to caprock integrity or wellbore cement degradation, and the change of the shallow groundwater in response to the potential leakage of CO2. Key finding are summarized and further research needs are identified. The lack of the detailed mineralogical composition information at the storage formation, caprock and overlying aquifers is currently the first obstacle for quantitative prediction of geochemical evolution. The thermodynamic properties of relevant minerals under high temperature and pressure have to be refined. Reliable reaction rates of minerals dissolution/precipitation at field are still the bottle neck of the calculating the long term mineral trapping of CO2. Issues related to relatively fast reactions such sorption and ion exchange need special attention when the impact of CO2 leakage on shallow groundwater was evaluated. The role of organic compounds in water-gas-mineral reactions needs further study. 相似文献
17.
刘志刚 《石油与天然气化工》2022,51(4):24-32
目的在全球节能减排的大背景以及我国“碳达峰、碳中和”的双碳战略目标指导下,有针对性地研究适用于不同工况的CO2捕集技术成为极其重要的研究趋势。 方法结合碳捕集领域最新发展动态,针对燃烧过程中CO2的排放,对比了吸收法、吸附法、深冷分离、膜吸收法、超重力法等技术的优缺点以及应用动态,分析总结了CO2捕集技术的发展趋势。 结果阐明了几种CO2燃烧后捕集技术的技术特点。明晰了当前吸收法中吸收剂的选择是核心,反应器与操作条件的优化是重点。对于吸附法,面向大规模工业应用,开发选择性高、吸附容量高、解吸能力强、价格便宜的吸附剂是关键。而对于膜技术,其特点是操作简便、灵活,但提高膜的性能依然是需要持续进行的研究。总体而言,阐明了几种捕集技术的特点、应用潜力和研究方向。 结论尽管当前已经有较多CO2吸收与分离技术得到广泛的研究与应用,但在具体应用中仍存在诸多问题,针对CO2吸收与分离的新材料、新溶剂的研究仍是碳捕集领域研究的前沿与热点课题。从碳捕集技术层面出发,今后的发展趋势很可能是两种或两种以上技术串联使用,以满足更多工况条件下的脱碳需求。 相似文献
18.
Abstract Water content of carbon dioxide (CO2) is an important parameter in engineering applications, such as CO2 storage in deep saline aquifers and enhanced oil recovery processes. A large number of experimental data have been reported on solubility of CO2 in brine. However, experimental data on water content of CO2 in equilibrium with formation brine are not reported in the literature. Water content of natural gas is traditionally calculated by general water content charts; however, these charts are not available for CO2 in equilibrium with formation brine. Using an accurate fugacity and activity model available in the literature, the authors developed an efficient and simple procedure to estimate the water content of CO2 in equilibrium with formation brine. To validate the developed procedure, the predicted CO2-rich phase water content is compared with the reported experimental data in the literature and other predictive models for CO2-water system. A CO2 water content chart is presented that can be simply used to predict the water content of CO2 in equilibrium with formation brine. The procedure presented may be used for generating necessary input data for flow simulation of CO2 storage in deep saline aquifers. 相似文献
19.
Ashkan Khoshkharam Mohammad Ali Ghayyem Reza Mosayyebi Behbahani 《Petroleum Science and Technology》2017,35(5):471-478
Removal of carbon dioxide from methane is a critical issue in the gas sweetening and treatment units. The aim of this study is to investigate the capability of PES/Pebax composite membrane in order to CO2 removal from the CH4. In this regard, permeability values of both carbon dioxide and methane have been measured. The ranges of temperature and pressure used for pure gases experiments were 20–50°C and 2.5–10 bar, respectively. Moreover, influence of CO2 concentration on the CH4 permeability and its selectivity was studied. Results indicated that the pressure and temperature have significant influence on permeability and selectivity. In addition, for the gas mixtures, experiments were carried out at 5 bar and 35°C. Results also indicated that at higher CO2 concentrations the CO2 permeability increased significantly. 相似文献
20.
Abstract The authors quantitatively investigates the recovery efficiency, pattern behavior, and relative permeability of (a) condensate following supercritical carbon dioxide (CO2) injection, methane (CH4) injection, and the injection of their mixtures; and (b) natural gas of various compositions following pure supercritical CO2 injection. A high-pressure high-temperature experimental laboratory was established to simulate reservoir conditions and to perform relative permeability measurements on sandstone cores. This work is part of an integrated enhanced natural gas and condensate recovery project conducted for a local reservoir in Western Australia. This data will help the operators develop operational and design strategies for their present and future EOR projects. 相似文献