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1.
A 3D numerical model for gas–solid flow was developed and used to study the sorption enhanced steam methane reforming (SE-SMR) and the sorbent regeneration processes with CaO based sorbent in fluidized bed reactors. The SE-SMR process (i.e., SMR and adsorption of CO2) was carried out in a bubbling fluidized bed. The effects of pressure and steam-to-carbon ratio on the reactions are studied. High pressure and low steam-to-carbon ratio will decrease the conversion of methane. But the high pressure makes the adsorption of CO2 faster. The methane conversion and heat utility are enhanced by CO2 adsorption. The produced CO2 in SMR process is adsorbed almost totally in a relative long period of time in the bubbling fluidized bed. It means that the adsorption rate of CO2 is fast enough compared with the SMR rate. The process of sorbent regeneration was carried out in a riser. An unfeasible residence time is required to complete the regeneration process. Higher temperature makes the release of CO2 faster, but the rate is severely restrained by the increased CO2 concentration in gas phase. The temperature distribution is uniform over the whole reactor. Regeneration rate and capacity of sorbents are important factors in selecting the type of reactors for SE-SMR process.  相似文献   

2.
A novel concept for capturing CO2 from biomass combustion using CaO as an active solid sorbent of CO2 is discussed and experimentally tested. According to the CaO/CaCO3 equilibrium, if a fuel could be burned at a sufficiently low temperature (below 700 °C) it would be possible to capture CO2in situ” with the CaO particles at atmospheric pressure. A subsequent step involving the regeneration of CaCO3 in a calciner operating at typical conditions of oxyfired-circulating fluidized combustion would deliver the CO2 ready for purification, compression and permanent geological storage. Several series of experiments to prove this concept have been conducted in a 30 kW interconnected fluidized bed test facility at INCAR-CSIC, made up of two interconnected circulating fluidized bed reactors, one acting as biomass combustor-carbonator and the other as air-fired calciner (which is considered to yield similar sorbent properties than those of an oxyfired calciner). CO2 capture efficiencies in dynamic tests in the combustor-carbonator reactor were measured over a wide range of operating conditions, including different superficial gas velocities, solids circulation rates, excess air above stoichiometric, and biomass type (olive pits, saw dust and pellets). Biomass combustion in air is effective at temperatures even below the 700 °C, necessary for the effective capture of CO2 by carbonation of CaO. Overall CO2 capture efficiencies in the combustor-carbonator higher than 70% can be achieved with sufficiently high solids circulation rates of CaO and solids inventories. The application of a simple reactor model for the combined combustion and CO2 capture reactions allows an efficiency factor to be obtained from the dynamic experimental test that could be valuable for scaling up purposes.  相似文献   

3.
Calcium looping (CaL) is a promising post-combustion CO2 capture technology which is carried out in a dual fluidized bed (DFB) system with continuous looping of CaO, the CO2 carrier, between two beds. The system consists of a carbonator, where flue gas CO2 is adsorbed by CaO and a regenerator, where captured CO2 is released. The CO2-rich regenerator flue gas can be sequestered after gas processing and compression. A parametric study was conducted on the 10 kWth DFB facility at the University of Stuttgart, which consists of a bubbling fluidized bed carbonator and a riser regenerator. The effect of the following parameters on CO2 capture efficiency was investigated: carbonator space time, carbonator temperature and calcium looping ratio. The active space time in the carbonator, which is a function of the space time and the calcium looping ratio, was found to strongly correlate with the CO2 capture efficiency. BET and BJH techniques provided surface area and pore volume distribution data, respectively, for collected sorbent samples. The rate of sorbent attrition was found to be 2 wt.%/h which is below the expected sorbent make-up rate required to maintain sufficient sorbent activity. Steady-state CO2 capture efficiencies greater than 90% were achieved for different combinations of operational parameters. Moreover, the experimental results obtained were briefly compared with results derived from reactor modeling studies. Finally, the implications of the experimental results with respect to commercialization of the CaL process have been assessed.  相似文献   

4.
Calcium oxide (CaO) is a material that is being widely investigated in the context of CO2 capture. One such application is as a CO2 sorbent in the sorption-enhanced steam methane reforming processes (SERP). CO2 is captured in an adsorption mode, where the conversion of CH4 to H2 is also enhanced, and released later in a separate desorption mode. This work presents an analysis of the relation between different process conditions and parameters during both adsorption and desorption modes. The interrelation between these conditions and the sorbent properties as well as the targeted carbon capture ratio is analysed. Conditions relevant for capturing 85% of carbon in the feed on CaO are determined and interlinked. A steam-to-carbon ratio of 4.2 has been determined to be relevant under 600 °C and 17 bar adsorption conditions. Similarly, process conditions relevant for regenerating the sorbent are determined and interlinked. For purge steam-to-CO2 ratio of 1.8 at a desorption pressure of 1 bar, relevant desorption temperature has been calculated to be 820 °C. System simulations under these adsorption and desorption conditions resulted in a system efficiency of 50.8%. Effect of tuning process operating conditions on system efficiency as well as the efficiency penalty associated with the regeneration of the sorbent are investigated by process simulations using Aspen Plus®. Possible system heat integration routes to reduce the efficiency penalty are proposed and the results of the process simulations are presented.  相似文献   

5.
In this work several Li4SiO4-based sorbents from fly ashes for CO2 capture at high temperatures have been developed. Three fly ash samples were collected and subjected to calcination at 950 °C in the presence of Li2CO3. Both pure Li4SiO4 and fly ash-based sorbents were characterised and tested for CO2 sorption at different temperatures between 400 and 650 °C and adding different amounts of K2CO3 (0–40 mol%). To examine the sorbents performance, multiple CO2 sorption/desorption cycles were carried out. The temperature and the presence of K2CO3 strongly affect the CO2 sorption capacity for the sorbents prepared from fly ashes. When the sorption temperature increases by up to 600 °C both the CO2 sorption capacity and the sorption rate increase significantly. Moreover when the amount of K2CO3 increases, the CO2 sorption capacity also increases. At optimal experimental conditions (600 °C and 40 mol% K2CO3), the maximum CO2 sorption capacity for the sorbent derived from fly ash was 107 mg CO2/g sorbent. The Li4SiO4-based sorbents can maintain its original capacity during 10 cycle processes and reach the plateau of maximum capture capacity in less than 15 min, while pure Li4SiO4 presents a continual upward tendency for the 15 min of the capture step and attains no equilibrium capacity.  相似文献   

6.
The dry sorbent CO2 capture process is an advanced concept to efficiently remove CO2 from flue gas with two fluidized-bed reactors. This paper summarizes the results of performance of the two fluidized-bed reactors in the continuous solid circulation mode to investigate the feasibility of using potassium carbonate-based solid sorbent (Sorb KX35). The parameters such as gas velocity, solid circulation, carbonation temperature, and water vapor content were investigated during several continuous operations of two fluidized-bed reactors. The CO2 removal increased as gas velocity was decreased and as solid circulation rate was increased. The CO2 removal ranged from 26% to 73% was rather sensitive to the water vapor content among other parameters. A 20 h continuous operation conducted in a bench scale fast fluidized-bed reactor system indicated that the spray-dried potassium-based sorbent, Sorb KX35 having superior attrition resistance and high bulk density, had a promising CO2 removal capacity of 50–73% at steady state and was able to regenerate and reuse. The results from this work are good enough to prove the concept of the dry sorbent CO2 capture process to be one of viable methods for capturing CO2 from dilute flue gas of fossil fuel-fired power plants.  相似文献   

7.
The chilled ammonia process absorbs the CO2 at low temperature (2–10 °C). The heat of absorption of carbon dioxide by ammonia is significantly lower than for amines. In addition, degradation problems can be avoided and a high carbon dioxide capacity is achieved. Hence, this process shows good perspectives for decreasing the heat requirement. However, a scientific understanding of the processes is required. The thermodynamic properties of the NH3–CO2–H2O system were described using the extended UNIQUAC electrolyte model developed by Thomsen and Rasmussen in a temperature range from 0 to 110 °C and pressure up to 100 bars. The results show that solid phases consisting of ammonium carbonate and bicarbonate are formed in the absorber. The heat requirements in the absorber and in the desorber have been studied. The enthalpy calculations show that a heat requirement for the desorber lower than 2 GJ/ton CO2 can be reached.  相似文献   

8.
CO2 and SO2 are some of the main polluting gases emitted into atmosphere in combustion processes using fossil fuel for energy production. The former is one of the major contributors to build-up the greenhouse effect implicated in global climate change and the latter produces acid rain. Oxy-fuel combustion is a technology, which consists in burning the fuel with a mix of pure O2 and recirculated CO2. With this technology the CO2 concentration in the flue gas may be enriched up to 95%, becoming possible an easy CO2 recovery. In addition, oxy-fuel combustion in fluidized beds allows in situ desulfurization of combustion gases by supplying calcium based sorbent.In this work, the effect of the principal operation variables affecting the sulfation reaction rate in fluidized bed reactors (temperature, CO2 partial pressure, SO2 concentration and particle size) under typical oxy-fuel combustion conditions have been analyzed in a batch fluidized bed reactor using a limestone as sorbent. It has been observed that sulfur retention can be carried out by direct sulfation of the CaCO3 or by sulfation of the CaO (indirect sulfation) formed by CaCO3 calcination. Direct sulfation and indirect sulfation operating conditions depended on the temperature and CO2 partial pressure. The rate of direct sulfation rose with temperature and the rate of indirect sulfation for long reaction times decreased with temperature. An increase in the CO2 partial pressure had a negative influence on the sulfation conversion reached by the limestone due to a higher temperature was needed to work in conditions of indirect sulfation. Thus, it is expected that the optimum temperature for sulfur retention in oxy-fuel combustion in fluidized bed reactors be about 925–950 °C. Sulfation reaction rate rose with decreasing sorbent particle size and increasing SO2 concentration.  相似文献   

9.
Saline aquifers of high permeability bounded by overlying/underlying seals may be surrounded laterally by low-permeability zones, possibly caused by natural heterogeneity and/or faulting. Carbon dioxide (CO2) injection into and storage in such “closed” systems with impervious seals, or “semi-closed” systems with non-ideal (low permeability) seals, is different from that in “open” systems, from which the displaced brine can easily escape laterally. In closed or semi-closed systems, the pressure buildup caused by continuous industrial-scale CO2 injection may have a limiting effect on CO2 storage capacity, because geomechanical damage caused by overpressure needs to be avoided. In this research, a simple analytical method was developed for the quick assessment of the CO2 storage capacity in such closed and semi-closed systems. This quick-assessment method is based on the fact that native brine (of an equivalent volume) displaced by the cumulative injected CO2 occupies additional pore volume within the storage formation and the seals, provided by pore and brine compressibility in response to pressure buildup. With non-ideal seals, brine may also leak through the seals into overlying/underlying formations. The quick-assessment method calculates these brine displacement contributions in response to an estimated average pressure buildup in the storage reservoir. The CO2 storage capacity and the transient domain-averaged pressure buildup estimated through the quick-assessment method were compared with the “true” values obtained using detailed numerical simulations of CO2 and brine transport in a two-dimensional radial system. The good agreement indicates that the proposed method can produce reasonable approximations for storage–formation–seal systems of various geometric and hydrogeological properties.  相似文献   

10.
The feasibility of the sorption enhanced water gas shift (SEWGS) process under sour conditions is shown. The sour-SEWGS process constitutes a second generation pre-combustion carbon capture technology for the application in an IGCC. As a first critical step, the suitability of a K2CO3 promoted hydrotalcite-based CO2 sorbent is demonstrated by means of adsorption and regeneration experiments in the presence of 2000 ppm H2S. In multiple cycle experiments at 400 °C and 5 bar, the sorbent displays reversible co-adsorption of CO2 and H2S. The CO2 sorption capacity is not significantly affected compared to sulphur-free conditions. A mechanistic model assuming two different sites for H2S interaction explains qualitatively the interactions of CO2 and H2S with the sorbent. On the type A sites, CO2 and H2S display competitive sorption where CO2 is favoured. The type B sites only allow H2S uptake and may involve the formation of metal sulphides. This material behaviour means that the sour-SEWGS process likely eliminates CO2 and H2S simultaneously from the syngas and that an almost CO2 and H2S-free H2 stream and a CO2 + H2S stream can be produced.  相似文献   

11.
In order to evaluate the risk of hydrate formation in CO2 transport one has to be able to predict the water content in the fluid phase in equilibrium with the CO2-hydrate. A literature review has identified some knowledge gaps, for example, there are no results available at temperatures lower than 243.15 K (?30 °C); and none of the models found in literature predicts the water content with high accuracy. A model based on equality of water fugacity in fluid and hydrate phase is presented here and used for the predictions of water content in equilibrium with hydrates. Although this model gives better accuracy in the overall temperature and pressure ranges of measurements than the models found in the literature, it is not accurate enough to satisfy the requirements of CO2 transport. The simulation results also show that it is possible to form hydrate at low water content, such as xw = 50 vppm, if temperature is low enough. In order to verify the results and improve the model accuracy further, more experimental data in a larger temperature and pressure region are required.  相似文献   

12.
In this work, the Aspen Hysys conceptual design of a new process for energy generation at large scale with implicit CO2 capture is presented. This process makes use of the CaO capability for CO2 capture at high temperature and the possibility of regenerating this sorbent working in interconnected fluidised bed reactors operating at different temperatures. The proposed process has the advantage of producing power with minimum CO2 emissions and very low energy penalties compared with similar air-based combustion power plants. In this system, five main parts can be distinguished: the combustor where coal is burnt with air, the calciner where the fresh and the recycled CaCO3 is calcined, the carbonator where the CO2 produced in the combustor is captured, the supercritical steam cycle and the CO2 compression system. In this arrangement, the three fluidised bed reactors are interconnected in such a way that it is possible to perform the CaCO3 calcination at a temperature of 950 °C with the energy transported by a hot solid stream produced in the circulating fluidised bed combustor operating at 1030 °C. The stream rich in CaO produced in the calciner is split into three parts. One of them is transported to the carbonator operating at 650 °C where most of the CO2 in the flue gas produced in the combustor is captured. The second one is sent to the combustor, where it is heated up and used as energy carrier. The third solid stream that leaves the calciner is a purge in order to maintain the capture system activity and to avoid inert material accumulation. Because of the high temperatures involved in all the system, it is possible to recover most of the energy in the fuel and to produce power in a supercritical steam cycle. A case study is presented and it is demonstrated that under these operating conditions, 90% CO2 capture efficiency can be achieved with no energy penalty further than the one originated in the CO2 compression system.  相似文献   

13.
Simple models for permeability and selectivity variations of the CO2/CH4 system in 6FDA-2,6-DAT membrane have been derived that include both temperature and pressure effects simultaneously in a single equation. The proposed models were used in MATLAB, for a membrane-based CO2-removal process design for natural gas sweetening. The effects of the following factors on design parameters were examined: feed temperature, feed pressure and permeate pressure. The effect of permeate pressure was found to be very significant in the optimization process. In order to reduce hydrocarbon losses to below 2%, a two-stage membrane process was modeled and simulated in MATLAB, and the extent of desired hydrocarbon recovery was shown to be crucial in the optimization process. It has also been shown that there exist minima for the total required area of the two-stage membrane-based process, and as the CO2 load increases in the feed, the position of these minima shift to higher values of methane loss.  相似文献   

14.
Lime is considered a feasible sorbent for the capture of CO2 from large stationary sources. The positive attributes of a natural source material, low cost and lack of harmful by-products are offset by rapid deterioration in performance and high regeneration temperature. Performance can be improved by hydrating the lime using steam. We investigate a steam hydration process wherein lime is hydrated for 5 min at 300 °C and atmospheric pressure in a mixture of steam and CO2. The experiments consisted of 10 capture cycles with 60% of the lime active at the end. Extrapolation using a decay model suggests a residual carbonation level of 48%, significantly higher than the 8% achieved by dry lime cycles. The cost of replacement sorbent under these conditions is less than $1/t of CO2 captured. The hydrated lime process also reduces the thermal load, for heating and cooling, by half as well as the inventory, and therefore solids handling, by a factor 5 over dry lime. The introduction of the hydration reaction provides another exothermic reaction for heat management.  相似文献   

15.
Many studies on geological carbon dioxide (CO2) storage capacity neglect the influence of complex coupled processes which occur during and after the injection of CO2. Storage capacity is often overestimated since parts of the reservoirs cannot be reached by the CO2 plume due to gravity segregation and are thus not accessible for storage. This work investigates the effect of reservoir parameters like depth, temperature, absolute and relative permeability, and capillary pressure on the processes during CO2 injection and thus on estimates of effective storage capacity. The applied statistical characteristics of parameters are based on a large reservoir parameter database. Different measured relative permeability relations are considered. The methodology of estimating storage capacity is discussed. Using numerical 1D and 3D experiments, detailed time-dependent storage capacity estimates are derived. With respect to the concept developed in this work, it is possible to estimate effective CO2 storage capacity in saline aquifers. It is shown that effective CO2 mass stored in the reservoir varies by a factor of 20 for the reservoir setups considered. A high influence of the relative permeability relation on storage capacity is shown.  相似文献   

16.
CO2 storage capacity estimation: Methodology and gaps   总被引:3,自引:0,他引:3  
Implementation of CO2 capture and geological storage (CCGS) technology at the scale needed to achieve a significant and meaningful reduction in CO2 emissions requires knowledge of the available CO2 storage capacity. CO2 storage capacity assessments may be conducted at various scales—in decreasing order of size and increasing order of resolution: country, basin, regional, local and site-specific. Estimation of the CO2 storage capacity in depleted oil and gas reservoirs is straightforward and is based on recoverable reserves, reservoir properties and in situ CO2 characteristics. In the case of CO2-EOR, the CO2 storage capacity can be roughly evaluated on the basis of worldwide field experience or more accurately through numerical simulations. Determination of the theoretical CO2 storage capacity in coal beds is based on coal thickness and CO2 adsorption isotherms, and recovery and completion factors. Evaluation of the CO2 storage capacity in deep saline aquifers is very complex because four trapping mechanisms that act at different rates are involved and, at times, all mechanisms may be operating simultaneously. The level of detail and resolution required in the data make reliable and accurate estimation of CO2 storage capacity in deep saline aquifers practical only at the local and site-specific scales. This paper follows a previous one on issues and development of standards for CO2 storage capacity estimation, and provides a clear set of definitions and methodologies for the assessment of CO2 storage capacity in geological media. Notwithstanding the defined methodologies suggested for estimating CO2 storage capacity, major challenges lie ahead because of lack of data, particularly for coal beds and deep saline aquifers, lack of knowledge about the coefficients that reduce storage capacity from theoretical to effective and to practical, and lack of knowledge about the interplay between various trapping mechanisms at work in deep saline aquifers.  相似文献   

17.
The estimates for geological CO2 storage capacity worldwide vary, but it is generally believed that the capacity in saline aquifers will be sufficient for the amounts of CO2 that will need to be stored. The effort required to select and qualify a geological storage site for safe storage will, however, be significant and storage capacity may be a limited resource regionally. Both from a economic and resource management perspective it is therefore important that potential storage sites are exploited to their full potential.In static capacity estimates, where the maximum stored amount of CO2 is given as a fraction of the formation pore volume, typically arrive at efficiency factors in the range of a few per cents. Recent work has shown that when the dynamic behaviour of the injected CO2 is taken into account, the efficiency factor will be reduced because of the increase in pore pressure in the region around the injection well(s). The increase in pore pressure will propagate much further than the CO2. The EU directive on geological CO2 storage specifically addresses the restriction that will apply when different storage sites are interacting due to pressure communication. Consequently, the pore pressure increase at the boundary of the storage license area will be an important limiting factor for the amount of CO2 that can be injected.One obvious method to control the pore pressure is to produce water from the aquifer at some distance from the CO2 injection wells. This paper discusses results from simulations of CO2 injection in two aquifers on the Norwegian Continental Shelf; the Johansen aquifer and the southern part of the Utsira aquifer. These aquifers are candidates for injection of CO2 shipped out via pipeline from the Norwegian West Coast. The injected amounts of CO2 over a period of 50 years are 0.518 Gtonne for the Johansen aquifer and 1.04 Gtonne for the Utsira aquifer.Several design options for the injection operations are investigated: Injection of CO2 without water production; injection into several wells to distribute the injected fluids and reduce the local pressure increase around each injection well; and injection with simultaneous production of water from one or more wells. The boundaries of the aquifer formations are assumed closed in all simulations. The possible consequences of other types of boundary conditions (semi-closed or open) are briefly discussed.  相似文献   

18.
These two part papers analyse three plant configurations for high efficiency, near-zero emissions power generation from coal, suitable for long-term installations. In the first part the Zecomix cycle, a novel power plant based on various innovative processes, is presented. Zecomix plant is based on a coal hydrogasification process, using recycled steam and hydrogen as gasifying agents, to produce a CH4 rich syngas. Methane is then converted to an H2/H2O based syngas and CO2 is captured, by reacting in two carbonator reactors with CaO-based solid sorbent. CaCO3 produced in carbonators is thermally regenerated in a calciner. The synthetic fuel is burned with oxygen in a semi-closed high temperature steam cycle, with a supercritical heat recovery.The paper presents a detailed analysis of the thermodynamic aspects of the process, with the scope of assessing its potential performance in terms of efficiency and emissions. Main operating parameters of the chemical island (e.g. hydrogasifier and calciner pressure, steam flow rates to carbonators, syngas recycle fraction) and of the power island (e.g. pressure ratio, turbine inlet temperature and reheat pressure) were varied in order to evaluate their effect on plant performance and to optimize the process. Critical issues are specifically discussed: the calcination process, the calcium oxide utilization in carbonators, the cooling requirement of the high temperature turbine, the presence of incondensable species in the steam cycle. An accurate performance estimation is therefore developed by considering advanced components, as an evolution of today's technology, excluding unproven devices whose feasibility cannot be anticipated.Depending on sorbent utilization, a net plant efficiency of 44–47% with a virtually complete carbon capture was obtained, a very interesting result with respect to other proposed coal-fired power plants with carbon capture. The high complexity of the chemical island and the importance of a good sorbent performance should be however taken into account for a fair comparison with other plant concepts. Further experimental investigations are mandatory to demonstrate the technical and economical feasibility of the Zecomix plant.  相似文献   

19.
Industrial-scale injection of CO2 into saline formations in sedimentary basins will cause large-scale fluid pressurization and migration of native brines, which may affect valuable groundwater resources overlying the deep sequestration aquifers. In this paper, we discuss how such basin-scale hydrogeologic impacts (1) may reduce current storage capacity estimates, and (2) can affect regulation of CO2 storage projects. Our assessment arises from a hypothetical future carbon sequestration scenario in the Illinois Basin, which involves twenty individual CO2 storage projects (sites) in a core injection area most suitable for long-term storage. Each project is assumed to inject five million tonnes of CO2 per year for 50 years. A regional-scale three-dimensional simulation model was developed for the Illinois Basin that captures both the local-scale CO2–brine flow processes and the large-scale groundwater flow patterns in response to CO2 storage. The far-field pressure buildup predicted for this selected sequestration scenario support recent studies in that environmental concerns related to near- and far-field pressure buildup may be a limiting factor on CO2 storage capacity. In other words, estimates of storage capacity, if solely based on the effective pore volume available for safe trapping of CO2, may have to be revised based on assessments of pressure perturbations and their potential impacts on caprock integrity and groundwater resources. Our results suggest that (1) the area that needs to be characterized in a permitting process may comprise a very large region within the basin if reservoir pressurization is considered, and (2) permits cannot be granted on a single-site basis alone because the near- and far-field hydrogeologic response may be affected by interference between individual storage sites. We also discuss some of the challenges in making reliable predictions of large-scale hydrogeologic impacts related to CO2 sequestration projects.  相似文献   

20.
An ideal solvent for CO2 capture by chemical absorption has to meet a number of requirements, such as high CO2 capacity, high rate of reaction, low costs, low corrosive behaviour, low degradation and low vapour pressure; above all, it has to show a low regeneration heat duty. This heat can be approximated as the sum of three terms: the sensible heat to raise the solvent from absorber to desorber temperature, the heat of evaporation required to produce the stripping steam in the reboiler, and the heat necessary to desorb the CO2 from the solution (heat of absorption).Many solvent screening studies focus almost exclusively on solvents that show a low heat of absorption. In these studies, the strong dependence of the three contributors to the overall regeneration heat duty on the chosen process parameters and on one another are often neglected.This work explains why the focus on solvents with a low heat of absorption, without considering the overall process, is not sufficient in quantifying the energy performance of alternative solvents. By using thermodynamic interrelations and underpinned by process simulations it is shown that operating parameters of the process, in particular the desorber pressure, must be taken into consideration in the evaluation of new solvents.  相似文献   

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