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1.
CO2 mineralization as a promising CO2 mitigation strategy can employ industrial alkaline solid wastes to achieve net emission reduction of atmospheric CO2. The red mud is a strong alkalinity waste residue produced from the aluminum industry by the Bayer process which has the potential for the industrial CO2 large scale treatment. However, limited by complex components of red mud and harsh operating conditions, it is challenging to directly mineralize CO2 using red mud to recover carbon and sodium resources and to produce mineralized products simultaneously with high economic value efficiently. Herein, we propose a novel electrochemical CO2 mineralization strategy for red mud treatment driven by hydrogen-cycled membrane electrolysis, realizing mineralization of CO2 efficiently and recovery of carbon and sodium resources with economic value. The system utilizes H2 as the redox-active proton carrier to drive the cathode and anode to generate OH- and H+ at low voltage, respectively. The H+ plays as a neutralizer for the alkalinity of red mud and the OH- is used to mineralize CO2 into generate high-purity NaHCO3 product. We verify that the system can effectively recover carbon and sodium resources in red mud treatment process, which shows that the average electrolysis efficiency is 95.3% with high-purity (99.4%) NaHCO3 product obtained. The low electrolysis voltage of 0.453 V is achieved at 10 mA·cm-2 in this system indicates a potential low energy consumption industrial process. Further, we successfully demonstrate that this process has the ability of direct efficient mineralization of flue gas CO2 (15% volume) without extra capturing, being a novel potential strategy for carbon neutralization.  相似文献   

2.
A two-stage vacuum pressure swing adsorption (VPSA) process that coupled kinetically controlled and equilibrium controlled separation process with reflux has been investigated for capturing carbon dioxide from dry flue gas (85% N2/15% CO2). In the first enriching stage, carbon molecular sieve (CMS), which shows kinetic selectivity for CO2/N2, is adopted as the adsorbent to remove most N2 in feed gas, thereby upgrading CO2 and significantly reducing the amount for further refinement. The second stage loads zeolite 13X as adsorbent to purify the CO2-rich flow from the first stage for meeting the requirements of National Energy Technology Laboratory. Series of experiments have been conducted for adsorption isotherms measuring and lab-scale experimental validation as well as analysis. The effect of feed composition on the separation performance of the PSA system was studied experimentally and theoretically here. The optimal results achieved 95.1% purity and 92.9% recovery with a high CO2 productivity (1.89 mol CO2·h-1·kg-1) and an appropriate energy consumption of 1.07 MJ·(kg CO2)-1. Further analysis has been carried out by simulation for explicating the temperature, pressure, and concentration distribution at cyclic steady state.  相似文献   

3.
Dimethyl carbonate is an eco-friendly essential chemical that can be sustainably produced from CO2,which is available from carbon capture activities or can even be captured from the air.The rapid increase in dimethyl carbonate demand is driven by the fast growth of polycarbonates,solvent,pharmaceutical,and lithium-ion battery industries.Dimethyl carbonate can be produced from CO2through various chemical pathways,but the most convenient route reported is the indirect alcoholysis of urea.Previous research used techniques such as heat integration and reactive distillation to reduce the energy use and costs,but the use of an excess of methanol in the trans-esterification step led to an energy intensive extractive distillation required to break the dimethyl carbonate-methanol azeotrope.This work shows that the production of dimethyl carbonate by indirect alcoholysis of urea can be improved by using an excess of propylene carbonate(instead of an excess of methanol),a neat feat that we showed it requires only 2.64 kW·h·kg-1 dimethyl carbonate in a reaction-separation-recycle process,and a reactive distillation column that effectively replaces two conventional distillation columns and the reactor for dimethyl carbonate synthesis.Therefore,less equipment is required,the methanol-dimethyl carbonate azeotrope does not need to be recycled,and the overall savings are higher.Moreover,we propose the use of a reactive distillation column in a heat integrated process to obtain high purity dimethyl carbonate(>99.8 wt-%).The energy requirement is reduced by heat integration to just 1.25 kW·h·kg-1 dimethyl carbonate,which is about 52%lower than the reaction-separation-recycle process.To benefit from the energy savings,the dynamics and control of the process are provided for10%changes in the nominal rate of 32 ktpy dimethyl carbonate,and for uncertainties in reaction kinetics.  相似文献   

4.
The present paper reports a new fluoride-free and energy-saving lead electrolytic refining process in order to solve the serious problems of the existing Betts lead electrorefining process, such as low production efficiency,high energy consumption and fluorine pollution. In the process, a mixed solution of perchloric acid and lead perchlorate(HClO_4-Pb(ClO_4)_2) with the additives of gelatin and sodium lignin sulfonate is employed as the new electrolyte. The cathodic polarization curves show that HClO_4 is very stable, and there is no any reduction reaction of HClO_4 during the electrolytic process. The redox reactions of lead ions in HClO_4 solution are very reversible with an ultrahigh capacity efficiency, so the HClO_4 acts as a stable support electrolyte with higher ionic conductivity than the traditional H_2SiF_6 electrolyte. The results of the scale-up experiments show that under the optimal conditions of 2.8 mol·L~(-1) HClO_4, 0.4 mol·L~(-1) Pb(ClO_4)2 and electrolysis temperature of 45 ℃, the energy consumption is as low as 24.5 kW·h·(t Pb)~(-1) , only about 20% of that by Betts method at the same current density of 20 mA·cm~(-2), and the purity of the refined lead is up to 99.9992%, much higher than that specified by Chinese national standard(99.994%, GB/T 469-2013) and European standard(99.99%, EN 12659–1999).  相似文献   

5.
搭建了鼓泡床碳酸化反应器,研究常温常压下电石渣直接液相碳酸化矿化封存CO2的能力,揭示了重要操作参数表观气速、液固比和CO2浓度对电石渣矿化封存CO2能力和碳酸化效率的影响规律。同时构建响应面模型,分析各参数对电石渣碳酸化效率的影响强度,优化获得最大碳酸化效率及相应操作工况。结果表明,增加气速有利于钙离子溶解和CO2吸收,但反应器中过高气速易导致气相通道效应,不利于气液充分接触。当液固比降低,溶液中钙离子浓度提高,更有利于碳酸化反应,但液固比过低会影响固液间传质。适当增加CO2浓度有利于提高碳酸化效率,但CO2浓度增至到一定值后,对碳酸化效率影响降低。响应面建模分析发现,各因素对碳酸化效率影响顺序为:液固比>CO2浓度>表观气速。优化结果发现碳酸化效率最高为93.58%,工况为表观气速0.07m/s,液固比为8.26mL/g和CO2体积分数为20.91%。研究可知,鼓泡床中常温常压下电石渣直接液相加速碳酸化反应,具有较大的CO2固定量和高的碳酸化效率,实验结果为电石渣加速矿化封存CO2技术的发展提供了基础数据。  相似文献   

6.
张亚萍 《无机盐工业》2022,54(8):96-100
有机胺法是最有效的燃煤烟气二氧化碳(CO2)捕集技术之一。使用Aspen plus模拟乙醇胺(MEA)捕获烟气CO2的过程,先进行单独的吸收塔与再生塔模拟,在单独系统模型收敛的基础上,再进行吸收-解吸的综合模拟。在入塔烟气流量为8.22 m3/min、CO2物质的量分数为0.18、MEA流量为2 311.3 kg/h、MEA物质的量分数为0.12条件下,MEA捕集燃煤烟气中CO2的模拟结果: CO2脱除率为69.3%,净化气中CO2物质的量分数为5.33×10-2,再生塔顶再生气中CO2物质的量分数为0.956,基本达到了设计要求。此为更深入地开展胺法吸收CO2的研究提供了依据。  相似文献   

7.
SAPO-34 zeolite membranes show high efficiency for CO2/CH4 separation but suffer from the reduction of separation performance when exposed to humid atmosphere. In this work, n-dodecyltrimethoxysilane (DTMS) was used to modify the hollow fibers supported SAPO-34 membranes to increase the external surface hydrophobicity and thus sustain their performance under moisture environment. The modified membranes were fully characterized. Their separation performance was extensively investigated in both dry and wet gaseous systems and compared with the un-modified ones. The un-modified SAPO-34 membrane exhibited a high separation selectivity of 160 and CO2 permeance of 1.18×10-6 mol·m-2·s-1·Pa-1 for separation of dry CO2/CH4 at 298 K. However, its separation selectivity declined to 0.9 and the CO2 permeance was only about 1.7×10-8 mol·m-2·s-1·Pa-1 for wet CO2/CH4 at same temperature. High temperature (e.g. 353 K) could reduce the effect of moisture to improve SAPO-34 separation selectivity, but further increasing temperature (e.g. 373 K) led to decrease in CO2/CH4 separation selectivity. A significant decrease of selectivity was observed at higher pressure drop. The modified SAPO-34 membrane showed decreased CO2 permeance but increased separation selectivity for dry CO2/CH4 gas mixture, and super performance for wet CO2/CH4 gas mixture due to the improved hydrophobicity of membrane surface. A separation selectivity of 65 and CO2 permeance of 4.73×10-8 mol·m-2·s-1·Pa-1 for wet CO2/CH4 mixture can be observed at 353 K with a pressure drop of 0.4 MPa. Furthermore, the modified membrane exhibited stable separation performance during the 120-hour test for wet CO2/CH4 mixture at 353 K. The hydrophobic modification paves a way for SAPO-34 membranes in real applications.  相似文献   

8.
The use of hybrid advanced oxidation processes(AOPs) for the removal of pollutants from industrial effluents has been extensively studied in recent literature. The aim of this study is to compare the performance of the photo,Fenton, photo-Fenton and ozone–photo–Fenton processes in terms of color removal and chemical oxygen demand(COD) removal of distillery industrial effluent together with the associated electrical energy per order. It was observed from the experimental results that the O_3/UV/Fe~(2 +)/H_2O_2 process yielded a 100% color and95.50% COD removals with electrical energy per order of 0.015 k W·h·m~(-3) compared to all other combinations of the AOPs. The effects of various operating parameters such as H_2O_2 and Fe~(2+) concentration, effluent pH, COD concentration and UV power on the removal of color, COD and electrical energy per order for the ozone–photo–Fenton process was critically studied and reported. The color and COD removals were analyzed using a UV/Vis spectrometer and closed reflux method.  相似文献   

9.
CO2矿物封存技术研究进展   总被引:1,自引:0,他引:1       下载免费PDF全文
CO2捕集与封存技术是目前实现碳减排最有效的方法。其中,CO2矿物封存(又称CO2矿化)是利用CO2与含钙镁硅酸盐矿物进行反应使CO2以稳定的碳酸盐形式永久储存起来。本文首先介绍了CO2矿化的基本原理和技术路线,其中间接矿化反应条件较温和、矿化效率更高、得到的产物也更纯,因此对于CO2间接矿化的研究也更广泛。本文综述并对比了天然矿物及工业固废矿化CO2的研究进展,指出工业固废更有利于CO2矿化过程。工业固废矿化CO2过程矿化CO2的同时处理了工业固废,实现以废治废,因此它在经济上也是具有一定优势。在此基础上,本文以高炉渣为代表,介绍了其矿化CO2的详细研究进展,指出采用可循环的助剂、回收高炉渣中有价元素可提升矿化过程经济性。对于CO2矿化过程的放大试验、生命周期的评估及低能耗的新工艺开发将是CO2矿物封存实现工业化的关键。  相似文献   

10.
SSZ-13 membranes with high separation performances were prepared using ball-milled nanosized seeds by once hydrothermal synthesis. Separation performances of SSZ-13 membranes in CO_2/CH_4 and N_2/CH_4 mixtures were enhanced after synthesis modification. Single-gas permeances of CO_2, N_2 and CH_4 and ideal selectivities were recorded through SSZ-13 membranes. The effects of temperature, pressure, feed flow rate and humidity on separation performance of the membranes were discussed. Three membranes prepared after synthesis modifications had an average CO_2 permeance of 1.16 × 10~(-6) mol·(m~2· s·Pa)~(-1)(equal to 3554 GPU) with an average CO_2/CH_4 selectivity of 213 in a 50 vol%/50 vol% CO_2/CH_4 mixture. It suggests that membrane synthesis has a good reproducible. The membrane also displayed a N_2 permeance of 1.07 × 10~(-7) mol·(m~2·s·Pa)~(-1)(equal to 320 GPU) with a N_2/CH_4 selectivity of 13 for a 50 vol%/50 vol% N_2/CH_4 mixture. SSZ-13 membrane displayed stable and good separation performance in the wet CO_2/CH_4 mixture for a long test period over 100 h at 348 K. The current SSZ-13 membranes show great potentials for the simultaneous removals of CO_2 and N_2 in natural gas purification as a facile process suitable for industrial application.  相似文献   

11.
马晓彤  李英杰  王文静  张婉  王泽岩 《化工学报》2016,67(12):5268-5275
提出在碳酸化气氛中间歇加入HCl(间歇氯化)提高电石渣在循环煅烧/碳酸化反应中捕集CO2性能的新思路。在双固定床反应器上,在不同循环次数加入HCl、碳酸化温度、CO2/HCl体积比等条件下,研究HCl间歇加入对电石渣循环碳酸化特性的影响。结果表明,在循环煅烧/碳酸化反应中间歇加入HCl使电石渣间歇氯化能提高其循环捕集CO2性能。在前N次循环碳酸化时加入0.1% HCl,当N=4时能使电石渣获得最优CO2捕集性能,第10个循环时的CO2吸收量比无HCl时提高了51%。HCl与CaCO3发生氯化反应,破坏致密产物层对CO2扩散的阻碍,提高了电石渣的碳酸化转化率。在碳酸化气氛加入HCl时,最佳碳酸化温度仍为700℃。随CO2/HCl体积比增大,HCl对电石渣捕集CO2性能的促进作用减弱。  相似文献   

12.
在“碳达峰、碳中和”的背景下,传统煤制甲醇工艺存在CO2排放强度大、能耗高等问题成为制约煤制甲醇工艺发展的瓶颈问题。本研究基于外源性的绿氢,重构粉煤气化煤制甲醇工艺,省掉了空分单元、变换单元,开发了短流程低温甲醇洗单元,提出了粉煤气化集成绿氢的近零碳排放煤制甲醇新工艺。从碳元素利用率、CO2排放、成本分析等角度对新工艺进行了评价。结果表明,与传统煤制甲醇工艺相比,新工艺碳元素利用率从41.50%提高到95.77%,CO2直接排放量由1.939降低至0.035 t·(t MeOH)-1,通过分析H2价格与碳税对产品成本的影响发现,当氢气价格和碳税分别为10.36 CNY·(kg H2)-1和223.3 CNY·(t CO2)-1时,两种工艺的产品成本相当。新工艺不仅减少了煤制甲醇过程碳排放,而且可以提高可再生能源就地消纳能力,具有良好的应用前景。  相似文献   

13.
刘冰  孙伟娜  安亚雄  江南  汪亚燕  邢瑞  张东辉 《化工学报》2018,69(11):4788-4797
针对日益严重的温室效应及传统CO2捕集和储存技术的不足,设计带循环的二阶四塔变压吸附装置捕集电厂烟道气中的二氧化碳,采用炭分子筛作为第一阶二塔处理装置吸附剂,采用13X作为第二阶二塔处理装置的吸附剂。建立上述工艺的数学模型,通过实验验证数学模型和模拟结果的准确性。模拟结果表明,本工艺可以将烟道气中的CO2(15%)富集为纯度95%的产品气,收率为93.92%,工艺处理量为4.576 mol CO2·h-1·kg-1,能耗为0.847 MJ·(kg CO2-1,通过对比,本工艺具有处理量大、回收率高、纯度高的优点。在此基础上,根据数学模型分析二阶床层在一个周期内的压力变化、温度分布、固相和气相组成分布、能耗组成、生产能力。  相似文献   

14.
Post-combustion CO2 capture (PCC) process faces significant challenge of high regeneration energy consumption. Biphasic absorbent is a promising alternative candidate which could significantly reduce the regeneration energy consumption because only the CO2-concentrated phase should be regenerated. In this work, aqueous solutions of triethylenetetramine (TETA) and N,N-diethylethanolamine (DEEA) are found to be efficient biphasic absorbents of CO2. The effects of the solvent composition, total amine concentration, and temperature on the absorption behavior, as well as the effect of temperature on the desorption behavior of TETA-DEEA-H2O system were investigated. An aqueous solution of 1 mol·L-1 TETA and 4 mol·L-1 DEEA spontaneously separates into two liquid phases after a certain amount of CO2 is absorbed and it shows high CO2 absorption/desorption performance. About 99.4% of the absorbed CO2 is found in the lower phase, which corresponds to a CO2 absorption capacity of 3.44 mol·kg-1. The appropriate absorption and desorption temperatures are found to be 30℃ and 90℃, respectively. The thermal analysis indicates that the heat of absorption of the 1 mol·L-1 TETA and 4 mol·L-1 DEEA solution is -84.38 kJ·(mol CO2)-1 which is 6.92 kJ·(mol CO2)-1 less than that of aqueous MEA. The reaction heat, sensible heat, and the vaporization heat of the TETA-DEEA-H2O system are lower than that of the aqueous MEA, while its CO2 capacity is higher. Thus the TETA-DEEA-H2O system is potentially a better absorbent for the post-combustion CO2 capture process.  相似文献   

15.
The industrial products or wastewater rich in the mixed salts(Cl~-/SO_4~(2-)) not only causes the environmental damage, but also induces waste of resource. In this study, an ED stack with monovalent selective AEMs and conventional CEMs was employed to separate the Cl~-and SO_4~(2-)from simulated wastewater. The effect of current density and mass fraction percentage was investigated in order to optimize the experimental conditions during ED process. It was found that at a concentration ratio between NaCl and Na_2SO_4 of 95/5(wt%/wt%) and a current density of40 m A·cm~(-2), a current efficiency of 72%, an energy consumption of 1.6 k W·h·kg~(-1) Na Cl and a Cl~-/SO_4~(2-)concentration(67.5/3.5 g·L~(-1)) were obtained. Hence, it is appropriate and effective to separate Cl~-and SO_4~(2-)by ED using the monovalent selective AEMs.  相似文献   

16.
在二氧化碳捕集、利用和封存(CCUS)技术中,海水固碳技术绿色环保、安全可靠,具有很好的发展前景。其中,双极膜电渗析法海水固碳技术的关键之处在于二氧化碳在系统中的溶解吸收。考察了结晶器中添加晶种、通气体系成分、模拟烟道气流量、双极膜电渗析装置的电流密度对海水固碳过程中二氧化碳溶解吸收效果的影响,结果表明:系统外加晶种、模拟烟道气作为通气体系时更有利于二氧化碳在双极膜电渗析系统中的溶解吸收,促进碳酸钙生成。在上述基础上,随着模拟烟道气流量的增加,二氧化碳的比吸收速率降低,二氧化碳在溶液中大部分转化成碳酸氢根,碳酸根和碳酸钙的生成速率则会降低;随着电渗析装置电流密度的提高,碳酸氢根、碳酸根和碳酸钙的生成速率均会随之提高。该研究为酸性气体在双极膜电渗析系统中溶解吸收和矿化利用提供了指导。  相似文献   

17.
Two-dimensional (2D) titanium carbide MXene Ti3C2 has attracted significant research interest in energy storage applications. In this study, we prepared Chl@Ti3C2 composites by simply mixing a chlorophyll derivative (e.g., zinc methyl 3-devinyl-3-hydroxymethyl- pyropheophorbide a (Chl)) and Ti3C2 in tetrahydrofuran, where the Chl molecules were aggregated among the multi-layered Ti3C2 MXene or on its surface, increasing the interlayer space of Ti3C2. The as-prepared Chl@Ti3C2 was employed as the anode material in the lithium-ion battery (LIB) with lithium metal as the cathode. The resulting LIB exhibited a higher reversible capacity and longer cycle performance than those of LIB based on pure Ti3C2, and its specific discharge capacity continuously increased along with the increasing number of cycles, which can be attributed to the gradual activation of Chl@Ti3C2 accompanied by the electrochemical reactions. The discharge capacity of 1 wt-% Chl@Ti3C2 was recorded to be 325 mA·h·g–1 at the current density of 50 mA·g–1 with a Coulombic efficiency of 56% and a reversible discharge capacity of 173 mA·h·g–1 at the current density of 500 mA·g–1 after 800 cycles. This work provides a novel strategy for improving the energy storage performance of 2D MXene materials by expanding the layer distance with organic dye aggregates.  相似文献   

18.
Different VSA(Vacuum Swing Adsorption) cycles and process schemes have been evaluated to find suitable process configurations for effectively separating CO2 from flue gases from different industrial sectors. The cycles were studied using an adsorption simulator developed in our research group, which has been successfully used to predict experimental results over several years. Commercial zeolite APGIII and granular activated carbon were used as the adsorbents. Three-bed VSA cycles with- and without-product purge and 2-stage VSA systems have been investigated. It was found that for a feed gas containing 15% CO2(representing flue gas from power plants), high CO2 purities and recoveries could be obtained using a three-bed zeolite APGIII VSA unit for one stage capture, but with more stringent conditions such as deeper vacuum pressures of 1–3 k Pa. 2-stage VSA process operated in series allowed us to use simple process steps and operate at more realistic vacuum pressures. With a vacuum pressure of 10 k Pa, final CO2 purity of 95.3% with a recovery of 98.2% were obtained at specific power consumption of 0.55 MJ·(kg CO2)-1from feed gas containing15% CO2. These numbers compare very well with those obtained from a single stage process operating at1 k Pa vacuum pressure. The feed CO2 concentration was very influential in determining the desorption pressure necessary to achieve high separation efficiency. For feed gases containing N 30% CO2, a singlestage VSA capture process operating at moderate vacuum pressure and without a product purge, can achieve very high product purities and recoveries.  相似文献   

19.
富氧燃烧技术是目前最有可能大规模推广和商业应用的碳捕集与封存技术之一,其中,烟气压缩净化及CO2提纯对于整个富氧燃烧系统至关重要。然而,目前研究多聚焦于富氧燃烧后烟气压缩净化的工艺验证,而对烟气压缩纯化各单元运行特性的研究仍不深入,特别是烟气压缩净化过程杂质污染组分的迁移转化、系统运行参数与污染物脱除效率的关联仍不明确。且现有研究对净化后烟气的深度提纯及高浓度CO2制备的关注也相对较少,直接关系到富氧燃烧系统运行经济性。因此,针对富氧燃烧烟气净化及CO2提纯需求,系统探究了富氧燃烧烟气压缩纯化过程SO2、NOx吸收脱除以及CO2深度提纯等各子系统的运行特性,其中SO2与NOx脱除采用压缩-酸液吸收,CO2深度提纯采用低温精馏。结果表明:通过烟气净化可实现SO2脱除效率达100%,NO脱除效率达99%,同时实现纯度为99.99%的食品级液态CO2制备。烟气净化过程中,气相反应占据主导,提高压力可缩短反应时间;当SO2吸收塔运行压力超过0.8 MPa时,SO2脱除效率可达100%;当NO吸收塔运行压力超过3.0 MPa时,NO排放浓度可达超低排放标准。CO2提纯过程中,提高压力会降低液体CO2纯度。SO2吸收塔运行压力为1.6 MPa、NO吸收塔运行压力为3.0 MPa、CO2提纯塔运行压力为3.8 MPa时,系统整体功耗最低,为0.37 MJ/kg。  相似文献   

20.
To solve the problems generally encountered during the plasma electrolytic oxidation (PEO) of Al alloys with high Si content, a pretreatment of chemical etching was applied before the process. The influence of such pre-treatment was studied by SEM, EDS and XRD. The pretreatment presents a significant effect on positive voltage at the beginning stage of PEO, leading to higher voltage over the whole process. The difference between the pos-itive voltages of non-etched and etched specimens decreases gradual y with the increase of processing time. The pretreatment exhibits much less influence on the negative voltage. For the sample with surface pretreatment, the average growth rate of PEO coating is increased from 0.50 to 0.84μm·min?1 and the energy consumption is de-creased from 6.30 to 4.36 kW·h·μm?1·m?2. At the same time, both mullite and amorphous SiO2 contents are decreased in the coating.  相似文献   

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