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1.
Carbon dioxide (CO2) adsorption on a standard metal-organic framework Mg2(dobdc) (Mg/DOBDC or Mg-MOF-74) and a tetraethylenepentamine (TEPA) modified Mgz(dobdc) (TEPA-Mg/DOBDC) were investigated and compared. The structural information, surface chemistry and thermal behavior of the adsorbent samples were characterized by X-ray powder diffraction (XRD), infrared spectroscopy (IR), thermogravimetric analysis (TGA) and nitrogen adsorption-desorption isotherm analysis. CO2 adsorption capacity was measured by dynamic adsorption experiments with N2-CO2 mixed gases at 60℃. Results showed that the CO2 adsorption capacity of Mg/DOBDC was significantly improved after amine modification, with an increase from 2.67 to 6.06 mmol CO2/g adsorbent. Moreover, CO2 adsorption on the TEPA-Mg/DOBDC adsorbent was promoted by water vapor, and the adsorption capacity was enhanced to 8.31 mmol CO2/g absorbent. The adsorption capacity of the TEPA-Mg/DOBDC adsorbent dropped only 3% after 5 consecutive adsorption]desorption cycles. Therefore, this kind of adsorbent can be considered as a promising material for the capture of CO2 from flue gas.  相似文献   

2.
Mesoporous carbon adsorbents, having high nitrogen content, were synthesized via nanocasting technique with melamine–formaldehyde resin as precursor and mesoporous silica as template. A series of adsorbents were prepared by varying the carbonization temperature from 400 to 700°C. Adsorbents were characterized thoroughly by nitrogen sorption, X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), thermogravimetric analysis (TGA), elemental (CHN) analysis, Fourier transform infrared (FTIR) spectroscopy and Boehm titration. Carbonization temperature controlled the properties of the synthesized adsorbents ranging from surface area to their nitrogen content, which play major role in their application as adsorbents for CO2 capture. The nanostructure of these materials was confirmed by XRD and TEM. Their nitrogen content decreased with an increase in carbonization temperature while other properties like surface area, pore volume, thermal stability and surface basicity increased with the carbonization temperature. These materials were evaluated for CO2 adsorption by fixed-bed column adsorption experiments. Adsorbent synthesized at 700°C was found to have the highest surface area and surface basicity along with maximum CO2 adsorption capacity among the synthesized adsorbents. Breakthrough time and CO2 equilibrium adsorption capacity were investigated from the breakthrough curves and were found to decrease with increase in adsorption temperature. Adsorption process for carbon adsorbent–CO2 system was found to be reversible with stable adsorption capacity over four consecutive adsorption–desorption cycles. From three isotherm models used to analyze the equilibrium data, Temkin isotherm model presented a nearly perfect fit implying the heterogeneous adsorbent surface.  相似文献   

3.
Mesoporous carbon adsorbents, having high nitrogen content, were synthesized via nanocasting technique with melamine–formaldehyde resin as precursor and mesoporous silica as template. A series of adsorbents were prepared by varying the carbonization temperature from 400 to 700°C. Adsorbents were characterized thoroughly by nitrogen sorption, X-ray diffraction(XRD), scanning electron microscopy(SEM), transmission electron microscopy(TEM), thermogravimetric analysis(TGA), elemental(CHN) analysis, Fourier transform infrared(FTIR) spectroscopy and Boehm titration. Carbonization temperature controlled the properties of the synthesized adsorbents ranging from surface area to their nitrogen content, which play major role in their application as adsorbents for CO_2 capture.The nanostructure of these materials was confirmed by XRD and TEM. Their nitrogen content decreased with an increase in carbonization temperature while other properties like surface area, pore volume, thermal stability and surface basicity increased with the carbonization temperature. These materials were evaluated for CO_2 adsorption by fixed-bed column adsorption experiments. Adsorbent synthesized at 700°C was found to have the highest surface area and surface basicity along with maximum CO_2 adsorption capacity among the synthesized adsorbents. Breakthrough time and CO_2 equilibrium adsorption capacity were investigated from the breakthrough curves and were found to decrease with increase in adsorption temperature. Adsorption process for carbon adsorbent–CO_2 system was found to be reversible with stable adsorption capacity over four consecutive adsorption–desorption cycles. From three isotherm models used to analyze the equilibrium data, Temkin isotherm model presented a nearly perfect fit implying the heterogeneous adsorbent surface.  相似文献   

4.
N-doped mesoporous alumina has been synthesized using chitosan as the biopolymer template. The adsorbent has been thoroughly investigated for the adsorption of CO2 from a simulated flue gas stream (15% CO2 balanced with N2) and compared with commercially available mesoporous alumina procured from SASOL, Germany. CO2 adsorption was studied under different conditions of pre-treatment and adsorption temperature, inlet CO2 concentration and in the presence of oxygen and moisture. The adsorption capacity was determined to be 29.4 mg CO2/g of adsorbent at 55℃. This value was observed to be 4 times higher in comparison to that of commercial mesoporous alumina at a temperature of 55℃. Basicity of alumina surface coupled with the presence of nitrogen in template in synthesized sample is responsible for this enhanced CO2 adsorption. Adsorption capacity for CO2 was retained in the presence of oxygen; however moisture had a deteriorating effect on the adsorption capacity reducing it to nearly half the value.  相似文献   

5.
CO2 is the main greenhouse gas which causes global climatic changes on larger scale. Many techniques have been utilised to capture CO2. Membrane gas separation is a fast growing CO2 capture technique, particularly gas separation by composite membranes. The separation of CO2 by a membrane is not just a process to physically sieve out of CO2 through the controlled membrane pore size. It mainly depends upon diffusion and solubility of gases, particularly for composite dense membranes. The blended components in composite membranes have a high capability to adsorb CO2. The adsorption kinetics of the gases may directly affect diffusion and solubility. In this study, we have investigated the adsorption behaviour of CO2 in pure and composite membranes to explore the complete understanding of diffusion and solubility of CO2 through membranes. Pure cellulose acetate (CA) and cellulose acetate-titania nanoparticle (CA-TiO2) composite membranes were fabricated and characterised using SEM and FTIR analysis. The results indicated that the blended CA-TiO2 membrane adsorbed more quantity of CO2 gas as compared to pure CA membrane. The high CO2 adsorption capacity may enhance the diffusion and solubility of CO2 in the CA-TiO2 composite membrane, which results in a better CO2 separation. The experimental data was modelled by Pseudo first-order, pseudo second order and intra particle diffusion models. According to correlation factor R2, the Pseudo second order model was fitted well with experimental data. The intra particle diffusion model revealed that adsorption in dense membranes was not solely consisting of intra particle diffusion.  相似文献   

6.
利用海藻酸钠包埋和戊二醛交联法固定碳酸酐酶,并在立式反应器进行了固定化酶吸收CO2的特性实验.实验结果表明:固定化酶的酶活力回收率是56.3%;固定化酶显著加快模拟烟气中CO2的吸收;载酶量小时,气体流量是影响吸收CO2效果的主要因素,气体流量增大,载酶量成为主要因素;气体流量增大,载酶量对反应终止p H的影响减小;载酶量增大,气体流量对反应终止p H的影响减小;气体流量增大,CO2吸收效率下降,载酶量提高,CO2吸收效率上升;气体流量为650 m L·min-1和载酶量为1 mg时,固定化酶催化吸收CO2效果显著;固定化酶具有较高的操作稳定性;SEM显示反应后的固定化酶表面出现大量形状不规则的小孔,空隙结构变得发达.  相似文献   

7.
TiO2 nanotubes (TiNT) were prepared by a hydrothermal treatment and modified by three kinds of amines,namely ethylenediamine,polyetherimide and tetraethylenepentamine (TEPA),to study their CO2 adsorption properties from gas streams.The resultant samples were characterized by X-ray diffraction,transmission electron microscopy,and infrared spectroscopy,as well as low temperature N 2 adsorption.CO2 capture was investigated in a dynamic packed column at 30℃.TEPA-modified TiO2 nanotubes showed the highest adsorption capacity of 167.64 mg/g because it had the highest amino-group content among the three amines.CO2 fixation on TiNT impregnated by TEPA was investigated at 30,50,and 70℃,and the adsorption capacity increased slightly with temperature.Following the adsorption step,the sorbents were regenerated by temperature programmed desorption,and the TiNT-TEPA sample,as CO2 sorbent,was found to be readily regenerated and energy-efficient.The cycle test also revealed that the TiNT-TEPA adsorbent is fairly stable,with only a 5% drop in the adsorption capacity after 10 adsorption/desorption cycles.In addition,the CO2 adsorption behavior was investigated with the deactivation model,and which showed an excellent prediction for the TiNT-TEPA breakthrough curves.  相似文献   

8.
In this study,a series of polyetherimide/SBA-15: 2-D hexagonal P6 mm,Santa Barbara USA(PEI/SBA-15) adsorbents modified by phosphoric ester based surfactants(including tri(2-ethylhexyl)phosphate(TEP),bis(2-ethylhexyl) phosphate(BEP) and trimethyl phosphonoacetate(TMPA))were prepared for CO_2 adsorption.Experimental results indicated that the addition of TEP and BEP had positive effects on CO_2 adsorption capacity over PEI/SBA-15.In particular,the CO_2 adsorption amount could be improved by around 20% for 45PEI–5TEP/SBA-15 compared to the additive-free adsorbent.This could be attributed to the decrease of CO_2 diffusion resistance in the PEI bulk network due to the interactions between TEP and loaded PEI molecules,which was further confirmed by adsorption kinetics results.In addition,it was also found that the cyclic performance of the TEP-modified adsorbent was better than the surfactant-free one.This could be due to two main reasons,based on the results of in situ DRIFT and TG-DSC tests.First and more importantly,adsorbed CO_2 species could be desorbed more rapidly over TEP-modified adsorbent during the thermal desorption process.Furthermore,the enhanced thermal stability after TEP addition ensured lower degradation of amine groups during adsorption/desorption cycles.  相似文献   

9.
The objective of this research was to investigate CO_2adsorption capacity of tetraethylenepentamine-functionalized basic-modified calcined hydrotalcite(TEPA/b-c HT)sorbents at atmospheric pressure formed under varying TEPA loading levels,temperatures,sorbent weight to total gaseous flow rate(W/F)ratios and CO_2concentrations in the influent gas.The TEPA/b-c HT sorbents were characterized by means of X-ray diffraction(XRD),Fourier transform infrared spectrometry(FT–IR),thermal gravimetric analysis(TGA),Brunauer–Emmet–Teller(BET)analysis of nitrogen(N_2)adsorption/desorption and carbon–hydrogen–nitrogen(CHN)elemental analysis.Moreover,a full 2~4factorial design with three central points at a 95%confidence interval was used to screen important factor(s)on the CO_2adsorption capacity.It revealed that85.0%variation in the capacity came from the influence of four main factors and the15.0%one was from their interactions.A face-centered central composite design response surface method(FCCCD–RSM)was then employed to optimize the condition,the maximal capacity of 5.5–6.1 mmol/g was achieved when operating with a TEPA loading level of 39%–49%(W/W),temperature of 76–90°C,W/F ratio of 1.7–2.60(g·sec)/cm~3and CO_2concentration of 27%–41%(V/V).The model fitted sufficiently the experimental data with an error range of±1.5%.From cyclical adsorption/desorption and selectivity at the optimal condition,the 40%TEPA/b-c HT still expressed its effective performance after eight cycles.  相似文献   

10.
为了考察将电厂烟气注入采空区实现防火与气体封存的可行性,采用自制的煤大样量吸附装置测定了常温、常压条件下塔山烟煤对各种烟气成分的饱和吸附量,并对烟煤在空气和烟气氛围下对氧气的吸附行为进行了研究. 结果表明:将电厂烟气注入井下采空区,每t煤可封存约1.20 m3的CO2,烟气中SO2和NO2可全部被烟煤封存;在物理吸附阶段,烟煤对CO2的吸附量分别为对N2吸附量的13倍,对O2吸附量的41倍;在常温、常压条件下,烟煤对N2和CO2的吸附为物理吸附,12 h已基本达到饱和状态,但烟煤对O2的吸附随着时间的增加逐渐由物理吸附转变为化学吸附,因此在较长时间内未能达到平衡状态. 通过不同气体氛围下烟煤吸附氧气量的数据分析发现,将电厂烟气注入到采空区,因烟煤对氧气的吸附量降低了29%,可有效抑制其自燃反应的进行. 研究显示,电厂烟气注入采空区可实现节能减排和灾害治理的统一.   相似文献   

11.
The influence of CO2 content and presence of SO2 on the sequestration of CO2 by municipal solid waste incinerator(MSWI) fly ash was studied by investigating the carbonation reaction of MSWI fly ash with different combinations of simulated flue gas.The reaction between fly ash and 100% CO2 was relatively fast;the uptake of CO2 reached 87g CO2/kg ash,and the sequestered CO2 could be entirely released at high temperatures.When CO2 content was reduced to 12%,the reaction rate decreased;the uptake fell to 41g CO2/kg ash,and 70.7% of the sequestered CO2 could be released.With 12% CO2 in the presence of SO2,the reaction rate significantly decreased;the uptake was just 17g CO2/kg ash,and only 52.9% of the sequestered CO2 could be released.SO2 in the simulated gas restricted the ability of fly ash to sequester CO2 because it blocked the pores of the ash.  相似文献   

12.
To decrease the operating cost of flue gas purification technologies based on carbon-based materials, the adsorption and regeneration performance of low-price semi-coke and activated coke were compared for SO2 and NO removal in a simulated flue gas. The functional groups of the two adsorbents before and after regeneration were characterized by a Fourier transform infrared (FTIR) spectrometer, and were quantitatively assessed using temperature programmed desorption (TPD) coupled with FTIR and acid–base titration. The results show that semi-coke had higher adsorption capacity (16.2% for SO2 and 38.6% for NO) than activated coke because of its higher content of basic functional groups and lactones. After regeneration, the adsorption performance of semi-coke decreased because the number of active functional groups decreased and the micropores increased. Semi-coke had better regeneration performance than activated coke. Semi-coke had a larger SO2 recovery of 7.2% and smaller carbon consumption of 12% compared to activated coke. The semi-coke carbon-based adsorbent could be regenerated at lower temperatures to depress the carbon consumption, because the SO2 recovery was only reduced a small amount.  相似文献   

13.
A series of MgO-based adsorbents were prepared through solution–combustion synthesis and ball-milling process.The prepared MgO-based powders were characterized using X-ray diffraction,scanning electron microscopy,N_2 physisorption measurements,and employed as potential adsorbents for CO_2 adsorption.The influence of structural and textural properties of these adsorbents over the CO_2 adsorption behaviour was also investigated.The results showed that MgO-based products prepared by solution–combustion and ball-milling processes,were highly porous,fluffy,nanocrystalline structures in nature,which are unique physico-chemical properties that significantly contribute to enhance their CO_2 adsorption.It was found that the MgO synthesized by solution combustion process,using a molar ratio of urea to magnesium nitrate(2:1),and treated by ball-milling during 2.5 hr(MgO-BM2.5h),exhibited the maximum CO_2 adsorption capacity of 1.611 mmol/g at 25℃ and 1 atm,mainly via chemisorption.The CO_2 adsorption behaviour on the MgO-based adsorbents was correlated to their improved specific surface area,total pore volume,pore size distribution and crystallinity.The reusability of synthesized MgO-BM2.5h was confirmed by five consecutive CO_2adsorption–desorption times,without any significant loss of performance,that supports the potential of MgO-based adsorbent.The results confirmed that the special features of MgO prepared by solution–combustion and treated by ball-milling during 2.5 hr are favorable to be used as effective MgO-based adsorbent in post-combustion CO_2 capture technologies.  相似文献   

14.
树脂基固态胺吸附剂室温下对低浓度CO2的吸附性能研究   总被引:2,自引:1,他引:1  
以大孔甲基丙烯酸酯吸附树脂为载体,聚乙烯亚胺(PEI)为有机胺,采用液相浸渍法制备出固态胺吸附剂,并研究了其在室温下对低浓度CO2的吸附行为.同时,利用氮气吸附、热重分析和扫描电镜表征了材料的物理化学性质,并采用热重法和固定床吸附法考察了材料的CO2吸附性能.结果表明,大孔树脂担载50%PEI(质量分数)时吸附性能最佳,对纯CO2的最大吸附量为175 mg·g-1;CO2的吸附行为由扩散动力学与吸附热力学共同决定,低温有利于提高吸附容量;吸附剂对400 ppm~15%浓度的CO2都具有优异的动态吸附性能,其中对400 ppm CO2的吸附量达到86 mg·g-1,对15%CO2的吸附量达到150 mg·g-1;湿度对吸附起促进作用,相对湿度为10%时,对400 ppm CO2的吸附量提高至139mg·g-1;吸附剂具有优异的循环性能,具有直接空气捕集CO2的潜力.  相似文献   

15.
The oxycoal process with cryogenic oxygen supply   总被引:1,自引:0,他引:1  
Due to its large reserves, coal is expected to continue to play an important role in the future. However, specific and absolute CO2 emissions are among the highest when burning coal for power generation. Therefore, the capture of CO2 from power plants may contribute significantly in reducing global CO2 emissions. This review deals with the oxyfuel process, where pure oxygen is used for burning coal, resulting in a flue gas with high CO2 concentrations. After further conditioning, the highly concentrated CO2 is compressed and transported in the liquid state to, for example, geological storages. The enormous oxygen demand is generated in an air-separation unit by a cryogenic process, which is the only available state-of-the-art technology. The generation of oxygen and the purification and liquefaction of the CO2-enriched flue gas consumes significant auxiliary power. Therefore, the overall net efficiency is expected to be lowered by 8 to 12 percentage points, corresponding to a 21 to 36% increase in fuel consumption. Oxygen combustion is associated with higher temperatures compared with conventional air combustion. Both the fuel properties as well as limitations of steam and metal temperatures of the various heat exchanger sections of the steam generator require a moderation of the temperatures during combustion and in the subsequent heat-transfer sections. This is done by means of flue gas recirculation. The interdependencies among fuel properties, the amount and the temperature of the recycled flue gas, and the resulting oxygen concentration in the combustion atmosphere are investigated. Expected effects of the modified flue gas composition in comparison with the air-fired case are studied theoretically and experimentally. The different atmosphere resulting from oxygen-fired combustion gives rise to various questions related to firing, in particular, with regard to the combustion mechanism, pollutant reduction, the risk of corrosion, and the properties of the fly ash or the deposits that form. In particular, detailed nitrogen and sulphur chemistry was investigated by combustion tests in a laboratory-scale facility. Oxidant staging, in order to reduce NO formation, turned out to work with similar effectiveness as for conventional air combustion. With regard to sulphur, a considerable increase in the SO2 concentration was found, as expected. However, the H2S concentration in the combustion atmosphere increased as well. Further results were achieved with a pilot-scale test facility, where acid dew points were measured and deposition probes were exposed to the combustion environment. Besides CO2 and water vapour, the flue gas contains impurities like sulphur species, nitrogen oxides, argon, nitrogen, and oxygen. The CO2 liquefaction is strongly affected by these impurities in terms of the auxiliary power requirement and the CO2 capture rate. Furthermore, the impurity of the liquefied CO2 is affected as well. Since the requirements on the liquid CO2 with regard to geological storage or enhanced oil recovery are currently undefined, the effects of possible flue gas treatment and the design of the liquefaction plant are studied over a wide range.  相似文献   

16.
In this work, the effects of different methods of activation on CO2 adsorption performance of activated carbon were studied. Activated carbons were prepared from biochar, obtained from fast pyrolysis of white wood, using three different activation methods of steam activation, CO2 activation and Potassium hydroxide (KOH) activation. CO2 adsorption behavior of the produced activated carbons was studied in a fixed-bed reactor set-up at atmospheric pressure, temperature range of 25–65°C and inlet CO2 concentration range of 10–30 mol% in He to determine the effects of the surface area, porosity and surface chemistry on adsorption capacity of the samples. Characterization of the micropore and mesopore texture was carried out using N2 and CO2 adsorption at 77 and 273 K, respectively. Central composite design was used to evaluate the combined effects of temperature and concentration of CO2 on the adsorption behavior of the adsorbents. The KOH activated carbon with a total micropore volume of 0.62 cm3/g and surface area of 1400 m2/g had the highest CO2 adsorption capacity of 1.8 mol/kg due to its microporous structure and high surface area under the optimized experimental conditions of 30 mol% CO2 and 25°C. The performance of the adsorbents in multi-cyclic adsorption process was also assessed and the adsorption capacity of KOH and CO2 activated carbons remained remarkably stable after 50 cycles with low temperature (160°C) regeneration.  相似文献   

17.
张源  他旭鹏  覃述兵  郝佑民 《环境科学》2023,44(9):5308-5315
CO2捕集、利用与封存是碳中和技术体系的重要组成部分,混凝土在大规模吸收CO2方面具有巨大的发展潜力.为了掌握CO2泡沫混凝土的碳封存潜力,分析了CO2泡沫混凝土的固碳机制,建立了CO2泡沫混凝土固碳能力的数学模型,估算了CO2泡沫混凝土的固碳和储碳能力.结果表明,CO2泡沫混凝土碳封存能力的99%以上是由混凝土骨架的化学碳化方式完成的,而泡孔的储碳能力较弱;按照30%碳化率估算,我国每年生产的混凝土在全生命周期内的碳封存量平均为2.18亿t,超过大兴安岭林区森林1 a的碳汇;近5年,我国CO2泡沫混凝土的碳封存潜力为5.80亿t ·a-1,在煤电一体化矿区的固废和废气资源化利用方面具有很好的应用前景.CO2泡沫混凝土在凝固前的稳定性是下一步要重点解决的技术难题.  相似文献   

18.
Global warming, the major environmental issue confronted by humanity today, is caused by rising level of green house gases. Carbon capture and storage technologies offer potential for tapering CO2 emission in the atmosphere. Adsorption is believed to be a promising technology for CO2 capture. For this purpose, a polyester was synthesized by polycondensation of1,3,5-benzenetricarbonyl trichloride and cyanuric acid in pyridine and dichloromethane mixture. The polymer was then characterized using FT-IR, TGA, BET surface area and pore size analysis, FESEM and CO2 adsorption measurements. The CO2 adsorption capacities of the polyester were evaluated at a pressure of 1 bar and two different temperatures(273 and 298 K).The performance of these materials to adsorb CO2 at atmospheric pressure was measured by optimum CO2 uptake of 0.244 mmol/g at 273 K. The synthesized polyester, therefore, has the potential to be exploited as CO2 adsorbent in pre-combustion capture process.  相似文献   

19.
本文考察了流动态体系中,烟气主要组分(O2和水蒸汽)的含量对SO2在活性炭上吸附量的影响;研究了SO2吸附动力学。结果表明,在一定空速和吸附温度下,烟气中O2和水蒸汽含量分别为5%和8%(Ⅴ%)左右时,SO2吸附量为最大。SO2在活性炭上吸附动力学曲线很好地遵循Elovich方程;SO2吸附活化能Ea0为21.939×103J/mol以及Elovich参数,进而得出吸附活化能Ea,与吸附温度的关系。  相似文献   

20.
高继贤  王铁峰  王金福 《环境科学》2010,31(5):1152-1159
通过动态吸附烟气脱硫实验,考察了烟气中不同SO2体积分数对ZL50脱硫脱硝活性炭脱硫行为的影响,并进行了动力学分析.随着烟气中SO2体积分数增大,脱硫率和ZL50脱硫脱硝活性炭的活性度下降;SO2吸附量和吸附速率增大.模拟结果表明,Bangham模型模拟效果最优,SO2的催化氧化反应对化学吸附有重要影响;Lagergren准一级吸附速率常数随SO2进口体积分数的增加而增大,表明SO2的催化氧化反应在吸附前期可能为速控步骤.推导和定义了Lagergren模型和Bangham模型的初始吸附速率;推导了文献上的Ho模型和Elovich模型的初始速率式。定义的Bangham初始吸附速率与初始吸附速率实验值吻合最好;建立的Bangham吸附反应动力学模型能较好地描述SO2动态吸附速率.结果表明,SO2的初始反应速率分级数为1或接近1,而O2和水蒸气的初始速率分级数分别为0.15~0.20和0.45~0.50之间的常数.  相似文献   

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