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1.
利用水热法合成Co3O4/USY复合材料,研究其对有机污染物甲苯的吸附和催化氧化特性,同时结合微波对Co3O4的精准加热特性,考察不同负载量Co3O4/USY在微波作用下的升温特性及催化甲苯氧化降解特性。结果表明,通过水热反应,Co3O4在USY表面形成多孔蜂窝状结构;负载Co3O4后的USY保持较高的吸附容量,Co3O4/USY-1.5m室温下的吸附容量为85 mg/g;Co3O4/USY在干、湿两种状态下均在325℃表现出优良的催化氧化特性、CO2选择性和稳定性;Co3O4/USY能够与微波高效耦合,快速升温启动其催化作用,控制反应温度为250℃,发现微波诱导甲苯催化氧化过程的CO2选择性优于常规催化,表明所制备Co3O4/USY复合材料具备吸附甲苯并进行微波快速再生协同有机污染物高效催化氧化降解的可行性。  相似文献   

2.
Metal-organic frameworks (MOFs) have great potentials as adsorbents for natural gas purification. However, the trade-off between selectivity and adsorption capacity remains a challenge. Herein, we report a pillared-layer metal-organic framework Ni(HBTC)(bipy) for efficiently separating the C3H8/C2H6/CH4 mixture. The experimental results show that the adsorption capacity of C3H8 and C2H6 on Ni(HBTC)(bipy) are as high as 6.18 and 5.85 mmol·g-1, while only 0.93 mmol·g-1 for CH4 at 298 K and 100 kPa. Especially, the adsorption capacity of C3H8 at 5 kPa can reach an unprecedented 4.52 mmol·g-1 and for C2H6 it is 1.48 mmol·g-1 at 10 kPa. The ideal adsorbed solution theory predicted C3H8/CH4 selectivity is as high as 1857.0, superior to most of the reported materials. Breakthrough experiment results indicated that material could completely separate the C3H8/C2H6/CH4 mixture. Therefore, Ni(HBTC)(bipy) is a promising material for separation of natural gas.  相似文献   

3.
刘有毅  黄艳  何嘉杰  肖静  夏启斌  李忠 《化工学报》2015,66(11):4469-4475
主要研究了MOF-74(Ni)材料对CO/N2/CO2的吸附分离性能。应用水热法合成制备MOF-74(Ni),分别采用全自动表面积吸附仪、P-XRD、扫描电子显微镜对材料的孔隙结构和晶体形貌进行了表征,应用静态吸附法测定了CO、N2和CO2在MOF-74(Ni)上的吸附等温线,应用DSLF方程模拟了3种气体MOF-74(Ni)上的吸附等温线,依据IAST理论模型计算了MOF-74(Ni)对CO/N2二元混合物和CO/CO2二元混合物的吸附选择性。研究结果表明:在0.1 MPa和常温条件下,MOF-74(Ni)材料对CO吸附容量高达6.15 mmol·g-1,而相同条件下N2的吸附量只有0.86 mmol·g-1。MOF-74(Ni)在低压下(0~40 kPa)对CO的吸附量明显高于其对CO2的吸附量。应用IAST模型估算MOF-74(Ni)对二元混合物吸附选择性的结果表明:MOF-74(Ni)对CO/N2混合物的吸附选择性在1000以上;MOF-74(Ni)对CO/CO2的吸附选择性在4~9范围,在所研究的二元气体混合物吸附体系中,MOF-74(Ni)都能优先吸附CO。  相似文献   

4.
以Ni(NO32·6H2O、Al(NO33·9H2O、尿素和MCNTs为原料,采用原位均相沉淀法制备了MCNTs含量(质量分数)分别为1%、3%和5%的Ni/Al-LDH/MCNTs复合电极活性材料。采用X射线衍射(XRD)、傅里叶变换红外光谱(FTIR)和场发射扫描电子显微镜(FESEM)表征了材料的微观结构和形貌;采用循环伏安(CV)、电化学交流阻抗(EIS)和充放电测试研究了该复合材料作为镍氢电池正极材料的电化学性能。结果表明,在Ni/Al-LDH中复合MCNTs能够提高材料的电化学活性,降低电化学反应电阻,显著改善材料的大电流充放电性能。其中MCNTs含量为3%的Ni/Al-LDH/MCNTs复合材料具有最佳的电化学性能,在200、500、1000和2000 mA·g-1电流密度下的放电比容量分别为330、321、307和288 mA·h·g-1,而未复合MCNTs的Ni/Al-LDH在2000 mA·g-1电流密度下放电比容量仅为205 mA·h·g-1。  相似文献   

5.
Cu3(BTC)2, a common type of metal organic framework (MOF), was synthesized through electrochemical route for CO2 capture and its separation from N2. Taguchi method was employed for optimization of key parameters affecting the synthesis of Cu3(BTC)2. The results indicated that the optimum synthesis conditions with the highest CO2 selectivity can be obtained using 1 g of ligand, applied voltage of 25 V, synthesis time of 2 h, and electrode length of 3 cm. The single gas sorption capacity of the synthetized microstructure Cu3(BTC)2 for CO2 (at 298 K and 1 bar) was a considerable value of 4.40 mmol·g−1. The isosteric heat of adsorption of both gases was calculated by inserting temperature-dependent form of Langmuir isotherm model in the Clausius-Clapeyron equation. The adsorption of CO2/N2 binary mixture with a concentration ratio of 15/85 vol-% was also studied experimentally and the result was in a good agreement with the predicted value of IAST method. Moreover, Cu3(BTC)2 showed no considerable loss in CO2 adsorption after six sequential cycles. In addition, artificial neural networks (ANNs) were also applied to predict the separation behavior of CO2/N2 mixture by MOFs and the results revealed that ANNs could serve as an appropriate tool to predict the adsorptive selectivity of the binary gas mixture in the absence of experimental data.  相似文献   

6.
徐舟  侯程  王诗琴  王佳其  庄严  贾海浪  关明云 《化工进展》2020,39(10):4088-4094
以Ni(NO3)2为原料、NaOH为沉淀剂和羟基化碳纳米管(CNT)为基质首先制备了Ni(OH)2/CNT复合材料, 然后将其于一定温度下煅烧,使其转变为NiO/CNT复合材料。用X射线粉末衍射仪(XRD)、场发射电子显微镜(FESEM)和透射电子显微镜(TEM)表征了样品的晶相与形貌,结果表明NiO纳米粒子紧密锚附在碳纳米管表面。复合材料可能的形成机理被提出。采用循环伏安法(CV)、单电极充放电和电化学阻抗研究了反应条件对其电化学性能的影响,确定最佳制备条件。将复合材料正极、活性炭负极和PVA-KOH电解质膜组装成准固态不对称超级电容器,电化学性能测试结果表明,在充放电电流密度11.2mA/cm2下,其比电容达到868.0F/g并保持稳定循环3700圈。7500次循环后,其比电容值仍有564.2F/g,显示出高的比电容和长的循环稳定性。  相似文献   

7.
采用分步浸渍法制备了碱/碱土金属修饰Ni基催化剂Ni-M/Al2O3 (M=K2CO3, Na2CO3, MgO, CaO)。探究了碱/碱土金属的添加对改性Ni基催化剂CO2吸附和甲烷化性能的影响。研究发现,碱/碱土金属的添加提高了Ni/Al2O3催化剂表面的碱性活性位点密度,强化了其CO2吸附性能。碱/碱土金属类型影响Ni-M/Al2O3催化剂碱性活性位点的分布、NiO物相的转化及Ni的分散度,进而影响其甲烷化性能。MgO添加使NiO物相转化为与载体呈强相互作用的β型和γ型NiO,降低了催化剂表面的强碱性活性位点比例,有利于CO2吸附活化。Ni-MgO/Al2O3的CO2吸附容量最高为0.68mmolCO2/g,其CO2转化率和CH4选择性分别高达58.4%和95.4%,其在烟气CO2捕集与原位甲烷化中极具应用前景。  相似文献   

8.
In this work, nitrogen-doped porous carbons (NACs) were fabricated as an adsorbent by urea modification and KOH activation. The CO2 adsorption mechanism for the NACs was then explored. The NACs are found to present a large specific surface area (1920.72– 3078.99 m2·g1) and high micropore percentage (61.60%–76.23%). Under a pressure of 1 bar, sample NAC-650-650 shows the highest CO2 adsorption capacity up to 5.96 and 3.92 mmol·g1 at 0 and 25 °C, respectively. In addition, the CO2/N2 selectivity of NAC-650-650 is 79.93, much higher than the value of 49.77 obtained for the nonnitrogen-doped carbon AC-650-650. The CO2 adsorption capacity of the NAC-650-650 sample maintains over 97% after ten cycles. Analysis of the results show that the CO2 capacity of the NACs has a linear correlation (R2 = 0.9633) with the cumulative pore volume for a pore size less than 1.02 nm. The presence of nitrogen and oxygen enhances the CO2/N2 selectivity, and pyrrole-N and hydroxy groups contribute more to the CO2 adsorption. In situ Fourier transform infrared spectra analysis indicates that CO2 is adsorbed onto the NACs as a gas. Furthermore, the physical adsorption mechanism is confirmed by adsorption kinetic models and the isosteric heat, and it is found to be controlled by CO2 diffusion. The CO2 adsorption kinetics for NACs at room temperature and in pure CO2 is in accordance with the pseudo-first-order model and Avramís fractional-order kinetic model.  相似文献   

9.
Many solid adsorbents have been prepared for the CO2 capture. In particular, the photoresponsive adsorbents have attracted extensive interests because of their tunable pore structure and variable responsive behaviors provoked by the external light. However, it is challenging to fabricate the photoresponsive adsorbents featured the big CO2 capacity and high CO2 selectivity. Herein, copolymerized between 4-phenylazobenzoyl chloride, 2,4,6-trichloro-1,3,5-triazine and melamine, a series of azobenzene-functionalized porous polymers (PTM-AZOs) are successfully synthesized. The PTM-AZOs are verified in possession of proper pore structures, large surface area and photoconductive properties through a series of characterization. The PTM-AZO-2 with the trans-isomerization exhibits the best CO2 adsorption amount of 2.7 mmol·g-1 (273 K and 0.1 MPa), while the CO2/N2 selectivity can reach 2459 and 607 on the trans- and cis-isomerization, respectively. The regulatable pore structures controlled by the photoresponsive azobenzene groups affect the CO2 capture performance of the PTM-AZOs.  相似文献   

10.
Solid amine-based adsorbents were widely studied as an alternative to liquid amine for post-combustion CO2 capture (PCC). However, most of the amine adsorbents suffer from low thermal stability and poor cyclic regenerability at the temperature of hot flue gases. Here we present an amine loaded proton type Y zeolite (HY) where the amines namely monoethanolamine (MEA) and ethylenediamine (ED) are chemical immobilized via ionic bond to the zeolite framework to overcome the amine degradation problem. The MEA and ED of 5%, 10% and 20% (mass) concentration – immobilized zeolites were characterized by X-ray diffraction, Fourier-transform infrared spectroscopy, and N2 -196 ℃ adsorption to confirm the structure integrity, amine functionalization, and surface area, respectively. The determination of the amine loading was given by C, H, N elemental analysis showing that ED has successfully grafted almost twice as many amino groups as MEA within the same solvent concentration. CO2 adsorption capacity and thermal stability of these samples were measured using thermogravimetric analyser. The adsorption performance was tested at the adsorption temperature of 30, 60 and 90 ℃, respectively using pure CO2 while the desorption was carried out with pure N2 purge at the same temperature and then followed by elevated temperature at 150 ℃. It was found that all the amine@HY have a substantial high selectivity of CO2 over N2. The sample 20% ED@HY has the highest CO2 adsorption capacity of 1.76 mmol·g-1 at 90 ℃ higher than the capacity on parent NaY zeolite (1.45 mmol·g-1 only). The amine@HY samples presented superior performance in cyclic thermal stability in the condition of the adsorption temperature of 90 ℃ and the desorption temperature of 150 ℃. These findings will foster the design of better adsorbents for CO2 capture from flue gas in post-combustion power plants.  相似文献   

11.
周建海  赵会玲  胡军  刘洪来  胡英 《化工学报》2014,65(5):1680-1687
构建了氨基修饰微孔/介孔复合材料AM-5A-MCM-41的全原子模型,采用巨正则Monte Carlo(GCMC)方法研究了它的CO2吸附分离性能,采用加权混合规则来描述氨基和CO2分子的弱化学作用。模拟结果表明,CO2分子优先吸附在复合材料介孔表面的氨基附近,CO2纯气体的吸附量和吸附热有了显著提高,而N2的吸附量和吸附热则基本不受影响。对于CO2和N2的混合气分离,由于复合材料对CO2的弱化学吸附作用,显著提高了CO2吸附量和吸附选择性,在573 K和100 kPa时CO2/N2的选择性达到了87.0。通过分子模拟研究可以从微观角度了解CO2在氨基修饰的微孔/介孔复合材料中的吸附分离的细节和机理,为实验设计和合成高效CO2吸附剂提供指导。  相似文献   

12.
A new metal-organic framework(MOF) with the chemical formula of [Ni_2 F_2(4,4'-Bipy)_2(H_2 O)_2](VO_3)_2·8 H_2 O was introduced to adsorb Pb(Ⅱ) with the highest capacity.The sorbent was characterized by thermogravimetric analysis(TGA),infrared spectroscopy(FT-IR),field-emission scanning electron microscopy(FESEM),energy-dispersive Xray(EDX),and elemental analysis.The optimum conditions were obtained by a face-centered central composite design(FCCD) as follows:adsorbent dosage(m)=1.2 mg, initial concentration of Pb(Ⅱ)(C)=390 mg·L~(-1),and pH=5.According to the Langmuir model(R~2=0.9999),the maximum monolayer uptake capacity of lead(Ⅱ) is 2400.7 mg·g~(-1),which is the highe st observed amount for lead(Ⅱ) adsorption.Neither of the old adsorbents for lead(Ⅱ)has the uptake capacity over 2000 mg·g~(-1).The model of pseudo-second-order describes well the process kinetics.The adsorption process of lead(Ⅱ) is independent of temperature changes.This compound can adsorb lead(Ⅱ) from tap water.In addition to introducing a new MOF with the highest uptake capacity for removal of Pb(Ⅱ) that is the outright novelty of this study,the concurrent modeling of both the removal percent(R) and the uptake capacity(q) is another important advantage.Because it achieves the more economical and favorable optimum conditions in comparison with the single optimization of each response.  相似文献   

13.
A new extractant, [N,N-di(2-ethylhexyl)amino]methylphenylphosphinic acid (DEAPP), was synthesized to de-velop the mutual separation techniques of In(III), Ga(III) and Zn(II). The extraction selectivity for In(III), Ga(I I) and Zn(II) with DEAPP was higher than that of the commercial phosphorus acid extractants such as D2EHPA and PC-88A. The extraction selectivity for metal ions in 1 mol·L?1 aqueous ammonium nitrate solution with DEAPP was in the following order:In(III) N Ga(III) N Zn(II). These selective extraction behaviors indicate that the amino moiety of DEAPP plays an important role in the mutual separation of In(III), Ga(III) and Zn(II). The extraction equilibria of In(I I), Ga(II ) and Zn(II) with DEAPP (=HR) were expressed by the following reactions:In3++2eHRT2?InR3eHRT+3H+, Ga3++1.5eHRT2+NO3??GaR2eHRTeNO3T+2H+, and Zn2++2eHRT2?ZnR2eHRT 2 + 2H+. The extraction equilibrium constants of In(III), Ga(III) and Zn(II) with DEAPP were determined to be Kex,M=1.7 × 104 [dm3·mol?1], 4.17 [(dm3·mol?1)0.5], and 1.55 x 10?2 [–], respectively.  相似文献   

14.
CO2加氢制甲醇既能有效缓解温室效应带来的全球气温升高问题,也能促进CO2的资源化利用,成为研究热点之一。对Cu-Zn-Al水滑石(CZA-LDH)开展改性研究,以Cu(NO3)2·3H2O、Zn(NO3)2·6H2O和Al(NO3)3·9H2O为原料,以NaOH和NaCO3为沉淀剂,采用共沉淀法制备CZA-LDH,并在制备过程中引入聚乙二醇(PEG)、聚乙烯吡咯烷酮(PVP)和三乙醇胺(TEA),焙烧后得到4组催化剂。XRD、FT-IR、N2吸附-脱附、SEM表征结果及催化性能测试数据表明,引入TEA的CZA-LDH焙烧后得到的复合金属氧化物催化剂(CZA-LDO-TEA)表现出最优的性能。这是因为TEA 能够破坏表面晶体结构,促进催化剂中CuO组分的还原,提高了 CO2的化学吸附能力,从而提高了催化剂的CO2转化率。  相似文献   

15.
采用Co(NO_3)_2对活性炭进行改性,考察浸渍浓度和吸附温度等条件对活性炭吸附NO性能的影响,并对已吸附NO的0.3 mol·L~(-1)的Co(NO_3)_2改性活性炭进行再生。通过BET、SEM、吸附等温线和FT-IR表征样品的比表面积、颗粒形貌和表面官能团。结果表明,当浸渍溶液浓度为0.3 mol·L~(-1)时,吸附效果最佳,80 min时吸附效率达88.90%。活性炭的吸附效率随着温度升高而降低,用0.3 mol·L~(-1)Co(NO_3)_2改性的活性炭在200℃时的吸附效率大于90%,并可持续50 min。SEM和FT-IR表征结果表明,在Co(NO_3)_2改性的活性炭表面和孔隙生成了Co_3O_4,促进NO催化氧化为NO_2并进行吸附。加热再生后的0.3 mol·L~(-1)Co(NO_3)_2改性活性炭对NO的吸附效率在60 min内仍高于88.90%,再生效果较好,可持续再生利用。  相似文献   

16.
The effect of oxygen concentration on the pulse and steady-state selective catalytic reduction (SCR) of NO with C3H6 over CuO/γ-Al2O3 has been studied by infrared spectroscopy (IR) coupled with mass spectroscopy studies. IR studies revealed that the pulse SCR occurred via (i) the oxidation of Cu0/Cu+ to Cu2+ by NO and O2, (ii) the co-adsorption of NO/NO2/O2 to produce Cu2+(NO3)2, and (iii) the reaction of Cu2+(NO3)2 with C3H6 to produce N2, CO2, and H2O. Increasing the O2/NO ratio from 25.0 to 83.4 promotes the formation of NO2 from gas phase oxidation of NO, resulting in a reactant mixture of NO/NO2/O2. This reactant mixture allows the formation of Cu2+(NO3)2 and its reaction with the C3H6 to occur at a higher rate with a higher selectivity toward N2 than the low O2/NO flow. Both the high and low O2/NO steady-state SCR reactions follow the same pathway, proceeding via adsorbed C3H7---NO2, C3H7---ONO, CH3COO, Cu0---CN, and Cu+---NCO intermediates toward N2, CO2, and H2O products. High O2 concentration in the high O2/NO SCR accelerates both the formation and destruction of adsorbates, resulting in their intensities similar to the low O2/NO SCR at 523–698 K. High O2 concentration in the reactant mixture resulted in a higher rate of destruction of the intermediates than low O2 concentration at temperatures above 723 K.  相似文献   

17.
A spray-drying assisted solid-state method to prepare spherical layer-structured H2TiO3 ion sieve (LSTIS) particles is reported herein. The effects of synthesis parameters (calcination temperature, calcination time, and the lithium-titanium molar ratio) on adsorption–desorption performance (the delithiation ratio, titanium dissolution loss, and the adsorption capacity) were investigated. The as-prepared LSTIS exhibited an equilibrium adsorption capacity of 30.08 mg·g-1 (average of 25.85 mg·g-1 over 5 cycles) and ultra-low titanium dissolution loss of less than 0.12% (average of 0.086% over 5 cycles). The LSTIS showed excellent selectivity toward Li+ in Na+, K+, Mg2+, and Ca2+ coexisting saline solutions where its adsorption capacity reached 27.45 mg·g-1 and the separation factors of Li+ over the coexisting cations exceeded 100. The data suggests that the LSTIS is promising to competitively enrich Li+ from saline solutions.  相似文献   

18.
Ni supported on bentonite was prepared by the impregnation method with different nickel contents, applied to the hydrogenation of nitrobenzene to aniline in a fixed-bed reactor, and it was characterized by X-ray diffraction(XRD), H_2-temperature programmed reduction(H_2-TPR), and X-ray photoelectron spectrometry(XPS). The results showed that Ni/bentonite catalyst with 20 wt% nickel content provided a higher conversion of nitrobenzene and selectivity of aniline compared to other catalysts. Ni O was the precursor of the active component of the catalyst, and the small crystallite size as well as the highly dispersed Ni O on the Ni/bentonite-20 catalyst, contributed to the catalytic performance. The hydrogenation of nitrobenzene was carried out at 300 °C with a H_2 gaseous hourly space velocity of 4800 ml·(g cat)~(-1)·h~(-1)and a nitrobenzene liquid hourly space velocity of4.8 ml·(g cat)~(-1)·h~(-1)over Ni/bentonite-20. A 95.7% nitrobenzene conversion and 98.8% aniline selectivity were obtained. While the nitrobenzene liquid hourly space velocity was 4.8 ml·(g cat)~(-1)·h~(-1), the yield of aniline was more than 95.0% during a 10-hour reaction.  相似文献   

19.
蛇纹石与绿矾耦合提取镁用于矿化二氧化碳,并富集回收蛇纹石中的镍,这为处理蛇纹石和绿矾提供了一条新的路径。为得到富镁溶液,同时从溶液中分离镍,以蛇纹石与绿矾混合焙烧-浸出后得到的溶液为研究对象,采用水解沉淀法除铁,二乙基二硫代氨基甲酸钠(DDTC)络合法分离镍镁,得到镍的产物和富镁溶液并将其用于二氧化碳矿化。结果表明,该方法能够高效地去除杂质、分离镍镁。在30℃、p H为5.0条件下,铁的去除率达97.36%,而镍、镁的损失率较低。在最佳络合条件下,镍的络合率达到99.50%,而镁的损失率仅为3.03%。此外,对络合机理进行了研究,DDTC中的特征官能团是—SH,络合之后镍和铁分别以Ni[(C2H5)2NCS2]2,Fe[(C2H5)2NCS2]3的形式存在,而镁不会被络合。富镁溶液在80℃下矿化率达92.63%。每1 000 kg蛇纹石可固定227.38 kg的二氧化碳...  相似文献   

20.
The adsorption behavior of CO2, CH4 and their mixtures in bituminous coal was investigated in this study. First, a bituminous coal model was built through molecular dynamic (MD) simulations, and it was confirmed to be reasonable by comparing the simulated results with the experimental data. Grand Canonical Monte Carlo (GCMC) simulations were then carried out to investigate the single and binary component adsorption of CO2 and CH4 with the built bituminous coal model. For the single component adsorption, the isosteric heat of CO2 adsorption is greater than that of CH4 adsorption. CO2 also exhibits stronger electrostatic interactions with the heteroatom groups in the bituminous coal model compared with CH4, which can account for the larger adsorption capacity of CO2 in the bituminous coal model. In the case of binary adsorption of CO2 and CH4 mixtures, CO2 exhibits the preferential adsorption compared with CH4 under the studied conditions. The adsorption selectivity of CO2 exhibited obvious change with increasing pressure. At lower pressure, the adsorption selectivity of CO2 shows a rapid decrease with increasing the temperature, whereas it becomes insensitive to temperature at higher pressure. Additionally, the adsorption selectivity of CO2 decreases gradually with the increase of the bulk CO2 mole fraction and the depth of CO2 injection site.  相似文献   

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