烯胺溶液吸收和解吸模拟烟气中二氧化碳实验研究

采用搅拌实验装置对二乙烯三胺(DETA)、三乙烯四胺(TETA)、三乙烯二胺(TEDA)溶液吸收和解吸模拟烟道气中二氧化碳特性进行研究,揭示了吸收速率、吸收容量和解吸速率与酸碱度、时间之间的内在联系,并与一乙醇胺(MEA)、二乙醇胺(DEA)溶液进行了对比分析。实验表明,同浓度DETA、TETA吸收速率及吸收容量均高于MEA和DEA,再生简单,是优良的烟道气CO2吸收剂,具有较高的研究价值。     

APTES修饰粉煤灰漂珠/聚苯胺的制备及性能

讨论了不同浓度γ-氨基丙基三乙氧基硅烷(APTES)甲苯溶液对粉煤灰漂珠(FAFB)硅烷化反应程度的影响,再以获得APTES修饰FAFB (FAFB-APTES)表面引入的氨基为反应点,与苯胺(An)发生聚合,制备出以FAFB-APTES为核、聚苯胺(PAn)为壳的核/壳结构复合材料(FAFB-APTES/PAn).采用化学元素分析、FTIR、XRD、SEM、TGA以及数字式四探针测试仪对复合材料结构及其性能进行分析.结果表明:APTES修饰FAFB的最佳修饰浓度为1.5 mol/L,且表面接枝率达到6.44％;SEM结果表明该种复合材料具有明显的核/壳结构;TGA分析可知引入FAFB后复合材料的热稳定性明显提高且PAn的包覆量达到28.2％;四探针技术分析可知复合材料FAFB-APTES/PAn的电导率达到5×l0-3S·cm-1,仍处于半导体的范围.     

可循环胺类吸收剂用于烟气脱碳的研究

在水相中,将二乙烯三胺(DETA)、三乙烯四胺(TETA)、四羟丙基乙二胺(EDTP)、四甲基乙二胺(TEMED)、三乙烯二胺(TEDA)分别与硼酸(H_3BO_3)等摩尔反应制得胺类烟气脱碳吸收剂。结果表明,TETA/H_3BO_3吸收剂对烟气具有良好的CO_2脱除性能和可再生性能,在吸收温度30.0℃、吸收剂浓度0.60 mol/L的吸收条件下,CO_2吸收容量为0.920 mol/L,脱碳率均大于99.5%,在恒沸温度101.5℃、时间60 min解吸条件下,初次解吸率大于72%。考察了吸收剂TETA/H_3BO_3的重复使用性能,经34次吸收-解吸循环实验结果表明,CO2吸收后富液p H为8.85±0.05,脱碳率均超过99.5%,解吸CO_2后贫液p H为10.40±0.05,后33次解吸效率均大于90%。     

可循环胺类吸收剂用于烟气脱碳的研究

在水相中,将二乙烯三胺(DETA)、三乙烯四胺(TETA)、四羟丙基乙二胺(EDTP)、四甲基乙二胺(TEMED)、三乙烯二胺(TEDA)分别与硼酸(H_3BO_3)等摩尔反应制得胺类烟气脱碳吸收剂。结果表明,TETA/H_3BO_3吸收剂对烟气具有良好的CO_2脱除性能和可再生性能,在吸收温度30.0℃、吸收剂浓度0.60 mol/L的吸收条件下,CO_2吸收容量为0.920 mol/L,脱碳率均大于99.5%,在恒沸温度101.5℃、时间60 min解吸条件下,初次解吸率大于72%。考察了吸收剂TETA/H_3BO_3的重复使用性能,经34次吸收-解吸循环实验结果表明,CO2吸收后富液p H为8.85±0.05,脱碳率均超过99.5%,解吸CO_2后贫液p H为10.40±0.05,后33次解吸效率均大于90%。     

黄铜表面硅烷自组装膜在氯化钠溶液中的耐蚀性

采用自组装技术在黄铜表面分别制备γ-巯基丙基三甲氧基硅烷(PropS-SH)、十二烷基三甲氧基硅烷(DTMS)、氨基丙基三甲氧基硅烷(APS)和γ-氯丙基三甲氧基硅烷(CPTMS)自组装膜,并分别采用电化学极化法、接触角测试和傅里叶红外光谱研究硅烷膜的耐蚀性、疏水生和结构.结果表明:经PropS-SH、DTMS和CPT...     

介孔SiO_2表面的氨基修饰及吸附性能研究

以十六胺为模板剂、正硅酸乙酯为硅源合成了多孔球形结构的介孔SiO2,用γ-氨基丙基三乙氧基硅烷(ATES)对介孔SiO2进行了表面修饰,得到了氨基嫁接介孔ATES-SiO2。利用XRD、BET、IR等方法分别测定了SiO2和ATES-SiO2的结构与性质,结果表明-NH2已成功接枝于介孔ATES-SiO2的孔道内表面。在常温常压下测得介孔SiO2和ATES-SiO2对CO2的吸附量分别为0.93 mmol/g和4.87 mmol/g。     

(3-氨丙基)三乙氧基硅烷表面修饰Fe3O4对刚果红的吸附研究

文章利用(3-氨丙基)三乙氧基硅烷(APTES)对Fe3O4纳米粒子进行表面改性,制备了有机硅表面修饰的的Fe3O4纳米粒子(APTES-MNPs)。研究了APTES-MNPs对刚果红的吸附情况。APTES-MNPs对刚果红染料的吸附符合Langmuir等温吸附模型。吸附过程为自发的并且为吸热过程。     

氧化硅片表面配基疏水性及含量对蛋白质吸附行为的影响

采用双偏振极化干涉分析技术研究了氧化硅片表面配基疏水性及含量对蛋白质质吸附行为的影响,用3种不同疏水性配基3-(氨丙基)三乙氧基硅烷(APTES)、3-(N-甲氨基丙基)三甲氧基硅烷(MAPTMS)和3-(N,N-二乙基氨丙基)三甲氧基硅烷(DAPTMS)修饰氧化硅片,通过修饰时间控制硅片表面配基含量,研究了配基疏水性对牛血清白蛋白质(BSA)的影响和配基含量(N含量)对BSA、细胞色素C和糜蛋白酶吸附行为的影响. 结果表明,BSA在疏水性最强的DAPTMS修饰的氧化硅表面吸附量及吸附动力学常数最大,分别为1.371 ng/mm2和0.056 s?1; DAPTMS含量对3种蛋白质吸附的影响与蛋白质疏水性密切相关,疏水性中等的BSA和细胞色素C为单分子层吸附,吸附量随N含量增加先增大后减小,N含量2.1%时吸附量最大,分别为16.9和60.2 nmol/m2. 疏水性较强的糜蛋白酶为多分子层吸附,吸附量随N含量增大而减小,N含量1.1%时吸附量及吸附动力学常数分别为78.6 nmol/m2和0.040 s?1.     

PS@TiO_2复合粒子及其透明超疏水涂层的制备与性能研究

以单分散聚苯乙烯(PS)纳米球为模板,经浓硫酸刻蚀、钛酸四丁酯(TBT)水解缩聚,制得草莓型PS@TiO_2复合粒子(RPTS),表面经3-氨丙基三乙氧基硅烷(APTES)修饰提升附着力。通过浸渍提拉法在玻璃表面形成透明纳米粒子涂层,涂层表面通过辛基三乙氧基硅烷(IOTES)疏水化,形成透明超疏水涂层。考察了磺化时间对复合粒子表面形貌的影响;考察了APTES用量、IOTES用量和固化温度对涂层性能的影响。结果表明:当磺化时间为25 min时,表面乳突状结构最鲜明。当APTES用量为0.04%,IOTES用量为0.2%,固化温度为80℃,涂层透光率为89.1%,静态水接触角为152°,附着力2级,硬度3H。     

硅烷偶联剂热压粘接聚酰亚胺与钛箔的研究

采用甲苯/γ-氨丙基三乙氧基硅烷(APTES)溶剂热法对聚酰亚胺(Kapton)薄膜表面硅烷化，与盐酸水热处理后的Ti箔进行热压粘接。用拉伸试验评价Kapton薄膜与Ti箔的粘接效果，用原子力显微镜(AFM)、X射线光电子能谱仪(XPS)和材料显微镜研究其粘附机理。实验结果表明：甲苯溶剂热反应使Kapton薄膜表面的羧基与APTES分子中的氨基产生了化学键合。表面硅烷化的Kapton薄膜与Ti箔之间形成了稳定的界面粘附，抗拉强度高达46.2 MPa。     

TiO2掺杂对Na2CO3/Al2O3吸收剂CO2捕捉性能的影响

钠基固体吸收剂脱除燃煤烟气CO₂技术具有反应温度低、能耗低等优点,日益受到学术界的关注。该技术的主要不足是吸收剂的活性成分碳酸钠与CO₂的反应（碳酸化反应）活性较低。针对这一问题,本文旨在研制一种新型改性钠基固体吸收剂,采用活性氧化铝作为载体、TiO₂作为掺杂剂进行改性,利用热重分析装置、XRD、SEM和氮吸附仪研究钠基固体吸收剂的CO₂捕捉性能。结果表明：掺杂TiO₂后,钠基固体吸收剂与CO₂的反应速率加快,CO₂捕捉量增加;反应前后除TiO₂外无其他含Ti化合物生成;碳酸化反应产物为NaHCO₃和Na₅H₃（CO₃）₄;然而TiO₂掺杂过多会堵塞吸收剂的微观孔道,不利于甚至阻碍碳酸化反应的进行,因此,TiO₂的掺杂量应控制在一定的范围内。     

胺基CO2固体吸附剂脱碳特性及SO2的影响

燃煤电厂烟气中存在的微量SO₂对胺基CO₂固体吸附剂的碳酸化反应及循环特性有不利影响。利用固定床反应器,针对采用溶胶凝胶法制备的胺基CO₂固体吸附剂的碳酸化特性及其在含SO₂气氛下的失效规律进行了实验研究,并结合红外光谱、有机元素分析、BET等测试手段,研究其失效机理。结果表明,所制备的胺基CO₂固体吸附剂在反应温度50℃时具有较好的碳酸化反应特性和循环特性。当反应气氛中存在SO₂时,由于生成了不可再生的亚硫酸/硫酸盐类物质而导致胺基活性位损失,孔隙结构发生变化,影响了吸附剂的脱碳性能,但适当提高反应温度可提高吸附剂的碳酸化反应竞争性。     

钙基碳载体造粒的捕集CO特性及力学性能

采用挤出滚圆法对钙基碳载体Ca（OH）₂进行造粒。在双固定床反应器上研究了黏结剂、支撑体和造孔剂对造粒后钙基碳载体循环捕集CO₂性能的影响,并提出采用多孔Al₂O₃球粉作为新型支撑体。结果表明,选择聚乙烯吡咯烷酮为颗粒黏结剂时最佳添加量为2%。高铝水泥和多孔Al₂O₃球粉均可作为支撑体造粒。多孔Al₂O₃球粉作为支撑体造粒后碳载体的循环捕集CO₂性能更高,其10次循环后CO₂吸收量为0.23g/g,是添加高铝水泥造粒碳载体的1.35倍。微晶纤维素作为造孔剂显著提高了造粒碳载体的循环捕集CO₂性能。多孔Al₂O₃球粉作为支撑体造粒后碳载体的抗压强度略高于高铝水泥作为支撑体。多孔Al₂O₃球粉造粒钙基碳载体拥有大量30~100nm孔隙,其比孔容高于高铝水泥造粒碳载体,这有利于CO₂捕集。     

镁负载CaO基吸附剂捕集CO2性能及抗烧结机理

复合钙基吸附剂制备成本过高是限制其工业化应用的主要瓶颈问题。本文以不可溶的CaCO₃和Ca(OH)₂作为钙源,通过燃烧合成法制备钙镁复合吸附剂,在双固定床反应器上研究了其循环捕集CO₂性能。结果显示：制备得到的钙镁复合吸附剂具有更发达的孔隙结构,吸附剂表面Ca和Mg分散均匀,MgO均匀分布于CaO晶粒之间,有效提高了钙镁复合吸附剂的抗烧结特性,因此钙镁复合吸附剂循环反应过程中具有高捕集CO₂活性。以Ca(OH)₂作为钙源时,燃烧合成过程中Ca和Mg均匀同时析出,分散更加均匀,有效避免了CaCO₃作为钙源时Mg的团聚问题,因此得到的钙镁复合吸附剂循环捕集CO₂性能最优。最佳的Ca/Mg摩尔比为(8∶2)~(7.5∶2.5)。本研究以不可溶钙源制备得到高活性钙镁复合吸附剂,有效控制了吸附剂成本,具有更好的工程应用前景。     

Parametric study and effect of calcination and carbonation conditions on the CO2 capture performance of lithium orthosilicate sorbent

The world is currently facing the challenges of global warming and climate change. Numerous efforts have been taken to mitigate CO_2 emission, among which is the use of solid sorbents for CO_2 capture. In this work, Li_4SiO_4 was synthesised via a sol–gel method using lithium nitrate(LiNO_3) and tetraethylorthosilicate(Si C8 H20 O4) as precursors. A parametric study of Li:Si molar ratio(1-5), calcination temperature(600–800 °C) and calcination time(1–8 h) were conducted during sorbent synthesis. Calcination temperature(700–800 °C) and carbonation temperature(500–700 °C) during CO_2 sorption activity were also varied to confirm the optimum operating temperature. Sorbent with the highest CO_2 sorption capacity was finally introduced to several cyclic tests to study the durability of the sorbent through 10 cycles of CO_2 sorption–desorption test. The results showed that the calcination temperature of 800 °C and carbonation temperature of 700 °C were the best operating temperatures, with CO_2 sorption capacity of 7.95 mmol CO_2?(g sorbent)-1(93% of the theoretical yield). Throughout the ten cyclic processes, CO_2 sorption capacity of the sorbent had dropped approximately 16.2% from the first to the tenth cycle, which was a reasonable decline. Thus, it was concluded that Li_4SiO_4 is a potential CO_2 solid sorbent for high temperature CO_2 capture activity.     

Efficient MgO-doped CaO sorbent pellets for high temperature CO2 capture

Novel MgO-doped CaO sorbent pellets were prepared by gel-casting and wet impregnation. The effect of Na⁺ and MgO on the structure and CO₂ adsorption performance of CaO sorbent pellets was elucidated. MgO-doped CaO sorbent pellets with the diameter range of 0.5-1.5 mm exhibited an excellent capacity for CO₂ adsorption and adsorption rate due to the homogeneous dispersion of MgO in the sorbent pellets and its effects on the physical structure of sorbents. The results show that MgO can effectively inhibit the sintering of CaO and retain the adsorption capacity of sorbents during multiple adsorption-desorption cycles. The presence of mesopores and macropores resulted in appreciable change of volume from CaO (16.7 cm³∙mol⁻¹) to CaCO₃ (36.9 cm³∙mol⁻¹) over repeated operation cycles. Ca2Mg1 sorbent pellets exhibited favorable CO₂ capture capacity (9.49 mmol∙g⁻¹), average adsorption rate (0.32 mmol∙g⁻¹∙min⁻¹) and conversion rate of CaO (74.83%) after 30 cycles.     

高温下改性钙基吸附剂固定床反应器从烟气中捕捉二氧化碳(英文)

Four kinds of Ca-based sorbents were prepared by calcination and hydration reactions using different precursors: calcium hydroxide, calcium carbonate, calcium acetate monohydrate and calcium oxide. The CO2 absorption capacity of those sorbents was investigated in a fixed-bed reactor in the temperature range of 350-650℃. It was found that all of those sorbents showed higher capacity for CO2 absorption when the operating temperature higher than 450℃. The CaAc2-CaO sorbent showed the highest CO2 absorption capacity of 299mg·g-1. The morphology of those sorbents was examined by scanning electron microscope (SEM), and the changes of composition before and after carbonation were also determined by X-ray diffraction (XRD). Results indicated that those sorbents have the similar chemical compositions and crystalline phases before carbonation reaction [mainly Ca(OH)2], and CaCO3 is the main component after carbonation reaction. The SEM morphology shows clearly that the sorbent pores were filled with reaction products after carbonation reaction, and became much denser than before. The N2 adsorption-desorption isotherms indicated that the CaAc2-CaO and CaCO3-CaO sorbents have higher specific surface area, larger pore volume and appropriate pore size distribution than that of CaO-CaO and Ca(OH)2-CaO.     

Na2CO3基吸附剂颗粒制备及其脱碳性能

采用挤压-滚圆法制备Na₂CO₃基CO₂吸附剂微球颗粒,在自行设计的CO₂吸收系统中对制备的样品进行脱碳性能测试。结合相关表征测试,探明不同载体、不同负载量的Na₂CO₃基吸附剂的微观结构、脱碳性能以及机械性能的变化规律和内在原因。研究表明：不同载体的Na₂CO₃基吸附剂颗粒脱碳性能存在明显差异,其中氧化铝负载的吸附剂（Na₂CO₃/Al₂O₃）的脱碳性能最好,可达1.14mmol/g。铝酸钙水泥负载的吸附剂（Na₂CO₃/CA）机械性能较好,但其脱碳性能最差。结合吸附剂脱碳和机械性能的综合考量,Na₂CO₃/Al₂O₃是最为合适的CO₂吸附剂,并进一步研究不同Na₂CO₃负载量的影响。研究发现随着Na₂CO₃负载量的变化,吸附剂的微观结构、脱碳性能以及机械性能都存在明显的差异。虽然60%负载量的Na₂CO₃/Al₂O₃吸附剂颗粒的机械性能和脱碳效果较好,但其成球度较差,影响其实际应用。质量分数40%负载量的Na₂CO₃/Al₂O₃吸附剂颗粒具有良好的脱碳性能、机械性能以及成球度,CO₂脱除量为1.36mmol/g。总体而言,利用挤压-滚圆法制备的Na₂CO₃基吸附剂颗粒具有良好的流动特性、脱碳性能和机械性能,适用于电厂烟气中的CO₂脱除。     

Theoretical and experimental study on the fluidity performance of hard-to-fluidize carbon nanotubes-based CO2 capture sorbents

Carbon nanotubes-based materials have been identified as promising sorbents for efficient CO₂ capture in fluidized beds, suffering from insufficient contact with CO₂ for the high-level CO₂ capture capacity. This study focuses on promoting the fluidizability of hard-to-fluidize pure and synthesized silica-coated amine-functionalized carbon nanotubes. The novel synthesized sorbent presents a superior sorption capacity of about 25 times higher than pure carbon nanotubes during 5 consecutive adsorption/regeneration cycles. The low-cost fluidizable-SiO₂ nanoparticles are used as assistant material to improve the fluidity of carbon nanotubes-based sorbents. Results reveal that a minimum amount of 7.5 and 5 wt% SiO₂ nanoparticles are required to achieve an agglomerate particulate fluidization behavior for pure and synthesized carbon nanotubes, respectively. Pure carbon nanotubes + 7.5 wt% SiO₂ and synthesized carbon nanotubes + 5 wt% SiO₂ indicates an agglomerate particulate fluidization characteristic, including the high-level bed expansion ratio, low minimum fluidization velocity (1.5 and 1.6 cm·s^–1), high Richardson−Zakin index (5.2 and 5.3 > 5), and low Π value (83.2 and 84.8 < 100, respectively). Chemical modification of carbon nanotubes causes not only enhanced CO ₂ uptake capacity but also decreases the required amount of silica additive to reach a homogeneous fluidization behavior for synthesized carbon nanotubes sorbent.     

Enhancement of CO2 capture and microstructure evolution of the spent calcium-based sorbent by the self-reactivation process

The effect of self-reactivation on the CO_2 capture capacity of the spent calcium based sorbent was investigated in a dual-fixed bed reactor.The sampled sorbents from the dual-fixed bed reactor were sent for XRD,SEM and N_2 adsorption analysis to explain the self-reactivation mechanism.The results show that the CaO in the spent sorbent discharged from the calciner absorbs the vapor in the air to form Ca(OH)_2 and further Ca(OH)_2·2 H_2 O under environmental conditions,during which process the CO_2 capture capacity of the spent sorbent can be self-reactivated.The microstructure of the spent sorbent is improved by the self-reactivation process,resulting in more porous microstructure,higher BET surface area and pore volume.Compared with the calcined spent sorbent that has experienced 20 cycles,the pore volume and BET surface area are increased by 6.69 times and 56.3% after self-reactivation when φ=170%.The improved microstructure makes it easier for the CO_2 diffusion and carbonation reaction in the sorbent.Therefore,the CO_2 capture capacity of the spent sorbent is enhanced by self-reactivation process.A self-reactivation process coupled with calcium looping process was proposed to reuse the discharged spent calcium based sorbent from the calciner.Higher average carbonation conversion and CO_2 capture efficiency can be achieved when self-reactivated spent sorbent is used as supplementary sorbent in the calciner rather than fresh CaCO_3 under the same conditions.