等离子体辅助快速合成磁性Fe3O4/NaA复合材料及其CO2吸附性能

吸附法是捕集分离CO₂等温室气体的重要方法,磁性复合材料能实现气固相快速分离而备受关注。本文利用介质阻挡放电等离子体处理方法,分别对磁性Fe₃O₄和分子筛前体进行处理,再通过水热法快速制备了Fe₃O₄/NaA复合材料。利用X射线衍射、红外光谱、扫描电镜和元素扫描等技术进行了表征,并考察了复合材料中Fe₃O₄/NaA含量比对CO₂吸附性能和磁性能的影响。结果显示,当Fe₃O₄的质量分数为23.2％时,Fe₃O₄/NaA复合材料既具有优异CO₂吸附能力（2.10mmol/g）,又具有较好的磁性（25.92emu/g）,同时CO₂吸附-脱附循环稳定性高,是一种新型磁性CO₂吸附剂。在采用流化床吸附捕集CO₂技术中,有望实现气固高效磁分离。     

负载型K2CO3/Al2O3二氧化碳吸收剂的碳酸化反应特性

引言 全球变暖已经成为一个备受关注的环境问题.据预测,如不采取积极的温室气体减排措施,从现在起到2100年,全球近地面平均气温将继续升高1.4～5.8℃[1].CO2是主要的温室气体,而我国燃煤电厂是CO2排放量最大、最集中的化石燃料燃烧场所.因此研究和开发适用于燃煤电厂的CO2减排技术至关重要.     

基于Langmuir-Hinshelwood动力学解析O2/CO2/H2O气氛下烟煤焦反应机理

流化床富氧燃烧湿烟气循环兼具经济与环保优势。湿烟气循环（O₂/CO₂/H₂O）条件下煤焦与O₂、CO₂及H₂O的反应同时发生。为探究O₂/CO₂/H₂O气氛下煤焦-O₂、煤焦-CO₂、煤焦-H₂O反应间的相互作用机制,在自制高精度热重实验装置上系统考察了O₂、CO₂、H₂O及其混合气氛下,典型烟煤焦在900℃的反应特性。基于吸附和脱附原理的Langmuir-Hinshelwood（L-H）机理性模型分别计算了烟煤焦与O₂、CO₂和H₂O反应的动力学参数。通过采用单独活性位点与竞争活性位点两种假设分析了O₂/CO₂、O₂/H₂O和CO₂/H₂O气氛下烟煤焦-O₂、烟煤焦-CO₂和烟煤焦-H₂O两两反应间的作用机制,揭示了H₂O分子优先吸附于烟煤焦表面活性位点,O₂分子次之,而CO₂分子相对滞后。O₂/CO₂/H₂O气氛下烟煤焦-O₂、烟煤焦-CO₂、烟煤焦-H₂O反应表现出部分竞争反应活性位点,传统的单独活性位点与竞争活性位点假设均无法准确描述其反应速率特性。基于H₂O分子优先,O₂分子次优先吸附的原理,建立了O₂、CO₂、H₂O混合气氛下煤焦反应速率L-H动力学方程,方程计算结果与实验值良好吻合。研究结果为深入分析煤焦颗粒流化床富氧燃烧特性及构建可靠、准确的燃烧反应模型提供了理论支撑。     

Na2CO3/γ-Al2O3吸附剂对SO2吸附性能的研究

用浸渍法制备了 Na2 CO3 /γ- Al2 O3 吸附剂 ,考察了 Na2 CO3 含量、焙烧温度和吸附温度对 Na2 CO3 /γ- Al2 O3 吸附剂 SO2 吸附性能的影响 .结果表明 :Na2 CO3 含量从 4%增加到 2 0 %时 ,穿透时间和硫容在 1 6%时出现峰值 .未经焙烧的吸附剂穿透时间和硫容都比较低 ,较理想的焙烧温度为 30 0℃～ 40 0℃ .吸附温度对 SO2 吸附性能的影响明显 ,在室温下吸附时 ,穿透时间和硫容都较小 ,适宜的吸附温度为 1 2 0℃～ 1 60℃ .     

负载型K2CO3/Al2O3吸收剂吸收CO2反应机理

利用热重分析仪、扫描电镜和氮吸附仪对不同粒径的K₂CO₃颗粒和负载型K₂CO₃/Al₂O₃二氧化碳吸收剂的碳酸化特性进行研究。负载后的吸收剂比表面积和孔隙结构得到较大改善,使得碳酸化反应速率和转化率均提高,吸收剂碳酸化特性得到改善。纯K₂CO₃颗粒吸收剂的反应速率和转化率随着粒径的增加而减小,负载型吸收剂的反应速率和转化率随着粒径的增加略增大。研究了不同粒径和反应时间对K₂CO₃/Al₂O₃颗粒微观结构的影响,结果表明K₂CO₃/Al₂O₃颗粒具有较稳定的微观结构。采用负载型粒子模型对K₂CO₃/Al₂O₃吸收剂吸收CO₂碳酸化过程进行研究,所建立的粒子模型计算结果与试验值吻合较好。利用建立的模型对不同CO₂浓度下K₂CO₃/Al₂O₃吸收剂碳酸化反应特性进行模拟计算,模拟结果具备一定的合理性和准确性,为开展进一步研究提供了基础。     

O2/H2O燃烧方式下石灰石的间接硫化反应特性

利用水平管式炉和热重实验台架,对O₂/H₂O、O₂/N₂和O₂/CO₂ 3种不同燃烧方式下石灰石的间接硫化反应特性进行了研究。重点探究了燃烧方式、水蒸气浓度对石灰石间接硫化反应的影响规律与机理。同时,对硫化产物进行了X射线荧光光谱（XRF）、X射线衍射（XRD）、孔结构特性和扫描电镜（SEM）分析。结果表明,O₂/H₂O燃烧方式相比于相同氧浓度下的O₂/N₂和O₂/CO₂燃烧方式,石灰石间接硫化反应的钙转化率在化学反应控制阶段基本相同,在扩散控制阶段O₂/H₂O燃烧方式下的钙转化率有显著的提高。主要原因是水蒸气促进了硫化反应后期产物层内的固态离子扩散。此外,O₂/H₂O燃烧方式下,不同的水蒸气浓度对石灰石的钙转化率基本没有影响。     

金属有机框架材料吸附CO2研究进展

为有效应对全球气候变暖,减缓温室气体排放,实现中国提出的“双碳”目标,寻找有效的CO2吸附技术具有重大的现实意义。金属有机框架（MOFs）作为一种具有高度可调性和优异孔隙结构的新型吸附材料,在CO2捕集和分离方面展现出卓越的性能,具有巨大的应用潜能,其独特、稳定的三维空间结构和高度不饱和的活性吸附位点,特别适用于低温环境中吸附CO2。该文综述了近10年来MOFs在CO2吸附领域应用的研究进展,首先阐述了MOFs吸附材料的常见类型和合成方法,然后详细探讨了影响MOFs材料吸附性能的因素以及改性手段,最后提出了优化水热合成法、构建核-壳结构复合MOFs、引入非极性基团有机配体来提高水稳定性能、与多孔固体材料复合进行改性等MOFs在CO2吸附领域的研究方向。     

CO2/H2O环境下X80钢母材/焊缝腐蚀行为演变过程研究

与管线母材相比,焊缝是管线失效的关键部位之一.针对含CO2/H2O的天然气管线母材和焊缝在稳态和动态条件下的电化学腐蚀行为,通过三电极体系和高温高压反应釜相结合开展20 d的浸泡实验,得到不同条件下母材和焊缝的电化学阻抗特征,通过等效电路拟合相关参数的变化规律建立不同阶段母材和焊缝的腐蚀过程,并通过腐蚀形貌分析和腐蚀产...     

钛盐光度法测定O3/H2O2高级氧化系统中的过氧化氢

采用钛盐光度法测定O3/H2O2系统中的/H2O2,考察了pH值、O3/H2O2摩尔比、钛盐用量和显色时间的影响,确定了最佳的测定条件;通过加标回收率实验和对比实验,证明了该方法的可靠性.结果表明,pH值为3.0、λ=385nm、草酸钛钾浓度2.5mmol·L-1和显色时间8min条件下,H2O2浓度0～45mg·L-...     

13X沸石与CuCl/分子筛在甲醇制氢脱碳中的吸附特性研究

甲醇重整制氢是一种重要的氢气生产技术,但其过程中CO和CO₂等杂质对氢气纯度构成了挑战。实验研究了13X沸石分子筛和CuCl/分子筛在甲醇重整制氢过程中对CO和CO₂的静态吸附特性,并通过动态吸附实验探讨了不同气体流量、温度、吸附剂用量等条件对吸附效率的影响。结果表明,13X沸石和CuCl/分子筛分别对CO₂和CO吸附中表现出较高的容量。温度、压力、气体流量和分子筛填料比例对吸附效果具有显著影响。实验提供了吸附剂用量与气体处理量之间的关系,为甲醇重整脱碳技术的优化与工业化应用提供了理论支持。     

CO2 capture from dry flue gas by vacuum swing adsorption: A pilot plant study

The capture and concentration of CO₂ from a dry flue gas by vacuum swing adsorption (VSA) has been experimentally demonstrated in a pilot plant. The pilot plant has the provision for using two coupled columns that are each packed with approximately 41 kg of Zeochem zeolite 13X. Breakthrough experiments were first carried out by perturbing a N₂ saturated bed with 15% CO₂ and 85% N₂ feed, which is representative of a dry flue gas from coal‐fired power plants. The breakthrough results showed long plateaus in temperature profiles confirming a near adiabatic behavior. In the process study, a basic four‐step vacuum swing adsorption (VSA) cycle comprising the following steps: pressurization with feed, adsorption, forward blowdown, and reverse evacuation was investigated first. In the absence of any coupling among the steps, a single bed was used. With this cycle configuration, CO₂ was concentrated to 95.9 ± 1% with a recovery of 86.4 ± 5.6%. To improve the process performance, a four‐step cycle with light product pressurization (LPP) using two beds was investigated. This cycle was able to achieve 94.8 ± 1% purity and 89.7 ± 5.6% recovery. The Department of Energy requirements are 95% purity and 90% recovery. The proposed underlying physics of performance improvement of the four‐step cycle with LPP has also been experimentally validated. The pilot plant results were then used for detailed validation of a one‐dimensional, nonisothermal, and nonisobaric model. Both transient profiles of various measured variables and cyclic steady state performance results were compared with the model predictions, and they were in good agreement. The energy consumptions in the pilot plant experiments were 339–583 ± 36.7 kWh tonne^?1 CO₂ captured and they were significantly different from the theoretical power consumptions obtained from isentropic compression calculations. The productivities were 0.87–1.4 ± 0.07 tonne CO₂ m^?3 adsorbent day^?1. The results from our pilot plant were also compared with available results from other pilot plant studies on CO₂ capture from flue gas. © 2014 American Institute of Chemical Engineers AIChE J, 60: 1830–1842, 2014     

Effects of water vapor on gas permeation and separation properties of MFI zeolite membranes at high temperatures

Understanding the effects of water vapor on gas permeation and separation properties of MFI zeolite membranes, especially at high temperatures, is important to the applications of these zeolite membranes for chemical reactions and separation involving water vapor. The effects of water vapor on H₂ and CO₂ permeation and separation properties of ZSM‐5 (Si/Al ～ 80) zeolite and aluminum‐free silicalite membranes were studied by comparing permeation properties of H₂ and CO₂ with the feed of equimolar H₂/CO₂ binary and H₂/CO₂/H₂O ternary mixtures in 300–550°C. For both membranes, the presence of water vapor lowers H₂ and CO₂ permeance to the same extent, resulting in negligible effect on the H₂/CO₂ separation factor. The suppression effect of water vapor on H₂ and CO₂ permeation is larger for the less hydrophobic ZSM‐5 zeolite membrane than for the hydrophobic silicalite membrane, and, for both membranes, is stronger at lower temperatures and higher water vapor partial pressures. © 2011 American Institute of Chemical Engineers AIChE J, 2012     

Zeolite Apgiia for Adsorption Based Carbon Dioxide Capture

Adsorption of synthetic flue gas on a commercial zeolite 13X (APGIIA) with targeted Si/Al ratio has been studied aiming to design an adsorption process for CO₂ capture from post-combustion power plants. Adsorption equilibrium of pure gases (CO₂ and N₂) has been measured in a wide range of temperatures: 303, 333, 363, 393, 423, 473 K. Adsorption equilibrium was fitted with the multisite Langmuir model. The adsorption capacity of the zeolite pellets for CO₂ is 4.54 mol/kg and 0.26 mol/kg for N₂ at 303 K and 100 kPa. The dynamic behavior of the pellets in a fixed bed was also studied by measuring breakthrough curves. Adsorption and desorption was analyzed in order to understand the regeneration of the adsorbent.

Based on equilibrium and kinetic data, two different adsorption technologies were simulated: Vacuum Pressure Swing Adsorption (VPSA) and Temperature Swing Adsorption (TSA). A CO₂ recovery of 63.0% with 72.1% purity was obtained using a five-step PSA cycle included rinse step. In a 5-step TSA process, however, a CO₂ purity of 78.7% and recovery of 76.6% can be achieved under a heating temperature of 423 K.     

水蒸气纯氧条件下合成气燃烧特性

水蒸气纯氧燃烧技术因具有高效零污染物排放的特点而备受关注,对合成气在水蒸气纯氧条件下的燃烧特性进行了实验研究。在扩散燃烧实验台上测量了H₂O/O₂为2.0时,燃烧室中心气体成分和火焰温度随停留时间的变化规律,分析了过量氧气系数对合成气水蒸气纯氧燃烧过程的影响。研究结果表明:过量氧气系数为0时,H₂和CO的燃烧主要在前28 ms内,H₂的燃烧速率较快,能够快速燃尽;CO燃烧较慢,燃烧室出口含量依然很高。过量氧气系数从0增大到10%时,CO的浓度整体降低,燃烧速率提高,燃烧前期火焰温度提高。燃烧室出口CO浓度随过量氧气系数的增加逐渐降低,氧气微过量时CO浓度迅速下降,继续增大时,燃烧室出口CO的浓度下降缓慢。     

La2O3助剂对甲烷干燥重整催化剂 Ni-γ-Al2O3支撑作用的研究简

The nature of support and type of active metal affect catalytic performance. In this work, the effect of using La203 as promoter and support for Ni/γ-A1203 catalysts in dry reforming of methane was investigated. The reforming reactions were carried out at atmosphenc pressure in the temperature range of 500-2700℃. The activity and stability of the catalyst, carbon formation, and syngas （H2/CO） ratio were determined. Various techniques were applied for characterization of both fresh and used catalysts. Addition of La2O3 to the catalyst matrix improved the dispersion of Ni and adsorption of CO2, thus its activity and stability enhanced.     

浅析CO_2汽提法尿素装置合成系统的NH_3/CO_2

介绍CO2汽提法尿素装置合成系统的NH3/CO2的控制方法,合成系统NH3/CO2异常的症状,判断方法,偏离正常时的处理和防范措施。