负载型钾基CO2吸收剂的结构表征和碳酸化反应特性

The structure identification and carbonation characteristics of several potassium-based supported sorbents for CO₂ capture were investigated with TGA,XRD,XRF,SEM and N₂ adsorption method.Potassium-based sorbents were prepared by impregnation with potassium carbonate on supports,such as cocoanut activated charcoal（AC1）,coal active carbon（AC2）,silica gel（SG）and diatomite（DT）using the iso-volume impregnation method.The results showed that the K₂CO₃ loading amounts of AC1,AC2,SG and DT were 24.1%,22.5%,21.7% and 19.1% respectively.The surface area and pore volume of K₂CO₃/AC1 and K₂CO₃/AC2 were larger than others.In contrast,those of K₂CO₃/DT were small.For K₂CO₃/SG,pore volume was large but surface area was small.K₂CO₃/AC1 and K₂CO₃/AC2 showed excellent carbonation capacity.However,the carbonation capacities of K₂CO₃/SG and K₂CO₃/DT were low.The difference in carbonation capacity of those sorbents were attributed to the difference in pore structure,leading to different supported sorbents.     

CO2跨临界双级压缩制冷循环的热力学分析

Two-stage vapor compression refrigeration cycle was accomplished with an intercooler.The state of the refrigerant vapor leaving the intercooler affects the system performance.The thermodynamic analysis of the trans-critical two-stage refrigeration cycle using CO₂ as the refrigerant was made with a condensing temperature of 35℃.When the intercooler operated at about the geometric mean of the evaporating and condensing pressures,compared with the single stage cycle,the coefficient of performance（COP）of the two-stage cycle was improved.As the degree of superheating of the CO₂ vapor leaving the intercooler increased,the COP of the two-stage system decreased.     

288 K下Li+,K+//CO2-3,B4O2-7-H2O四元体系的相平衡

Solubilities and properties (density, conductivity and pH value) of solutions in the quaternary system Li⁺,K⁺//CO^2-₃,B₄O^2-₇-H₂O at 288 K were experimentally studied with the isothermal equilibrium method. The phase diagram of the system consisted of two invariant points E and F, five univariant curves, and four crystallization fields that belonged to K₂CO₃·3/2H₂O,Li₂B₄O₇·3H₂O,K₂B₄O₇·4H₂O and Li₂CO₃. The composition of the solution corresponding to E was w（CO^2-₃）=2.27 %,w（B₄O^2-₇）=6.05 %,w（K⁺ ）=4.30%,w(Li⁺)=0.30 % and the equilibrium solids were Li₂B₄O₇· 3H₂O+K ₂B₄O₇·4H₂O+Li₂CO₃;The composition of the solution for F was w(CO^2-₃)=22.45%,w(B₄O^2-₇)=1.88%,w(K⁺ )=29.96%,w(Li⁺ )=0.03% and the equilibrium solids were K₂CO₃·3/2H₂O+K ₂B₄O₇·4H₂O+Li₂CO₃. K₂CO₃ possesses strong salting-out effect on K₂B₄O₇,Li₂CO₃ and Li₂B₄O₇.     

辉光放电等离子体增强制备甲烷催化燃烧的高分散Pd/Al2O3催化剂

A novel Pd/Al₂O₃ catalyst prepared by glow discharge plasma technology is reported.The results of H₂-chemisorption indicate that palladium dispersion of the plasma-prepared Pd/Al₂O₃ reaches 29.7%,which is about 5 times higher than Pd/Al₂O₃ prepared by conventional preparation.Meanwhile,the particle diameter of the plasma-prepared catalyst is 3.8 nm, but the particle diameter of the conventional catalyst is 20.4 nm.Such plasma-prepared Pd/Al₂O₃ catalyst shows a higher activity for catalytic combustion of methane than the conventional catalyst.Methane conversion reaches 90% at 400 ℃, but it is only near 30% for the conventional catalyst at the same temperature.     

碳酸化法制备α-Al(OH)3包覆CaCO3复合晶须

A carbonation process was developed to coat Al(OH)₃ on aragonite whisker. Al(OH)₃ coating was obtained in a suspension,which contained 3Cao·Al₂O₃·6H₂O(C₃AH₆)-NaOH prepared by adding Ca(OH)₂ to NaAlO₂ aqueous solution.The CaCO₃ whiskers coated with fine particles of Al(OH)₃ were prepared by blowing CO₂ gas into the suspension.The formed Al(OH)₃ adhered to the CaCO₃ fibers as the substrate.In order to coat α -Al(OH)₃ on aragonite whisker , the pH value of the solution must be higher than 10.5.The formation of C₃AH₆ and complexation of calcium carbonate molecule with C₃A were the domain factors to get single aragonite phase whisker. Micro-analysis demonstrated that the existence of Al(OH)₃ crystal coating on the surface of aragonite-type calcium carbonate whisker.After the coated whiskers were treated strongly in an ultrasonic water bath.Al(OH)₃ still adhered to the CaCO₃ whiskers well.The reaction mechanism was also mentioned in this paper.     

硅酸钠溶液分步碳分制备高纯沉淀氧化硅

By using industrial sodium silicate solution as raw material,high purity SiO₂ powder was successfully synthesized by the split-step carbonation method.The relations between pH value of end point and the removal percentage of impurity at the first carbonation and the purity and yield of product SiO₂ powder at the second carbonation were studied.The SiO₂ powder was characterized by using XRD,SEM,IR and composition analysis.The results showed that when the pH value of end point at the first carbonation was 10.9,the purity of SiO₂ prepared was up to 99.9%.The SiO₂ powder synthesized was amorphous with regular sphere shape,uniform size and no reunion.The reaction mechanism was also discussed.     

煅烧升温速率对于钙基吸收剂脱碳性能的影响

A wire-mesh reactor capable of heating samples at a given heating-rate (1—1000 K•s^-1) was used to investigate the effect of heating-rate on Ca-based absorbent performance of CO₂ capture.BET method was used to analyze the morphology of the produced CaO, and the capabilities of the absorbent were compared.It was found that CaO calcined at a higher heating-rate had more appropriate pore distribution for CO₂ capture, and the capability of CaO calcined at 1000 K•s^-1 was 15% higher than that calcined at 1 K•s^-1 determined by TGA.     

PVAm/PAN复合膜的制备及其对CO2/CH4的分离性能

New polymeric membrane materials——polyvinyl amine (PVAm) with different primary amine contents were synthesized.By covering polyacrylonitrile(PAN) ultrafiltration membranes with PVAm, the PVAm/PAN composite membranes for CO₂/CH₄ separation were prepared. The composite membranes containing more primary amino groups have higher selectivity for CO₂/CH₄.The cross-linking of acid or glutaradehyde could improve the gas permselectivity of the composite membranes. With decreasing CO₂ content in the feed gas, the CO₂/CH₄ separation factor increased.When the feed gas was 25%(vol) CO₂ and 75%(vol) CH₄, the CO₂ permeation rate was 4.1×10^-9cm³(STP) •cm^-2•Pa^-1•s^-1, and the CO₂/CH₄ separation factor was 180.     

Al2O3-CoCrAlY 复合陶瓷激光熔覆层的组织与性能

The wear resistance, structure and composition distribution of Al₂O₃/CoCrAlY composite ceramic coatings on W18Cr4V steel were studied. The results show that structure of plasma sprayed coatings is laminars in shape, and the Al₂O₃ top coating consists of α-Al₂O₃ and a small amount of γ-Al₂O₃. There is a mechanically combined interface between Al₂O₃ and CoCrAlY coatings, and also between CoCrAlY and substrate. The average hardness of plasma sprayed Al₂O₃ coatings is about 897 HV_0.2. The structure of coatings cladded by laser is columnar, which consists of α-Al₂O₃. There is an interface phase of metallurgical combination and a little composition gradient was observed between CoCrAlY and substrate. The bonding of interface between Al₂O₃ and CoCrAlY has been improved obviously. The hardness of Al₂O₃ coatings cladded by laser is about 2 479～2 691 HV_0.2 and the wear resistance is 2～3 times that of plasma sprayed coatings. The wear mechanism is fatigue wear and abrasive wear.     

Al2O3掺杂对微晶(Y,Mg)-PSZ材料性能的影响

The effect of Al₂O₃ addition was investigated on sinterability,grain size and mechanical properties of fine-grained(Y,Mg)-PSZ ceramics.It is found that small amount of Al₂O₃ addition has considerable effects on material properties mentioned above.Al₂O₃ addition could inhibit grain growth of ZrO₂,as well as improve mechanical properties at room temperature.On the other hand,excessive amount of Al₂O₃ could hinder not only grain growth of ZrO₂ but also densifications.However,mechanical properties at high temperature (800℃) could be improved.     

钾基CO2吸收剂的碳酸化反应特性

对钾基CO₂吸收剂的碳酸化反应机理进行研究。利用热重分析、XRD、扫描电镜和氮吸附仪进行试验。结果表明：分析纯碳酸钾的组分为K₂CO₃·1.5H₂O,碳酸化反应速率缓慢;先将分析纯碳酸钾样品脱除结晶水后再进行碳酸化反应时,K₂CO₃与气氛中的水蒸气迅速生成K₂CO₃·1.5H₂O,不利于碳酸化反应的进行;由KHCO₃分解产生的K₂CO₃却表现出优越的碳酸化反应性能,20 min内转化率高达85%以上,经过多次循环试验后吸收剂仍保持很高的活性。从微观角度分析了两种改性钾基CO₂吸收剂碳酸化反应机理差异的原因,通过拟合计算得到了这3种钾基吸收剂的碳酸化反应速率常数,为干法K₂CO₃/KHCO₃循环脱除CO₂的研究提供了一定的基础数据。     

O2/CO2气氛下煤燃烧SO2/NO析出特性

在水平管式炉上研究了O₂浓度、CO₂浓度、温度及石灰石添加等各参数对O₂/CO₂气氛下徐州烟煤和龙岩无烟煤燃烧过程中SO₂/NO排放特性的影响。结果发现,O₂/CO₂气氛下,烟煤和无烟煤燃烧SO₂/NO的析出规律与空气气氛下不同,同等O₂浓度下析出量比空气气氛下小。O₂/CO₂气氛下,随着O₂浓度的提高,烟煤和无烟煤SO₂/NO排放量均增大;随着CO₂浓度的升高, SO₂/NO排放量均减小。O₂/CO₂气氛下,石灰石添加对SO₂排放的抑制作用低于空气气氛下;石灰石添加对NO的排放有一定减排作用。对煤灰的元素分析显示O₂/CO₂燃烧对SO₂的抑制主要是由于煤灰的自固硫能力增强,而对NO的减排作用则是促进燃料N向其他含N气体的转换。     

纳米钙基CO2吸附剂反应吸附与分解动力学

采用TGA测定纳米钙基CO₂吸附剂在500～650℃温度范围内,CO₂分压0.015～0.025 MPa氮气气氛中的吸附反应动力学。针对纳米钙基CO₂吸附剂吸附CO₂反应特征,提出以两倍最大吸附速率对应的时间点前后分别为快速反应段与慢速反应段。分别采用Boltzmann方程与Avrami-Erofeev方程拟合快速反应段与慢速反应段吸附反应动力学方程,得到纳米钙基CO₂吸附剂在快速反应段与慢速反应段的活化能分别为27.52、70.25 kJ·mol^-1。吸附率拟合与实验值平均相对误差分别为10.29％、4. 17%。研究测试了纳米钙基CO₂吸附剂在650～800℃温度范围内,N₂,0.02、0.04 MPa CO₂分压氮气气氛中的分解反应动力学。忽略反应过程中传热、传质影响,采用收缩核模型,分别求得吸附剂在N₂,0.02、0.04 MPa CO₂分压氮气气氛中的活化能为141.9、34.7、113.2 kJ·mol^-1。碳酸钙分解率与实验值比较平均相对误差分别小于5.66% 、7.82%、5.01%。     

Al2O3纳米颗粒对氨水鼓泡吸收过程的强化影响

在试制出了性能稳定的Al₂O₃纳米流体的基础上,通过定氨气流量和定入口压力两种实验方案,验证了Al₂O₃纳米颗粒对氨水吸收过程的强化影响,同时找出了引起强化吸收的两个主要影响因素：纳米流体性能的稳定性和吸收器入口与吸收器内气相界面的压力差。在添加十二烷基苯磺酸钠（SDBS）的情况下,可以获得性能稳定而具有强化吸收效果的Al₂O₃纳米流体,尽管SDBS本身对Al₂O₃纳米流体强化吸收具有抑制作用。较大的压力差下Al₂O₃纳米流体在吸收开始阶段就表现出强化吸收效果。随着氨水浓度的增加,氨水对氨气的吸收潜力减小,而Al₂O₃纳米流体对氨水溶液强化吸收的效果更加明显。对强化现象的可能机理给出了合理解释,为纳米流体对传热传质强化研究提供参考。     

O2/CO2气氛煤焦的燃烧及其孔隙结构变化

采用热力工况与实际煤粉炉相近的沉降炉实验装置,制备了不同环境气氛下（O₂/N₂及O₂/CO₂气氛）、不同燃尽率的煤焦试样,并采用低温氮吸附仪和扫描电子显微镜测定了其孔隙结构和表面形貌。结果表明,在相同的操作条件下,相同O₂浓度的O₂/CO₂气氛下煤焦的燃烧速率较慢、燃尽率较低,各试样的孔比表面积和比孔容积均较小。两种气氛下燃尽过程孔结构参数（SBET和VBJH）均呈减小趋势,且在孔径变化较明显的区域内（<5 nm）在CO₂气氛下煤焦的孔径分布较小且与煤种相关。SEM图像显示CO₂气氛下的煤焦表面致密,孔隙较少,其定性结果与N₂吸附法的定量测量结果吻合较好。     

CO2载体CaO循环煅烧/碳酸化反应的分形特征

捕捉煤燃烧释放出的CO₂时,作为CO₂载体的CaO微观结构特性对其循环碳酸化性能具有显著影响。采用分形维数作为表征CaO微观结构的特征参数,研究在循环煅烧/碳酸化反应过程中CaO的分形特征及其对CO₂捕捉性能的影响规律。结果表明,随着循环次数的增加CaO分形维数逐渐下降,CaO孔道也由粗糙和不规则变得越来越平滑和有规则性。煅烧温度升高则CaO分形维数下降。分形维数较大的CaO具有较高的碳酸化速率。在碳酸化过程的前10 min内CaO的分形维数迅速减小,此后随时间变化缓慢。在分形维数D≤2.61的实验范围内,CaO分形维数与其循环碳酸化转化率呈线性正相关;当D＞2.61时,可能存在临界分形维数D_cr,当D＞D_cr时随着分形维数的进一步增大CaO转化率反而减小。     

US/H2O2系统协同降解苯酚的动力学研究

超声波/过氧化氢（US/H₂O₂）复合氧化过程在废水处理领域有很广泛的应用前景，但在动力学方面的研究很少，为此研究了US/H₂O₂工艺降解苯酚的动力学.结果表明，苯酚在单独超声波辐射（US）、过氧化氢（H₂O₂）氧化和超声波/过氧化氢（US/H₂O₂）协同下的降解均符合表观一级动力学.在单独的超声波辐射或者过氧化氢氧化下苯酚去除率很小，而在复合氧化过程US/H₂O₂工艺中有显著的提高，表明协同效应存在.苯酚去除的速率常数增强因子可达到6.904.进一步从US/H₂O₂系统中存在US、H₂O₂和羟基自由基（&#8226;OH）3部分协同作用的降解机理，推导出了简化的机理动力学模型，很好地反应过氧化氢浓度过量条件下苯酚的降解.