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1.
在热重分析仪中考察了不同升温速率下油砂的热解特性,结果表明:油砂样品失重过程分为少量气体脱附、低温热解、主要热解、半焦缩聚4个阶段。通过微型固定床与在线质谱耦合测得的气体释放顺序为CO 2、CO、C 2H 6、CH 4和H 2,所对应的初释温度分别为155、178、146、174、354℃。结合核磁和红外对不同温度段液固产物的化学结构进行分析,发现350℃前主要是油砂中轻质油脱附,还包括羧基和烷基侧链的断裂,轻质油品中芳碳率达7.92%;350~520℃之间为油砂的主要热解阶段,油砂油结构中芳碳率为23.51%。据Coats-Redfern法计算得到油砂低温热解和主要热解段的活化能分别为27.63和90.30 kJ·mol -1,说明开环与裂解反应所需活化能大于油砂油脱附、羧基分解和弱键断裂反应的活化能,揭示了分段热解机理。 相似文献
2.
在外热式内构件(多级折流板和多段集气管)移动床反应器内研究了淖毛湖煤的热解特性,并与常规固定床反应器中煤热解行为进行对比,考察了两反应器内的传热速率以及热解温度对产物分布、热解气组成、焦油组成和品质等影响规律。结果表明:在450℃低温热解时,煤颗粒在内构件移动床内的升温时间比固定床缩短了60%以上,内构件具有显著提高反应器内颗粒间传热速率的作用。随着热解温度的升高,热解气中的C 2H 4/C 2H 6和C 3H 6/C 3H 8的比值变大,挥发分的二次反应程度加大,但裂解程度低于固定床。内构件移动床中的焦油产率随温度的升高先增加后降低,在550℃时达到最高为10.8%(质量分数),比固定床增高约28.6%。当热解温度越高时,移动床所产焦油中的沥青质组分含量越低,在750℃时焦油中轻质组分质量分数达到85.17%,脂肪烃含量降低到了28.00%。通过与固定床对比,揭示了内构件(多级折流板和集气管)调控淖毛湖煤热解反应并提高热解焦油产率和品质的作用。 相似文献
3.
The homogeneous gas phase O 2-based oxidation of methane was studied in the temperature range, from 500°C to 750°C at methane partial pressures ranging from 3 bar to 40 bar. At the lower end of the temperature range methanol, formaldehyde, and CO represent the main products, while at temperatures exceeding 650° C/C-coupled products, C 2H 6, C 2H 4, C 3H 6 and C 3H 8 predominate. The change in selectivity as function of the temperature is well explained based on a free radical chain mechanism with degenerate branching, initiated by the gas phase reaction, CH 4+O 2→CH ·3+HO ·2. Bringing in basic catalysts known to catalyze the system at low methane partial pressures, in the reactor e.g. SrCO 3, BaCO 3, and 7% Li/MgO resulted in reduced rates of methane and oxygen conversions, and only minor changes in the selectivity to coupled products were observed. 相似文献
4.
大庆罐底油泥属于高含油污泥,资源回收潜力大,同时具有黏度大、黏结性强、成分复杂、自然沉降慢等特性。本文对大庆油田高含油污泥的热解特性及污染物释放特性进行研究,分别测试了不同热解终温和升温速率下气/液/渣三相产品的品质和成分。结果表明,热解气中C 2H 4的释放量明显高于其余气体。CO 2气体仅在700℃处出现一个峰值,H 2在700℃之前释放量偏低,在700~800℃之间大量释放;热解终温和升温速率的增加会导致热解油低链烃类的大量生成,中链烃类呈现先增加后降低的趋势;热解终温会对固相产物中的SiO 2和CaCO 3产生一定的影响,而升温速率对固相产物几乎无影响。采用在线烟气分析仪测试了气相产物中的N、S、Cl小分子污染物的释放特性。HCN、NH 3在600℃时向NO x转化;600℃以下绝大部分含氯化合物会发生释放;含硫污染物成双峰释放,600℃以上的峰主要源于硫酸盐的分解。 相似文献
5.
鉴于传统微波吸收剂在协同微波热解含油污泥时存在热解效率较低、处理成本较高等问题,本文引入磁性纳米粒子作为新型微波吸收剂,探究了磁性纳米粒子种类和质量浓度在强化微波热解含油污泥中的作用效果和规律。实验结果表明:(1)在6种磁性纳米粒子(Zn Fe 2O 4、Fe 3O 4、Ni、Ni Fe 2O 4、γ-Fe 2O 3和Co 3O 4)中,添加Zn Fe 2O 4的实验组热解终温最高,为284℃,气、液相产物最多,分别为382m L和10.5m L;(2)当微波功率为800W、微波加热时间为20min时,添加纳米Zn Fe 2O 4实验组的热解终温在质量浓度5.0mg/g时最高;(3)随着纳米Zn Fe 2O 4质量浓度的增加,气相热解产物中H 2、CH... 相似文献
6.
The effect of the addition of a second fuel such as CO, C 3H 8 or H 2 on the catalytic combustion of methane was investigated over ceramic monoliths coated with LaMnO 3/La-γAl 2O 3 catalyst. Results of autothermal ignition of different binary fuel mixtures characterised by the same overall heating value show that the presence of a more reactive compound reduces the minimum pre-heating temperature necessary to burn methane. The effect is more pronounced for the addition of CO and very similar for C 3H 8 and H 2. Order of reactivity of the different fuels established in isothermal activity measurements was: CO>H 2≥C 3H 8>CH 4. Under autothermal conditions, nearly complete methane conversion is obtained with catalyst temperatures around 800 °C mainly through heterogeneous reactions, with about 60–70 ppm of unburned CH 4 when pure methane or CO/CH 4 mixtures are used. For H 2/CH 4 and C 3H 8/CH 4 mixtures, emissions of unburned methane are lower, probably due to the proceeding of CH 4 homogeneous oxidation promoted by H and OH radicals generated by propane and hydrogen pyrolysis at such relatively high temperatures. Finally, a steady state multiplicity is found by decreasing the pre-heating temperature from the ignited state. This occurrence can be successfully employed to pilot the catalytic ignition of methane at temperatures close to compressor discharge or easily achieved in regenerative burners. 相似文献
7.
为了进一步探究大型海藻与陆生生物质共热解的协同效应,选取条浒苔与稻壳生物质作为代表进行了单样以及不同混合比例的共热解台架试验。通过三相产物产率的计算,以及生物油产物的GC-MS、FT-IR、热值分析和对气相产物的GC分析,研究了条浒苔与稻壳共热解协同效应的影响。共热解的气相产物产率在各个混合比例下均高于理论值,说明共热解对气相产物的生成具有促进作用,同时共热解气相产物中甲烷、乙烷、乙烯、丙烷为主的小分子烃类物质产率高于理论值,生物油中以乙酸为代表的小分子产物明显增多,分析认为条浒苔灰分中Na、K等碱金属具有促进大分子产物进一步裂解的催化作用,进一步验证了条浒苔与稻壳共热解的协同效应。 相似文献
8.
The synthesis conditions of SiC ultrafine particles from SiH 4 and C 2H 4 using a CO 2 laser were studied and a comparison was made between SiH 4---C 2H 4 and SiH 2Cl 2---C 2H 4 systems. Ultrafine SiC particles were synthesized by irradiating a SiH 4 and C 2H 4 gas mixture with a CO 2 laser at atmospheric pressure. SiC particles were obtained at a laser power of more than 0·92 kW/cm 2. The behavior of the reaction flame temperature and the extent of the laser light absorption by SiH4---C2H4 was different from that of SiH2Cl2---C2H4, although an abrupt temperature increase was observed in both cases. In the case of SiH4---C2H4 an abrupt increase in the laser light absorption was not observed, whilst it was observed in the case of SiH2Cl2---C2H4. This difference resulted from the difference in liability to form solid carbon particles. 相似文献
9.
K、Ca元素以无机态和有机态的形式赋存于生物质内,影响着生物质热解过程中木质素、纤维素及半纤维素分子的断链及解聚过程,进而一定程度地影响着生物质热解气相产物形成与转化。热解反应过程中中间瞬态产物作为气体合成的中间产物对于热解反应最终气相产物的形成具有极为重要的研究意义。将生物质(稻壳)进行了酸洗处理,再定向负载K、Ca元素,利用Py-GC/MS在500~900℃热解温度下,对生物质原料进行了快速热解的实验研究。利用气相色谱质谱仪(GC/MS)对进样延迟时间为20 s时生物质快速热解瞬态轻烃及含氧气态组分的种类及含量进行了在线半定量分析,从而进一步表征了K和Ca元素对生物质快速热解气相组分的影响以及热解反应过程中气相中间产物的形成转化机制。研究结果表明:低温条件下(≤600℃),H-form、K-loaded和Ca-loaded生物质快速热解瞬态气体产物以CO、CO 2、CH 4为主,K与Ca元素促进了生物质热解CO与CO 2的生成。高温条件下(≥700℃),C 3H 6成为20 s瞬态热解过程的主要气相产物,Ca元素对C 3(C 3H 6)等物质的形成具有一定的促进作用,而K元素一定程度上抑制了C 3H 6的生成。 相似文献
10.
含油污泥中石油烃组分复杂,仅靠产物的宏观分析结果难以揭示热解过程组分之间的相互作用。以正十二烷、1-十二烯、甲基环己烷、对二甲苯和1-甲基萘五种化合物分别代表含油污泥中石油烃的链烷烃、链烯烃、环烷烃、单环芳烃和多环芳烃五种组分,构建含油污泥石油烃的模型化合物。采用基于反应力场的分子动力学模拟方法,研究了热解过程中的产物分布及各组分之间的相互作用。结果表明,模型化合物热解产物以H 2和C 1~3的小分子化合物为主,热解前期主要为C 2H 4、C 3H 6,热解后期主要为C 2H 2、C 3H 4和H 2。相对于模型化合物中各组分单独热解,混合热解过程中石油烃各组分的消耗速率明显加快,且热解产物的片段数也有一定程度的增加。根据一级反应动力学模型,石油烃各组分在混合热解过程中的表观活化能有不同程度降低,其中链烷烃、链烯烃和环烷烃的表观活化能分别降低了16.493 kJ/mol、50.571 kJ/mol和146.289 kJ/mol,这从分子模拟层面证明了含油污泥石油烃各组分之间热解的协同作用。 相似文献
11.
将酸洗后的准东煤(H-form coal)进行离子交换得到含羧酸钠的离子交换煤(Na-form coal),再次酸洗脱钠得到的二次酸洗煤(H-form-1 coal)作为对照试样,在固定床反应器上进行热解。借助便携式气体分析仪、热重分析仪和红外光谱仪研究总挥发分和焦油产率、热解气体组分、焦炭反应活性以及焦炭官能团的变化。研究表明:温度高于600℃时,羧酸钠会减小挥发分产率,抑制CH 4、C 2H 4、C 2H 6气体的产生,高于800℃时促进了CO的生成;羧酸钠抑制了焦油的生成且在700℃时抑制作用最为明显;羧酸钠显著提高了焦炭的反应活性,700℃时效果更为明显。羧酸钠的存在对热解过程中煤焦官能团有显著影响。 相似文献
12.
The adsorption of HCN on, its catalytic oxidation with 6% O 2 over 0.5% Pt/Al 2O 3, and the subsequent oxidation of strongly bound chemisorbed species upon heating were investigated. The observed N-containing products were N 2O, NO and NO 2, and some residual adsorbed N-containing species were oxidized to NO and NO 2 during subsequent temperature programmed oxidation. Because N-atom balance could not be obtained after accounting for the quantities of each of these product species, we propose that N 2 and was formed. Both the HCN conversion and the selectivity towards different N-containing products depend strongly on the reaction temperature and the composition of the reactant gas mixture. In particular, total HCN conversion reaches 95% above 250 °C. Furthermore, the temperature of maximum HCN conversion to N 2O is located between 200 and 250 °C, while raising the reaction temperature increases the proportion of NO x in the products. The co-feeding of H 2O and C 3H 6 had little, if any effect on the total HCN conversion, but C 3H 6 addition did increase the conversion to NO and decrease the conversion to NO 2, perhaps due to the competing presence of adsorbed fragments of reductive C 3H 6. Evidence is also presented that introduction of NO and NO 2 into the reactant gas mixture resulted in additional reaction pathways between these NO x species and HCN that provide for lean-NO x reduction coincident with HCN oxidation. 相似文献
13.
在煤热解过程中加入特定的催化剂可以改变煤结构中相关化学键的结合能,使热解在相对温和的条件下进行,促使更多的小分子从煤结构上解离成为产物释放,并调节产物的产率和组成,提高转化率及产物的品质。由于煤化学结构的复杂性,从分子水平研究煤的催化热解行为非常困难。基于此,以煤的催化热解为背景,采用煤模型化合物,借助密度泛函理论(DFT),选取苯甲酸(C 6H 5COOH)为煤基模型,以NiO和Ni为催化剂,研究催化热解过程中催化剂价态改变对煤催化剂热解的作用。DFT结果显示,苯甲酸热解的主要路径为:C 6H 5COOH CO 2+C 6H 6和C 6H 5COOH C 6H 6COO CO 2+C 6H 6;在NiO上的分解路径为:C 6H 5COOH(g) *C 6H 5COO + *H *CO 2 + *C 6H 6 CO 2(g) + C 6H 6(g) ;在金属Ni上的分解路径为:C 6H 5COOH(g) *C 6H 5COOH *C 6H 5COO + *H *CO 2 + *C 6H 6 CO 2(g) + C 6H 6(g) 。Ni基催化剂的加入能够促进C 6H 5COOH的热解,同时改变了苯甲酸的热解路径,但是产物不变。当NiO被还原为金属Ni时,催化效果减弱。 相似文献
14.
This paper deals with the activity of bimetallic potassium–copper and potassium–cobalt catalysts supported on alumina for the reduction of NO x with soot from simulated diesel engine exhaust. The effect of the reaction temperature, the soot/catalyst mass ratio and the presence of C 3H 6 has been studied. In addition, the behavior of two monometallic catalysts supported on zeolite beta (Co/beta and Cu/beta), previously used for NO x reduction with C 3H 6, as well as a highly active HC-SCR catalyst (Pt/beta) has been tested for comparison. The preliminary results obtained in the absence of C 3H 6 indicate that, at temperatures between 250 and 400 °C, the use of bimetallic potassium catalysts notably increases the rate of NO x reduction with soot evolving N 2 and CO 2 as main reaction products. At higher temperatures, the catalysts mainly favor the direct soot combustion with oxygen. In the presence of C 3H 6, an increase in the activity for NO x reduction has been observed for the catalyst with the highest metal content. At 450 °C, the copper-based catalysts (Cu/beta and KCu2/Al 2O 3) show the highest activity for both NO x reduction (to N 2 and CO 2) and soot consumption. The Pt/beta catalyst does not combine, at any temperature, a high NO x reduction with a high soot consumption rate. 相似文献
15.
Several hexaaluminate-related materials were prepared via hydrolysis of alkoxide and powder mixing method for high temperature combustion of CH 4 and C 3H 8, in order to investigate the effect of the concentration of the fuels, O 2 and H 2O on NO x emission and combustion characteristics. Among the hexaaluminate catalysts, Sr 0.8La 0.2MnAl 11O 19− prepared by the alkoxide method exhibited the highest activity for methane combustion and low NO x emission capability. NO x emission at 1500 °C was increased linearly with O 2 concentration, whereas water vapor addition decreased NO x emission in CH 4 combustion over the Sr 0.8La 0.2MnAl 11O 19− catalyst. In the catalytic combustion of C 3H 8 over the Sr 0.8La 0.2MnAl 11O 19− catalyst, the amount of NO x emitted was raised in the temperature range between 1000 and 1500 °C when the C 3H 8 concentration increased from 1 to 2 vol.%. It was found that NO x emission in this temperature range was reduced effectively by adding water vapor. 相似文献
16.
燃煤有机污染物对人类健康和生态环境存在严重危害,而O 2对火焰中有机产物的形成具有明显的调控作用。鉴于煤挥发分燃烧是燃煤过程中至关重要的一环,本文以煤热解气为燃料,通过数值模拟研究了氧化剂侧O 2浓度对对冲扩散火焰中碳氢产物生成特性和机制的影响。结果表明,O 2浓度升高促进了O和OH的生成,进而提高H浓度,突显了含H和OH参与的反应的重要性。此外,乙炔(C 2H 2)、丙炔(PC 3H 4)、炔丙基(C 3H 3)、乙烯基乙炔(C 4H 4)、苯(C 6H 6)和萘(C 10H 8)的浓度均增大。增加O 2浓度促进了C 2H 2向PC 3H 4的转化,并使得C 3H 3更倾向于转化为丁二烯(C 4H 6),而富烯更倾向于通过苯基(C 6H 5)生成C 6H 6,因此C 6H 5作为C 6H 6前体的地位被加强。 相似文献
17.
燃煤有机污染物对人类健康和生态环境存在严重危害,而O 2对火焰中有机产物的形成具有明显的调控作用。鉴于煤挥发分燃烧是燃煤过程中至关重要的一环,本文以煤热解气为燃料,通过数值模拟研究了氧化剂侧O 2浓度对对冲扩散火焰中碳氢产物生成特性和机制的影响。结果表明,O 2浓度升高促进了O和OH的生成,进而提高H浓度,突显了含H和OH参与的反应的重要性。此外,乙炔(C 2H 2)、丙炔(PC 3H 4)、炔丙基(C 3H 3)、乙烯基乙炔(C 4H 4)、苯(C 6H 6)和萘(C 10H 8)的浓度均增大。增加O 2浓度促进了C 2H 2向PC 3H 4的转化,并使得C 3H 3更倾向于转化为丁二烯(C 4H 6),而富烯更倾向于通过苯基(C 6H 5)生成C 6H 6,因此C 6H 5作为C 6H 6前体的地位被加强。 相似文献
18.
为探究典型生物质原料纤维素与多氢原料聚乙烯共热解过程中官能团的相互作用及协同效应,本文利用傅里叶变换红外光谱仪、热裂解-气相色谱/质谱联用仪、热重-质谱及流化床对纤维素及其与聚乙烯混合共同热解实验产物进行分析。傅里叶变换红外光谱实验表明,纤维素红外谱图的主要基团为CH 3、CH、CH 2,多氢原料的加入均会提升碳氢基团的相对含量。热重-质谱实验表明纤维素的实验主要产物为C 3H 8,聚乙烯的加入会提升C 2H 4的离子流强度。热裂解-气相色谱/质谱联用实验表明,纤维素的热解产物以左旋葡聚糖为主,聚乙烯的加入使得纤维素中烃类的含量得到较大幅度的提升,HZSM-5的催化使得芳烃类产物的相对含量得到提升。流化床热解验证实验的总体趋势与PY-GC/MS实验一致,在纤维素与聚乙烯共热解的基础上再加入HZSM-5催化,可以得到最佳的实验效果。 相似文献
19.
运用分子动力学的方法,对轮胎橡胶的热解过程进行了模拟,并结合模拟结果和密度泛函数对其气相产物的反应路径进行推测计算。模拟结果表明,热解过程主要分为两个阶段,低温热解阶段发生的主要反应是橡胶长链断裂形成单体,主要产物为异戊二烯、苯乙烯和1,3-丁二烯;高温热解阶段发生的主要反应是单体进一步生成小分子气体,产物中CH 4、H 2、C 2H 4占大部分,还有少量C 2H 6、C 3H 6。其中CH 3·攻击异戊二烯和苯乙烯单体夺取特定位置的H·是生成CH 4的最优路径,H·攻击苯乙烯单体夺取特定位置的H·是生成H 2的最优路径,CH 2CH·攻击1,3-丁二烯单体夺取特定位置的H·是生成CH 2CH 2的最优路径。本文还将热解产物分别跟天然橡胶单独热解和天然橡胶与丁苯橡胶共热解的热解产物做对比,为废旧轮胎橡胶热解得到特定的气相产物和催化热解提供理论依据。 相似文献
20.
The mechanism of the NO/C 3H 6/O 2 reaction has been studied on a Pt-beta catalyst using transient analysis techniques. This work has been designed to provide answers to the volcano-type activity behaviour of the catalytic system, for that reason, steady state transient switch (C 3H 6/NO/O 2 → C 3H 6/Ar/O 2, C 3H 6/Ar/O 2 → C 3H 6/NO/O 2, C 3H 6/NO/O 2 → Ar/NO/O 2, Ar/NO/O 2 → C 3H 6/NO/O 2, C 3H 6/NO/O 2 → C 3H 6/NO/Ar and C 3H 6/NO/Ar → C 3H 6/NO/O 2) and thermal programmed desorption (TPD) experiments were conducted below and above the temperature of the maximum activity ( Tmax). Below Tmax, at 200 °C, a high proportion of adsorbed hydrocarbon exists on the catalyst surface. There exists a direct competition between NO and O 2 for Pt free sites which is very much in favour of NO, and therefore, NO reduction selectively takes place over hydrocarbon combustion. NO and C 3H 6 are involved in the generation of partially oxidised hydrocarbon species. O 2 is essential for the oxidation of these intermediates closing the catalytic cycle. NO 2 is not observed in the gas phase. Above Tmax, at 230 °C, C 3H 6 ads coverage is negligible and the surface is mainly covered by O ads produced by the dissociative adsorption of O 2. NO 2 is observed in gas phase and carbon deposits are formed at the catalyst surface. From these results, the state of Pt-beta catalyst at Tmax is inferred. The reaction proceeds through the formation of partially oxidised active intermediates (CxHyOzNw) from C 3H 6 ads and NO ads. The combustion of the intermediates with O 2(g) frees the Pt active sites so the reaction can continue. Temperature has a positive effect on the surface reaction producing active intermediates. On the contrary, formation of NO ads and C 3H 6 ads are not favoured by an increase in temperature. Temperature has also a positive effect on the dissociation of O 2 to form O ads, consequently, the formation of NO 2 is favoured by temperature through the oxygen dissociation. NO 2 is very reactive and produces the propene combustion without NO reduction. These facts will determine the maximum concentration of active intermediates and consequently the maximum of activity. 相似文献
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