文献综述

1.1 背景及意义

空气，一个与人类生存密切相关的物质。目前，由于城市的发展、废气污染物的不节制排放，导致了许多的废气污染物直接进入到空气中，导致目前许多地方出现雾霾、空气灰尘颗粒漂浮等现象。因此，环境的保护、空气垃圾的过滤成为了目前人们一项十分紧迫的研究课题。

生物质能是继煤、石油和天然气三大化石能源之后的第四位能源ADDIN CNKISM.Ref.{ABB68EB312D34b47B50082E1C88DEFAC}^[2] 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，同时也是唯一能够储存和运输的可再生能源ADDIN CNKISM.Ref.{94516CC781194bc6A93556DDCA2554F6}^[3] 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，是唯一能替代化石能源转化为燃料以及其它化工原料实现炭资源循环利用的可再生资源ADDIN CNKISM.Ref.{59C1FA5C708E4f4d95FF863165AABB12}^[4] 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。同化石燃料相比，生物质能具有可再生、低污染，广泛分布，总量十分丰富等一系列显著优点。目前，我国可利用的生物质资源总量达到700 Mt标准煤，并且总量持续增加ADDIN CNKISM.Ref.{80A5F948DC1B47879516ABAAEDBABBDB}^[5] 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。

生物质气化是生物质能高品位利用的一种主要技术，其原理是将固态生物质原料在高温下转换成高品位的可燃气体ADDIN CNKISM.Ref.{8A5DD6FFC52345868C8E37AF25AA1876}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。此过程虽然产生可燃气体，但同时也在气化过程中产生了焦油等污染物。作为焦油中的污染物#8212;#8212;轻芳烃，其由于具有极强的致癌性，使工业生产上对其去除尤为重视。因此，控制轻芳烃的排放污染成为了国内外的研究热点。

轻芳烃目前在全世界各类生活生产中都有产生，垃圾的焚烧、汽车尾气的随意排放、烟草以及煤、石油的不完全燃烧，均会产生大量的轻芳烃。美国国家环保署1979年公布的129种优先检测监控的污染物中，轻芳烃就有16种。轻芳烃属于半挥发性有机化合物，在常温下轻芳烃以气相和固相共存^[3]。近年来，轻芳烃的排放越来越多，导致目前许多人类由于环境的污染而不得不生病治疗。为了进一步的探究轻芳烃的脱除机理，完善当前现有的轻芳烃脱除技术，我选择轻芳烃的吸附、脱附实验研究，希望通过自己的一份力量，能够为此项研究事业作出一点贡献。

1.2 轻芳烃的特征及分类

多环芳烃分为轻多环芳烃（低环轻芳烃，2~3环）和重多环芳烃（高环多环芳烃，≥4环）。重轻芳烃沸点较高，常温下处于固态或者液态，扩散到空气中大多数会附着在颗粒物上，可随着尘粒长期漂浮在空气中，并且可以随着粒径小于2.5μm的颗粒通过呼吸道、消化道、皮肤等进入人体，严重危害人体健^[4]。 虽然重轻芳烃危害较大，但是，工业生产应用中可以通过旋风除尘器、静电沉积法捕集或者利用降温激冷除去，而轻芳烃（2~3环）大多处于中等沸点，排放到大气中主要以气态形式存在，相比重轻芳烃更难被捕集，也不易通过冷却激冷的方式除去。故本课题主要是研究轻芳烃的去除。

1.3国内外轻芳烃去除进展

荷兰能源研究中心（Energy Research Center of the Netherlands，ECN）的 Bergman 等ADDIN CNKISM.Ref.{FCD2246D28DA4b62B4935F1BF0666F51}^[12] 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根据分子量和分子直径，可将焦油分为5类，如表1所示。

表1焦油分类

其中轻芳烃是第三类轻质芳烃和部分第二类焦油（苯酚）和部分第四类焦油（萘）。作为污染性强的有机污染物来讲，轻芳烃的去除方法主要是催化裂解法和吸附法^[7]。

1.3.1催化裂解法

催化裂解法针对轻轻芳烃主要是通过催化剂，将轻轻芳烃催化裂解成更小分子加以脱除。其关键是高效催化剂的研发。常见的催化剂有白云石、碱金属化合物催化剂、碳基催化剂等。但是催化裂解法主要目的是消除轻轻芳烃，相对本文主要介绍的吸附回收脱除，成本较高，技术不够成熟，因此，本课题对催化裂解法不作详细介绍。

1.3.2吸附法

吸附过程很早就被人们发现和利用，将其作为一个工业上的辅助单元过程，早已获得广泛的应用。近几十年来，由于吸附工艺的不断发展进步，因而使得吸附分离过程在化工、石油，尤其是环保领域中受到越来越广泛的应用，成为不可或缺的技术手段。

吸附技术主要是通过吸附剂与吸附质之间电荷转移的相互作用力、范德华力和静电力，使得吸附质在吸附剂上富集，从而实现分离与净化的方法。与催化裂解法等其他方法相比，吸附法具有脱除效率高、净化彻底、能耗低、操作方便、易与推广等独特的优点。更重要的是，大部分轻芳烃是重要的化工原料，通过吸附法吸附轻芳烃，后续可以通过各种手段对吸附剂进行再生解吸，将轻芳烃进行回收利用，大大地降低了成本。

近年来，国内外在利用吸附法脱除轻芳烃的研究，主要从吸附剂的选择和吸附过程的影响机理等方面来阐述吸附法在该领域的研究进展和方向。故我们从这两方面进行深入的探讨研究。

I. 吸附剂的选择

对于吸附剂的选择，除了要求吸附剂具有高选择性，根据不同的目的还要求具有其他的性能。如低浓度或低压力时的大吸附量，合适的比表面积和孔径分布，容易再生，性质稳定，寿命长，价格低廉等。因此，吸附剂的性能是决定轻轻芳烃吸附脱除效率的关键因素。

在吸附脱除轻芳烃方面，目前的研究主要集中在对比不同材质吸附剂的实际脱除效果。Tseng等^[6]对比了表面活性剂改性前后脱硫吸附剂Ca(OH)₂对烟道气中轻芳烃、BTEX的脱除效果^[24]，发现Ca基脱硫吸附剂对芳烃类有机物也有很好的净化能力。马正月等[7]研究六种吸附剂对电厂烟气排放的3种典型轻芳烃（萘、芴、菲）的吸附脱除行为^[25]，表明煤质活性炭对萘、芴、菲的吸附性能明显优于分子筛、Al₂O₃和半焦吸附剂，同时发现轻芳烃的吸附量与活性炭的表面积和微孔体积之间存在着很好的复相关性。

II. 吸附过程的影响机理

吸附过程影响因子的确定和详细表达是目前开展最广的研究内容。在大量研究^[8-17]的对比中发现，吸附剂对轻轻芳烃、的吸附性能与吸附剂的比表面积、微孔率、中孔率和孔径分布等结构特性有着密切的关系；同时，吸附剂的表面化学性质、吸附质的物化特性、吸附质之间的相互作用（竞争吸附）、吸附过程的操作条件等均能对最终的脱除效果产生影响。

1.4多组分轻芳烃吸附脱附研究

在实际工业应用中，吸附分离所遇到的体系几乎都是混合物，当混合物被吸附时，混合物的任一组分被吸附的量都会受到另一组分的存在的影响。一般来说，多组分吸附时，除了各组分的吸附亲和力大小不同外，各吸附组分之间还有相互作用和竞争的效应，使得吸附过程复杂化。

Yashushi等^[20]运用高硅分子筛研究了对二甲苯蒸汽和正丁酸蒸汽间的吸附竞争，结果表明两组分的吸附量随各自浓度的变化而变化。Mastral等^[21]在研究中发现，挥发性与PAHs在相同吸附剂上的吸附量有着密切的关系，即挥发性弱（高环）的PAHs吸附量更高。通过分析萘、芴、菲、荧蒽、芘组成的10 种二元混合气体的吸附行为，发现在吸附过程中，会出现弱吸附组分被强吸附组分取代的现象，并且弱吸附组分决定了体系的吸附效率。在另外的研究中^[22]，Mastral 等还发现CO₂的存在能显著降低吸附剂对菲的脱除性能。国内谢裕坛等在研究活性炭对混合蒸汽中多环有机物的吸附中发现多组分吸附时有如下趋势：1）分子量较大的有机物的吸附通常能置换低分子量有机物的吸附；2）多组分蒸汽同时吸附加大了传质区的长度，有可能需要增加吸附床长度；3）多组分吸附时，给定的系统的效率会降低。

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文献综述

1.1 背景及意义

空气，一个与人类生存密切相关的物质。目前，由于城市的发展、废气污染物的不节制排放，导致了许多的废气污染物直接进入到空气中，导致目前许多地方出现雾霾、空气灰尘颗粒漂浮等现象。因此，环境的保护、空气垃圾的过滤成为了目前人们一项十分紧迫的研究课题。

生物质能是继煤、石油和天然气三大化石能源之后的第四位能源ADDIN CNKISM.Ref.{ABB68EB312D34b47B50082E1C88DEFAC}^[2] 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，同时也是唯一能够储存和运输的可再生能源ADDIN CNKISM.Ref.{94516CC781194bc6A93556DDCA2554F6}^[3] 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，是唯一能替代化石能源转化为燃料以及其它化工原料实现炭资源循环利用的可再生资源ADDIN CNKISM.Ref.{59C1FA5C708E4f4d95FF863165AABB12}^[4] 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。同化石燃料相比，生物质能具有可再生、低污染，广泛分布，总量十分丰富等一系列显著优点。目前，我国可利用的生物质资源总量达到700 Mt标准煤，并且总量持续增加ADDIN CNKISM.Ref.{80A5F948DC1B47879516ABAAEDBABBDB}^[5] 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。

生物质气化是生物质能高品位利用的一种主要技术，其原理是将固态生物质原料在高温下转换成高品位的可燃气体ADDIN CNKISM.Ref.{8A5DD6FFC52345868C8E37AF25AA1876}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。此过程虽然产生可燃气体，但同时也在气化过程中产生了焦油等污染物。作为焦油中的污染物#8212;#8212;轻芳烃，其由于具有极强的致癌性，使工业生产上对其去除尤为重视。因此，控制轻芳烃的排放污染成为了国内外的研究热点。

轻芳烃目前在全世界各类生活生产中都有产生，垃圾的焚烧、汽车尾气的随意排放、烟草以及煤、石油的不完全燃烧，均会产生大量的轻芳烃。美国国家环保署1979年公布的129种优先检测监控的污染物中，轻芳烃就有16种。轻芳烃属于半挥发性有机化合物，在常温下轻芳烃以气相和固相共存^[3]。近年来，轻芳烃的排放越来越多，导致目前许多人类由于环境的污染而不得不生病治疗。为了进一步的探究轻芳烃的脱除机理，完善当前现有的轻芳烃脱除技术，我选择轻芳烃的吸附、脱附实验研究，希望通过自己的一份力量，能够为此项研究事业作出一点贡献。

1.2 轻芳烃的特征及分类

多环芳烃分为轻多环芳烃（低环轻芳烃，2~3环）和重多环芳烃（高环多环芳烃，≥4环）。重轻芳烃沸点较高，常温下处于固态或者液态，扩散到空气中大多数会附着在颗粒物上，可随着尘粒长期漂浮在空气中，并且可以随着粒径小于2.5μm的颗粒通过呼吸道、消化道、皮肤等进入人体，严重危害人体健^[4]。 虽然重轻芳烃危害较大，但是，工业生产应用中可以通过旋风除尘器、静电沉积法捕集或者利用降温激冷除去，而轻芳烃（2~3环）大多处于中等沸点，排放到大气中主要以气态形式存在，相比重轻芳烃更难被捕集，也不易通过冷却激冷的方式除去。故本课题主要是研究轻芳烃的去除。

1.3国内外轻芳烃去除进展

荷兰能源研究中心（Energy Research Center of the Netherlands，ECN）的 Bergman 等ADDIN CNKISM.Ref.{FCD2246D28DA4b62B4935F1BF0666F51}^[12] 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根据分子量和分子直径，可将焦油分为5类，如表1所示。

表1焦油分类