化工进展 ›› 2022, Vol. 41 ›› Issue (7): 3877-3889.doi: 10.16085/j.issn.1000-6613.2021-1910
收稿日期:
2021-09-07
修回日期:
2021-11-19
出版日期:
2022-07-25
发布日期:
2022-07-23
通讯作者:
赵芸
E-mail:Yangchao_BIT@163.com;zhaoyun@bit.edu.cn
作者简介:
杨超(1996―),男,硕士研究生,研究方向为工业催化。E-mail:
YANG Chao1(), JIAO Qingze1,2, FENG Caihong1, ZHAO Yun1(
)
Received:
2021-09-07
Revised:
2021-11-19
Online:
2022-07-25
Published:
2022-07-23
Contact:
ZHAO Yun
E-mail:Yangchao_BIT@163.com;zhaoyun@bit.edu.cn
摘要:
废旧轮胎因产量高、难降解、污染环境,被称为最难处理的“黑色垃圾”之一。催化裂解是一种处理废旧轮胎的重要手段,可以实现其高效转化与资源化利用,同时得到高附加值的化学产品,如单环芳烃、低碳烯烃与柠檬烯等。本文基于轮胎的物理结构与化学组成、催化裂解过程与裂解产物特征、反应器类型与特征、催化剂类型与作用原理、工艺条件等问题综述了废旧轮胎的催化裂解产物分布规律。通过对比反应器、催化剂与工艺条件对产物分布的影响,进一步分析了当前实现废旧轮胎催化裂解工业化的问题,并基于当前废旧轮胎催化裂解的研究现状,提出应集中设计适应于大规模处理的反应器与配套工艺,同时开发高稳定性与对特定产物高选择性的催化剂,从而实现对废旧轮胎以低能耗、高转化、高价值为特点的资源化利用。
中图分类号:
杨超, 矫庆泽, 冯彩虹, 赵芸. 废旧轮胎催化裂解研究进展[J]. 化工进展, 2022, 41(7): 3877-3889.
YANG Chao, JIAO Qingze, FENG Caihong, ZHAO Yun. Research progress on catalytic cracking of waste tires[J]. Chemical Industry and Engineering Progress, 2022, 41(7): 3877-3889.
表1
轮胎的化学处理方式"
方法 | 主要内容 | 特点 |
---|---|---|
燃烧 | 热值与天然气相当,约为36MJ/kg,可作为燃料使用 | 尾气含有二??英、酚类等致癌物质 |
热解 | 产物分布宽、操作温度高 | |
常规热解 | 在缺氧或惰性气体中高温(500~600℃)降解,可产生气、油及固体残渣 | |
熔融盐热解 | 在氯化锂/氯化钾共熔混合物中分解 | |
微波解聚 | 在氮气和微波条件下,炭黑吸收微波,促进橡胶裂解 | |
共热解 | 与导热剂(如生物质等)共混热解,可降低热解温度,减少积炭和结焦 | |
气化 | 在一定温度下与气化剂共混降解,目标产物是合成气 | 气化剂昂贵、成本高、气体产率低 |
炭化 | 在高温(>1000℃)下,降解形成高品质炭和其他产物 | 实现高温难度大、对工艺设备要求高 |
超临界水氧化 | 在水的超临界(Tc=374.3℃, pc=22.05MPa)和亚临界状态下,以过氧化氢为氧化剂对废旧轮胎颗粒降解,产物以燃料油和固体炭黑为主 | 操作条件要求高、装置复杂 |
催化裂解 | 在隔氧和催化剂的作用下,可降解形成气、液、固体残渣 | 产物分布窄、资源化利用率高 |
表2
轮胎的结构及组成[14]"
结构 | 组成及功能 |
---|---|
胎面 (tread) | 成分为天然或合成橡胶,具有优良的耐摩擦性和热稳定性 |
带层 (belts) | 包括冠带层与带束层等,一般由橡胶、钢和帘子布等多种材料制成,为外层提供结构支撑 |
胎侧 (sidewalls) | 由橡胶制成,主要用来缓冲来自路面的颠簸,同时保证轮胎结构的完整性 |
胎体层 (carcass) | 由涂有天然橡胶的金属制成,支撑轮胎的内部结构 |
内衬层 (inner line) | 成分为低透气性的(卤)丁基橡胶,具有存气、稳压等作用 |
胎圈 (beads) | 主要由钢丝与橡胶制成,具有高的拉伸强度,确保轮胎和轮辋之间的连接 |
胎圈填料 (beads filler) | 保证了胎圈线的刚性部分和内衬之间的过渡连接 |
表4
轮胎裂解常用固体酸催化剂对裂解产物分布的影响"
催化剂 | 催化方式 | 催料比 | 反应器 | 轮胎粉粒径 | (热解/催化温度)/℃ | 裂解产物组成(质量分数)/% | 参考 文献 | |||
---|---|---|---|---|---|---|---|---|---|---|
气体 | 液体 | 固体 | 其他 | |||||||
ZSM-5 | 先热解,再催化 | 0.5 | 常压固定床 | 1cm | 500/400 | 44.66 | 烷基苯系物:24.99 | [ | ||
USY | 先热解,再催化 | 0.5 | 常压固定床 | 1cm | 500/400 | 32.66 | 烷基苯系物:46.10 | |||
热解 | ― | ― | 常压固定床 | 1cm | 500 | 51.98 | 烷基苯系物:83.28 | |||
ZSM-5 | 共同催化热解 | 2g/min | 流化床 | ― | 500 | 19.32 | 约46.68 | 约34 | 芳香族(<C10):13.00 | [ |
HY | 共同催化热解 | 2g/min | 流化床 | ― | 500 | 2.49 | 约62.51 | 约35 | 芳香族(<C10):22.67 | |
热解 | ― | ― | 流化床 | ― | 500 | 3.25 | 约38.25 | 约35 | 芳香族(<C10):7.77 | |
HBeta | 先热解,再催化 | 0.25 | 常压固定床 | 20~40目 | 500/350 | 8 | 51 | 41.5 | 气体中硫:22 | [ |
HY | 先热解,再催化 | 0.25 | 常压固定床 | 20~40目 | 500/350 | 10 | 51.5 | 41.5 | 气体中硫:29 | |
HMOR | 先热解,再催化 | 0.25 | 常压固定床 | 20~40目 | 500/350 | 11 | 48 | 41 | 气体中硫:27 | |
Cu/Hβ | 先热解,再催化 | 0.25 | 常压固定床 | 20~40目 | 500/350 | 11.5 | 47.5 | 41 | 气体中硫:20 | |
Cu/HY | 先热解,再催化 | 0.25 | 常压固定床 | 20~40目 | 500/350 | 12 | 47 | 41 | 气体中硫:22 | |
Cu/HMOR | 先热解,再催化 | 0.25 | 常压固定床 | 20~40目 | 500/350 | 11 | 47.5 | 41.5 | 气体中硫:18 | |
热解 | ― | ― | 常压固定床 | 20~40目 | 500/350 | 11.5 | 46.5 | 42 | 气体中硫:20 | |
Ni/Hβ | 先热解,再催化 | 0.25 | 常压固定床 | ― | 500/350 | 8 | 49 | 43 | 气体中硫:20 | [ |
Ni/HMOR | 先热解,再催化 | 0.25 | 常压固定床 | ― | 500/350 | 10 | 46 | 44 | 气体中硫:18 | |
Ni/HY | 先热解,再催化 | 0.25 | 常压固定床 | ― | 500/350 | 7 | 51 | 42 | 气体中硫:12 | |
Ni/HZSM-5 | 先热解,再催化 | 0.25 | 常压固定床 | ― | 500/350 | 12 | 44 | 44 | 气体中硫:15 | |
热解 | ― | ― | 常压固定床 | ― | 500/350 | 12 | 47.5 | 40.5 | 气体中硫:29 | |
Fe/KL | 先热解,再催化 | 0.25 | 常压固定床 | ― | 500/350 | 12.1 | 42.9 | 42.5 | BTEX:58 | [ |
Fe/HMOR | 先热解,再催化 | 0.25 | 常压固定床 | ― | 500/350 | 13.3 | 42 | 42.4 | BTEX:52 | |
Fe/Hβ | 先热解,再催化 | 0.25 | 常压固定床 | ― | 500/350 | 11.4 | 43.6 | 41.7 | BTEX:13 | |
Fe/HZSM-5 | 先热解,再催化 | 0.25 | 常压固定床 | ― | 500/350 | 16.2 | 39 | 41.8 | BTEX:23 | |
热解 | ― | ― | 常压固定床 | ― | 500 | 11.6 | 46.0 | 42.4 | BTEX:20 | |
Ru/MCM-41 | 先热解,再催化 | 0.25 | 常压固定床 | ― | 500/350 | 30 | 25.5 | 44.5 | C1~C4:29.1 | [ |
MCM-41 | 先热解,再催化 | 0.25 | 常压固定床 | ― | 500/350 | 15 | 38 | 47 | C1~C4:11.8 | |
热解 | ― | ― | 常压固定床 | ― | 500 | 11 | 47 | 42 | C1~C4:8 | |
Cu/ZSM-5 | 先热解,再催化 | 0.25 | 常压固定床 | 1~3mm | 430/500 | 30 | 65 | 5 | 气体中硫:66 | [ |
Zn/ZSM-5 | 先热解,再催化 | 0.25 | 常压固定床 | 1~3mm | 430/500 | 28.5 | 66 | 5.5 | 气体中硫:65 | |
Cu/MCM-41 | 先热解,再催化 | 0.25 | 常压固定床 | 1~3mm | 430/500 | 27 | 67.5 | 5.5 | 气体中硫:62 | |
Zn/MCM-41 | 先热解,再催化 | 0.25 | 常压固定床 | 1~3mm | 430/500 | 27.5 | 68 | 4.5 | 气体中硫:75 | |
热解 | ― | ― | 常压固定床 | 1~3mm | 430/500 | 25 | 71 | 4 | 气体中硫:67 | |
Hβ | 共同催化热解 | 0.3 | 常压固定床 | 3~5mm | 550 | 32.5 | 34 | 33.5 | ― | [ |
HUSY | 共同催化热解 | 0.3 | 常压固定床 | 3~5mm | 550 | 32 | 33 | 35 | ― | |
TiO2 | 共同催化热解 | 0.3 | 常压固定床 | 3~5mm | 550 | 30.5 | 26.5 | 43 | ― | |
热解 | ― | ― | 常压固定床 | 3~5mm | 550 | 28.5 | 28.5 | 43 | ― |
表5
轮胎裂解常用固体碱催化剂对裂解产物分布的影响"
催化剂 | 催化方式 | 催料比 | 反应器 | 轮胎粉粒径 | (热解/催化 温度)/℃ | 裂解产物组成(质量分数)/% | 参考文献 | |||
---|---|---|---|---|---|---|---|---|---|---|
气体 | 液体 | 固体 | 其他 | |||||||
MgO | 先热解,再催化 | 0.03 | 常压固定床 | 2~3mm | 550/550 | 20 | 38 | 42 | 固体中S元素的残余:2.68 | [ |
Al2O3 | 先热解,再催化 | 0.03 | 常压固定床 | 2~3mm | 550/550 | 33 | 26 | 41 | 固体中S元素的残余:2.63 | |
CaCO3 | 先热解,再催化 | 0.03 | 常压固定床 | 2~3mm | 550/550 | 37 | 23 | 40 | 固体中S元素的残余:2.00 | |
ZSM-5 | 先热解,再催化 | 0.03 | 常压固定床 | 2~3mm | 550/550 | 25 | 35 | 40 | 固体中S元素的残余:2.59 | |
热解 | ― | ― | 常压固定床 | 2~3mm | 550/550 | 19 | 36 | 45 | 固体中S元素的残余:2.70 | |
CaO | 共同催化热解 | ― | 真空固定床 | 20~60目 | 520 | 14.9 | 48.84 | 36.26 | H2S:60 | [ |
ZnO | 共同催化热解 | ― | 真空固定床 | 20~60目 | 520 | 12.16 | 47.49 | 36.56 | H2S:25 | |
CaO/TiO2 | 共同催化热解 | ― | 真空固定床 | 20~60目 | 520 | 18.46 | 45.24 | 36.30 | H2S:55 | |
ZnO/TiO2 | 共同催化热解 | ― | 真空固定床 | 20~60目 | 520 | 24.82 | 39.98 | 35.20 | H2S:35 | |
热解 | ― | ― | 真空固定床 | 20~60目 | 520 | 16.72 | 45.96 | 37.32 | H2S:195 | |
Al2O3 | 共同催化热解 | ― | 常压固定床 | 5~10mm | 400 | 21 | 23.2 | 55.8 | 轻质油的相对密度:0.8288 | [ |
SiO2 | 共同催化热解 | ― | 常压固定床 | 5~10mm | 400 | 15.5 | 28.2 | 56.3 | 轻质油的相对密度:0.799 | |
Al2O3+SiO2 | 共同催化热解 | ― | 常压固定床 | 5~10mm | 400 | 5 | 14.8 | 80.2 | 轻质油的相对密度:0.7575 | |
CaC2 | 共同催化裂解 | 0.2 | 常压固定床 | 5~10mm | 400 | 29.6 | 38.4 | 32 | ― | [ |
热解 | ― | ― | 常压固定床 | 5~10mm | 400 | 37 | 22.8 | 40.2 | ― | |
Na2CO3 | 共同催化裂解 | 0.03 | 真空固定床 | 20~60目 | 500 | 14.6 | 47.8 | 37.6 | 低热值:18.1 | [ |
NaOH | 共同催化裂解 | 0.03 | 真空固定床 | 20~60目 | 500 | 13.3 | 48.1 | 38.6 | 低热值:16.9 | |
热解 | ― | ― | 真空固定床 | 20~60目 | 500 | 21.8 | 42.1 | 26.1 | 低热值:20.7 |
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