江苏大学汽车与交通工程学院,江苏 镇江 212013
朱勇晨(1994—),男,硕士研究生,1092280926@qq.com
李小华(1971—),男,博士,教授,lixiaohua@ujs.edu.cn
收稿:2018-12-28,
修回:2019-02-20,
网络首发:2026-07-24,
纸质出版:2019-05-05
移动端阅览
朱勇晨, 李小华, 张小雷, 胡超, 董文斌, 程静峰, 邵珊珊. NTP再生La改性多级孔HZSM-5及催化提质生物油的试验研究[J]. 化工学报, 2019, 70(5): 1795-1803
ZHU Yongchen, LI Xiaohua, ZHANG Xiaolei, HU Chao, DONG Wenbin, CHENG Jingfeng, SHAO Shanshan. Study on regeneration of La modified multistage pore HZSM-5 by NTP and catalytic upgrading of bio-oil[J]. CIESC Journal, 2019, 70(5): 1795-1803
朱勇晨, 李小华, 张小雷, 胡超, 董文斌, 程静峰, 邵珊珊. NTP再生La改性多级孔HZSM-5及催化提质生物油的试验研究[J]. 化工学报, 2019, 70(5): 1795-1803 DOI: 10.11949/j.issn.0438-1157.20181525.
ZHU Yongchen, LI Xiaohua, ZHANG Xiaolei, HU Chao, DONG Wenbin, CHENG Jingfeng, SHAO Shanshan. Study on regeneration of La modified multistage pore HZSM-5 by NTP and catalytic upgrading of bio-oil[J]. CIESC Journal, 2019, 70(5): 1795-1803 DOI: 10.11949/j.issn.0438-1157.20181525.
以氧气为气源,利用低温等离子体(NTP)喷射系统,在不同温度下对结焦失活的La改性多级孔HZSM-5分子筛进行再生,采用TG、XRD、Py-IR及N
2
吸附-脱附等测试技术对再生前后催化剂的理化性质进行表征,并利用再生催化剂进行在线催化提质生物油试验。结果表明,再生温度为250℃时,失活La改性多级孔HZSM-5分子筛再生效果最好,去除了97.4%的积炭,其表面结晶度、酸性、比表面积和孔容恢复程度最高。再生温度上升至300℃时,O
3
分解较多,此时O
3
分解已经成为积炭氧化分解的限制因素,排气中CO
2
和CO浓度峰值减小,失活催化剂再生效果有所下降。再生温度为250℃时,再生催化剂催化性能恢复最好,制得的生物油高位热值最大(36.48 MJ/kg),烃类含量最高(40.51%),其理化性质与新鲜催化剂制得的生物油理化性质最接近。
Regeneration experiments of La modified multistage pore HZSM-5 zeolite were carried out at different regeneration temperatures by non-thermal plasma (NTP) spray system with oxygen as gas source. The physicochemical properties of La modified multistage pore HZSM-5 zeolite before and after regeneration were characterized by TG
XRD
Py-IR and N
2
adsorption-desorption. The experiments of on-line catalytic upgrading of bio-oil were carried out over regenerated catalyst. The results showed that when regeneration temperature was 250℃
the deactivated La modified multistage pore HZSM-5 zeolite had the best regeneration effect
97.4% of coke was removed
and the surface crystallinity
acidity
specific surface area and pore volume recovery were the best. When regeneration temperature rose to 300℃
the decomposition amount of O
3
was more. At this time
the decomposition of O
3
had become the limiting factor for oxidative decomposition of coke. The peaks of CO
2
and CO concentration decreased
and the regeneration effect of deactivated catalyst declined. When regeneration temperature was 250℃
the catalytic performance recovery of regenerated catalyst was the best. The bio-oil produced by regenerated catalyst had the highest heating value (36.48 MJ/kg) and the highest hydrocarbon content (40.51%)
and its physical and chemical properties were closest to that of bio-oil produced by fresh catalyst.
Dan C , Wang L , Abolghasem S , et al . Characterization of the physical and chemical properties of the distillate fractions of crude bio-oil produced by the glycerol-assisted liquefaction of swine manure [J ] . Fuel , 2014 , 130 : 251 - 256 .
Xu L , Cheng J , Liu P , et al . Production of bio-fuel oil from pyrolysis of plant acidified oil [J ] . Renewable Energy , 2019 , 130 : 910 - 919 .
Yan B , Zhang S , Chen W , et al . Pyrolysis of tobacco wastes for bio-oil with aroma compounds [J ] . Journal of Analytical and Applied Pyrolysis , 2018 , 136 : 248 - 254 .
Hu C S , Zhagn H Y , Xiao R . Catalytic fast pyrolysis of biomass over core-shell HZSM-5@silicalite-1 in a bench-scale two-stage fluidized-bed/fixed-bed reactor [J ] . Journal of Analytical and Applied Pyrolysis , 2018 , 136 : 27 - 34 .
Li X H , Zhang X L , Shao S S , et al . Catalytic upgrading of pyrolysis vapor from rape straw in a vacuum pyrolysis system over La/HZSM-5 with hierarchical structure [J ] . Bioresource Technology , 2018 , 259 : 191 - 197 .
刘亚华 , 李扬 , 王科 , 等 . 二甲醚羰基化催化剂的烧炭再生 [J ] . 化工学报 , 2017 , 68 ( 10 ): 3816 - 3822 .
Liu Y H , Li Y , Wang K , et al . Charcoal regeneration of dimethyl ether carbonylation catalyst [J ] . CIESC Journal , 2017 , 68 ( 10 ): 3816 - 3822 .
刘守新 , 张世润 , 孙承林 . 木质活性炭的光催化再生 [J ] . 林产化学与工业 , 2003 , ( 2 ): 12 - 16 .
Liu S X , Zhang S R , Sun C L . Photocatalytic regeneration of woody activated carbon [J ] . Chemistry and Industry of Forest Products , 2003 , ( 2 ): 12 - 16 .
于丽丽 , 易红宏 , 宁平 , 等 . 改性活性炭水解COS催化剂的再生方法 [J ] . 中南大学学报(自然科学版) , 2011 , 42 ( 3 ): 841 - 847 .
Yu L L , Yi H H , Ning P , et al . Regeneration method of modified activated carbon hydrolyzed COS catalyst [J ] . Journal of Central South University(Natural Science) , 2011 , 42 ( 3 ): 841 - 847 .
López A , de Marco I , Caballero B M , et al . Deactivation and regeneration of ZSM-5 zeolite in catalytic pyrolysis of plastic wastes [J ] . Waste Management , 2011 , 31 ( 8 ): 1852 - 1858 .
Serrano D P , Aguado J , Rodríguez J M , et al . Catalytic cracking of polyethylene over nanocrystalline HZSM-5: catalyst deactivation and regeneration study [J ] . Journal of Analytical and Applied Pyrolysis , 2007 , 79 ( 1 ): 456 - 464 .
Li X Y , Li P , PAN X L , et al . Deactivation mechanism and regeneration of carbon nanocomposite catalyst for acetylene hydrochlorination [J ] . Applied Catalysis B: Environmental , 2017 , 210 : 116 - 120 .
Wang W Z , Wang H L , Zhu T L , et al . Removal of gas phase low-concentration toluene over Mn, Ag and Ce modified HZSM-5 catalysts by periodical operation of adsorption and non-thermal plasma regeneration [J ] . Journal of Hazardous Materials , 2015 , 292 : 70 - 78 .
Okubo M , Arita N , Kuroki T , et al . Carbon particulate matter incineration in diesel engine emissions using indirect nonthermal plasma processing [J ] . Thin Solid Films , 2007 , 515 ( 9 ): 4289 - 4295 .
Li X H , Li W J , Cai Y X , et al . Deposit removal in EGR cooler and effectiveness improvement by non-thermal plasma reactor with different gas sources [J ] . Applied Thermal Engineering , 2017 , 111 : 694 - 702 .
施蕴曦 , 蔡忆昔 , 王静 , 等 . 空气流量对低温等离子体再生DPF的影响 [J ] . 江苏大学学报(自然科学版) , 2017 , 38 ( 5 ): 509 - 515 .
Shi Y X , Cai Y X , Wang J , et al . Effect of air flow on low temperature plasma regeneration DPF [J ] . Journal of Jiangsu University(Natural Science Edition) , 2017 , 38 ( 5 ): 509 - 515 .
郑益 , 蔡忆昔 , 陈亚运 , 等 . 再生温度对NTP再生EGR冷却器的影响 [J ] . 内燃机工程 , 2016 , 37 ( 6 ): 210 - 215 .
Zheng Y , Cai Y X , Chen Y Y , et al . Effect of regeneration temperature on NTP regenerative EGR cooler [J ] . Internal Combustion Engine Engineering , 2016 , 37 ( 6 ): 210 - 215 .
邵珊珊 . 生物质催化热解中催化剂积炭与再生特性研究 [D ] . 南京 : 东南大学 , 2016 .
Shao S S . Study on catalyst carbon deposition and regeneration characteristics in biomass catalytic pyrolysis [D ] . Nanjing : Southeast University , 2016 .
张瑾 , 李小华 , 董良秀 , 等 . 碱处理HZSM-5分子筛在线催化提质生物油 [J ] . 燃料化学学报 , 2017 , 45 ( 7 ): 828 - 836 .
Zhang J , Li X H , Dong L X , et al . On-line catalytic catalyzed upgrading of bio-oil by alkali-treated HZSM-5 molecular sieve [J ] . Journal of Fuel Chemistry , 2017 , 45 ( 7 ): 828 - 836 .
Chu L B , Wang J L . Regeneration of sulfamethoxazole-saturated activated carbon using gamma irradiation [J ] . Radiation Physics and Chemistry , 2017 , 130 : 391 - 396 .
Calafta A , Sanchez N . Production of carbon nanotubes through combination of catalyst reduction and methane decomposition over Fe–Ni/ZrO 2 catalysts prepared by the citrate method [J ] . Applied Catalysis A: General , 2016 , 528 : 14 - 23 .
Jia L Y , Farouha A , Pinard L , et al . New routes for complete regeneration of coked zeolite [J ] . Applied Catalysis B: Environmental , 2017 , 219 : 82 - 91 .
唐松山 , 泮泽优 , 张长森 , 等 . 碱改性HZSM-5催化热解木质素催化剂失活分析 [J ] . 化工学报 , 2017 , 68 ( 12 ): 4739 - 4749 .
Tang S S , Pan Z Y , Zhang C S , et al . Deactivation analysis of catalyzed pyrolysis lignin catalyst by alkali-modified HZSM-5 [J ] . CIESC Journal , 2017 , 68 ( 12 ): 4739 - 4749 .
陆强 , 李文志 , 张栋 , 等 . 锯末快速热解气的在线催化裂解 [J ] . 化工学报 , 2009 , 60 ( 2 ): 351 - 357 .
Lu Q , Li W Z , Zhang D , et al . On-line catalytic cracking of rapid pyrolysis gas from sawdust [J ] . CIESC Journal , 2009 , 60 ( 2 ): 351 - 357 .
施梅勤 , 郑慧新 , 魏爱平 , 等 . Zn助剂对WC/HZSM-5催化正己烷芳构化性能影响 [J ] . 化工学报 , 2015 , 66 ( 2 ): 553 - 560 .
Shi M Q , Zheng H X , Wei A P , et al . Effect of Zn promoter on the aromatization performance of n -hexane catalyzed by WC/HZSM-5 [J ] . CIESC Journal , 2015 , 66 ( 2 ): 553 - 560 .
张向京 , 马仁娟 , 孙瑞钰 , 等 . HZSM-5催化剂在MTG反应中的积炭失活 [J ] . 化工学报 , 2015 , 66 ( 9 ): 3483 - 3489 .
Zhang X J , Ma R J , Sun R Y , et al . Carbon deposition inactivation of HZSM-5 catalyst in MTG reaction [J ] . CIESC Journal , 2015 , 66 ( 9 ): 3483 - 3489 .
Fan Y S , Cai Y X , Li X H , et al . Regeneration of the HZSM-5 zeolite deactivated in the upgrading of bio-oil via non-thermal plasma injection (NTPI) technology [J ] . Journal of Analytical and Applied Pyrolysis , 2015 , 111 : 209 - 215 .
Yang Y J , Jia J B , Liu Y , et al . The effect of tungsten doping on the catalytic activity of α-MnO 2 nanomaterial for ozone decomposition under humid condition [J ] . Applied Catalysis A: General , 2018 , 562 : 132 - 141 .
Jiang N , Guo L J , Qiu C , et al . Reactive species distribution characteristics and toluene destruction in the three-electrode DBD reactor energized by different pulsed modes [J ] . Chemical Engineering Journal , 2018 , 350 : 12 - 19 .
Guan B , Lin H , Zhan R , et al . Catalytic combustion of soot over Cu, Mn substitution CeZrO 2- δ nanocomposites catalysts prepared by self-propagating high-temperature synthesis method [J ] . Chemical Engineering Science , 2018 , 189 : 320 - 339 .
Lydia K E , Liu J , Sotira Y , et al . Contribution of acidic components to the total acid number (TAN) of bio-oil [J ] . Fuel , 2017 , 200 : 171 - 181 .
Leng L , Li H , Yuan X , et al . Bio-oil upgrading by emulsification/microemulsification: a review [J ] . Energy , 2018 , 161 : 214 - 232 .
赵岩 , 刘银 . HZSM-5分子筛催化热裂解生物质制备芳烃化合物 [J ] . 化工新型材料 , 2017 , 45 ( 2 ): 145 - 147 .
Zhao Y , Liu Y . Preparation of aromatic compounds by catalytic pyrolysis of biomass by HZSM-5 molecular sieve [J ] . New Chemical Materials , 2017 , 45 ( 2 ): 145 - 147 .
Melchor J J , Fortes I C P . Bio-oil production by pyrolysis of metal soaps derived from macauba pulp oil [J ] . Journal of Analytical and Applied Pyrolysis , 2018 , 135 : 101 - 110 .
Rahman M M , Liu R H , Cai J M . Catalytic fast pyrolysis of biomass over zeolites for high quality bio-oil — a review [J ] . Fuel Processing Technology , 2018 , 180 : 32 - 46 .
刘莎 , 蔡忆昔 , 樊永胜 , 等 . MCM-41分子筛在线提质生物油工艺优化及耐久性分析 [J ] . 林产化学与工业 , 2016 , 36 ( 4 ): 55 - 63 .
Liu S , Cai Y X , Fan Y S , et al . Process optimization and durability analysis of MCM-41 molecular sieve on-line bio-oil improvement [J ] . Chemistry and Industry of Forest Products , 2016 , 36 ( 4 ): 55 - 63 .
0
浏览量
1
下载量
0
CSCD
关联资源
相关文章
相关作者
相关机构
京公网安备11010102001995号