当前位置: X-MOL 学术Appl. Catal. B Environ. Energy › 论文详情
Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)
Catalytic conversion of pure glycerol over an un-modified H-ZSM-5 zeolite to bio-based aromatics
Applied Catalysis B: Environment and Energy ( IF 22.1 ) Pub Date : 2020-08-27 , DOI: 10.1016/j.apcatb.2020.119467
Songbo He , Kenny Zuur , Dian Sukmayanda Santosa , Andre Heeres , Chuncheng Liu , Evgeny Pidko , Hero Jan Heeres

The catalytic conversion of pure glycerol to bio-aromatics (bio-BTX) over an un-modified H-ZSM-5 (SiO2/Al2O3 molar ratio of 23) via an ex-situ catalytic pyrolysis approach in a continuous tandem-micro reactor at a scale of 1 g glycerol h−1 was investigated. A BTX peak carbon yield of 28.1 ± 0.2 % was obtained at a pyrolysis temperature of 400 °C, catalytic upgrading temperature of 500 °C, atmospheric pressure and a WHSV of 1 h−1. About 70 % of the bound oxygen in glycerol was converted to water. The latter was mainly formed in the catalytic upgrading unit (70 %), though conversion of glycerol to other oxygenates with water formation was also observed in the pyrolysis unit. Catalyst deactivation occurs at a time scale of hours and is mainly due to coke deposition (12.0 wt.%) on the catalyst surface. An oxidative regeneration procedure to remove coke was applied and 5 cycles of reaction-regeneration were performed successfully, though a drop in activity was observed after each cycle due to irreversible catalyst deactivation. Characterization of the fresh, deactivated and regenerated catalysts by various techniques revealed dealumination of the H-ZSM-5 framework and resulted in a dramatic decrease in Brønsted acidity of the catalyst. Dealumination mainly occurred in the catalytic upgrading reactor and to a by far lesser extent during catalyst regeneration. This information is relevant for a better understanding of the process on a molecular level but also for scale-up studies, e.g. for the design of pilot plants.



中文翻译:

在未改性的H-ZSM-5沸石上将纯甘油催化转化为生物基芳烃

纯甘油的催化转化为生物芳烃(BIO-BTX)上的未改性的H-ZSM-5(二氧化硅2 / Al的2 ö 3的23摩尔比)通过一个易地在连续串联催化热解方法研究了规模为1 g甘油h -1的微型反应器。在400°C的热解温度,500°C的催化升级温度,大气压和1 h -1的WHSV下获得BTX峰值碳收率为28.1±0.2%。甘油中约70%的结合氧转化为水。后者主要在催化提质单元中形成(70%),尽管在热解单元中也观察到甘油转化为其他含氧物并形成水。催化剂失活在几小时的时间尺度上发生,这主要归因于在催化剂表面上的焦炭沉积(12.0重量%)。进行了氧化再生程序以除去焦炭,并成功进行了5个循环的反应再生,尽管由于不可逆的催化剂失活,每个循环后活性均下降。通过各种技术对新鲜的,失活的和再生的催化剂进行表征,发现了H-ZSM-5骨架的脱铝反应,并导致催化剂的布朗斯台德酸度急剧下降。脱铝作用主要发生在催化提质反应器中,并且在催化剂再生期间的程度要小得多。这些信息不仅有助于在分子水平上更好地理解该过程,而且还有助于进行放大研究,例如。用于试验工厂的设计。

更新日期:2020-09-15
down
wechat
bug