Selective preparation of light aromatic hydrocarbons from catalytic fast pyrolysis vapors of coal tar asphaltene over transition metal ion modified zeolites

doi:10.1016/j.cjche.2021.06.006

Chinese Journal of Chemical Engineering ›› 2021, Vol. 35 ›› Issue (7): 275-287.DOI: 10.1016/j.cjche.2021.06.006

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Selective preparation of light aromatic hydrocarbons from catalytic fast pyrolysis vapors of coal tar asphaltene over transition metal ion modified zeolites

Yongqi Liu, Qiuxiang Yao, Ming Sun, Xiaoxun Ma

School of Chemical Engineering, Northwest University, International Science & Technology Cooperation Base of MOST for Clean Utilization of Hydrocarbon Resources, Chemical Engineering Research Center of the Ministry of Education for Advanced Use Technology of Shanbei Energy, Shaanxi Research Center of Engineering Technology for Clean Coal Conversion, Collaborative Innovation Center for Development of Energy and Chemical Industry in Northern Shaanxi, Xi'an 710069, China

Received:2021-02-20 Revised:2021-06-08 Online:2021-09-30 Published:2021-07-28
Contact: Ming Sun, Xiaoxun Ma
Supported by:
This work was financed by the projects of the National Natural Science Foundation of China (21776229, 21908180, 22078266), the National Key Research & Development Program of China (2018YFB0604603), the Key Research and Development Program of Shaanxi (2020ZDLGY11-02, 2018ZDXM-GY-167).

Selective preparation of light aromatic hydrocarbons from catalytic fast pyrolysis vapors of coal tar asphaltene over transition metal ion modified zeolites

Yongqi Liu, Qiuxiang Yao, Ming Sun, Xiaoxun Ma

School of Chemical Engineering, Northwest University, International Science & Technology Cooperation Base of MOST for Clean Utilization of Hydrocarbon Resources, Chemical Engineering Research Center of the Ministry of Education for Advanced Use Technology of Shanbei Energy, Shaanxi Research Center of Engineering Technology for Clean Coal Conversion, Collaborative Innovation Center for Development of Energy and Chemical Industry in Northern Shaanxi, Xi'an 710069, China

通讯作者: Ming Sun, Xiaoxun Ma
基金资助:
This work was financed by the projects of the National Natural Science Foundation of China (21776229, 21908180, 22078266), the National Key Research & Development Program of China (2018YFB0604603), the Key Research and Development Program of Shaanxi (2020ZDLGY11-02, 2018ZDXM-GY-167).

Abstract

Abstract: The catalytic cracking of coal tar asphaltene (CTA) pyrolysis vapors was carried out over transition metalion modified zeolites to promote the generation of light aromatic hydrocarbons (L-ArHs) in a pyrolysis-gas chromatography/mass spectrometry (Py-GC/MS) micro-reactor system. The effects of ultra stable Y (USY), Co/USY and Mo/USY on the selectivity and yield of L-ArHs products and the extent of deoxygenation (E_{deoxygenation}), lightweight (E_lightweight) from CTA pyrolysis volatiles were investigated. Results showed that the yields of L-ArHs are mainly controlled by the acid sites and specific surface area of the catalysts, while the deoxygenation effect is determined by theirs pore size. The E_lightweight of CTA pyrolysis volatiles over USY is 9.65%, while the E_{deoxygenation} of CTA pyrolysis volatiles over Mo/USY reaches 20.85%. Additionally, the modified zeolites (Mo/USY and Co/USY) exhibit better performance than USY on L-ArHs production, owing to the synergistic effect of metal ions (Mo, Co) and acid sites of USY. Compared with the non-catalytic fast pyrolysis of CTA, the total yield of L-ArHs obtained over USY (4032 mg·kg^-1), Co/USY (4363 mg·kg^-1) and Mo/USY (4953 mg·kg^-1) were increased by 27.03%, 38.19% and 54.78%, respectively. Furthermore, the possible catalytic conversion mechanism of transition metal ion (Co and Mo) modified zeolites was proposed based on the distribution of products and the characterizations of catalysts.

Key words: Coal tar asphaltene, Transition metal ion modification, Deoxygenation, Lightweight, Light aromatic compounds

摘要： The catalytic cracking of coal tar asphaltene (CTA) pyrolysis vapors was carried out over transition metalion modified zeolites to promote the generation of light aromatic hydrocarbons (L-ArHs) in a pyrolysis-gas chromatography/mass spectrometry (Py-GC/MS) micro-reactor system. The effects of ultra stable Y (USY), Co/USY and Mo/USY on the selectivity and yield of L-ArHs products and the extent of deoxygenation (E_{deoxygenation}), lightweight (E_lightweight) from CTA pyrolysis volatiles were investigated. Results showed that the yields of L-ArHs are mainly controlled by the acid sites and specific surface area of the catalysts, while the deoxygenation effect is determined by theirs pore size. The E_lightweight of CTA pyrolysis volatiles over USY is 9.65%, while the E_{deoxygenation} of CTA pyrolysis volatiles over Mo/USY reaches 20.85%. Additionally, the modified zeolites (Mo/USY and Co/USY) exhibit better performance than USY on L-ArHs production, owing to the synergistic effect of metal ions (Mo, Co) and acid sites of USY. Compared with the non-catalytic fast pyrolysis of CTA, the total yield of L-ArHs obtained over USY (4032 mg·kg^-1), Co/USY (4363 mg·kg^-1) and Mo/USY (4953 mg·kg^-1) were increased by 27.03%, 38.19% and 54.78%, respectively. Furthermore, the possible catalytic conversion mechanism of transition metal ion (Co and Mo) modified zeolites was proposed based on the distribution of products and the characterizations of catalysts.

关键词: Coal tar asphaltene, Transition metal ion modification, Deoxygenation, Lightweight, Light aromatic compounds

Yongqi Liu, Qiuxiang Yao, Ming Sun, Xiaoxun Ma. Selective preparation of light aromatic hydrocarbons from catalytic fast pyrolysis vapors of coal tar asphaltene over transition metal ion modified zeolites[J]. Chinese Journal of Chemical Engineering, 2021, 35(7): 275-287.

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Selective preparation of light aromatic hydrocarbons from catalytic fast pyrolysis vapors of coal tar asphaltene over transition metal ion modified zeolites

Selective preparation of light aromatic hydrocarbons from catalytic fast pyrolysis vapors of coal tar asphaltene over transition metal ion modified zeolites

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