Selective conversion of syngas to aromatics over metal oxide/HZSM-5 catalyst by matching the activity between CO hydrogenation and aromatization

被引:32
作者
Liu, Chang [1 ,2 ,3 ]
Liu, Su [3 ]
Zhou, Haibo [3 ]
Su, Junjie [3 ]
Jiao, Wenqian [3 ]
Zhang, Lin [3 ]
Wang, Yangdong [3 ]
He, Heyong [1 ,2 ]
Xie, Zaiku [4 ]
机构
[1] Fudan Univ, Dept Chem, Collaborat Innovat Ctr Chem Energy Mat, Shanghai 200433, Peoples R China
[2] Fudan Univ, Shanghai Key Lab Mol Catalysis & Innovat Mat, Collaborat Innovat Ctr Chem Energy Mat, Shanghai 200433, Peoples R China
[3] SINOPEC, Shanghai Res Inst Petrochem Technol, Shanghai 201208, Peoples R China
[4] China Petrochem Corp, SINOPEC Grp, Beijing 100728, Peoples R China
基金
中国国家自然科学基金;
关键词
Aromatics; Bifunctional catalyst; Syngas conversion; Zeolite acidity; Zn modification; GASOLINE-RANGE HYDROCARBONS; SYNTHESIS GAS CONVERSION; BIFUNCTIONAL CATALYST; ZEOLITE; METHANOL; TRANSFORMATION; OXIDES; PERFORMANCE; OXIDATION; OLEFINS;
D O I
10.1016/j.apcata.2019.117206
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Syngas conversion to aromatics has been studied over metal oxide/HZSM-5 bifunctional catalyst. In this reaction, CO is activated on metal oxide and hydrogenated to C-1/C-2 intermediate. The formation of aromatics involves C-C coupling, cycfization and dehydrogenation on acid sites of HZSM-5. The matching between CO hydrogenation and aromatization activity is key to the overall catalytic performance. High aromatic selectivity of up to 82.5% may be achieved over various metal oxide/HZSM-5 catalyst among which Cr2O3/HZSM-5 is the best in activity and aromatic selectivity. The CO activation and hydrogenation over Cr2O3 are facilitated by doping of Zn. The effect of Zn doping is revealed by systematic study on phase, morphology, reducibility and oxygen defect concentration. To enhance CO conversion and to prevent excessive hydrogenation, the strict control of Zn/Cr ratio and the phase of Zn species is required. The activity of HZSM-5 may be altered by changing Si/Al ratio and zeolite/oxide ratio and a moderate acid strength and density is necessary to balance the competition between aromatization and side reactions. Furthermore, the stability of the optimal catalyst 1Zn-3Cr/HZSM-5(18) is demonstrated with no significant deactivation after 100 h on stream.
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页数:9
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