Selective conversion of syngas to light olefins

被引:1334
作者
Jiao, Feng [1 ]
Li, Jinjing [1 ]
Pan, Xiulian [1 ]
Xiao, Jianping [1 ]
Li, Haobo [1 ]
Ma, Hao [1 ]
Wei, Mingming [1 ]
Pan, Yang [2 ]
Zhou, Zhongyue [2 ]
Li, Mingrun [1 ]
Miao, Shu [1 ]
Li, Jian [1 ]
Zhu, Yifeng [1 ]
Xiao, Dong [1 ]
He, Ting [1 ]
Yang, Junhao [1 ]
Qi, Fei [2 ]
Fu, Qiang [1 ]
Bao, Xinhe [1 ]
机构
[1] Chinese Acad Sci, Dalian Inst Chem Phys, Collaborat Innovat Ctr Chem Energy Mat 2011, State Key Lab Catalysis, Zhongshan Rd 457, Dalian 116023, Peoples R China
[2] Univ Sci & Technol China, Natl Synchrotron Radiat Lab, Hefei 230029, Peoples R China
基金
中国国家自然科学基金;
关键词
PHOTOIONIZATION MASS-SPECTROMETRY; SYNTHESIS GAS; CO HYDROGENATION; CATALYSTS; KETENE; TRANSFORMATION; NANOPARTICLES; HYDROCARBONS; CHEMISTRY;
D O I
10.1126/science.aaf1835
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
Although considerable progress has been made in direct synthesis gas (syngas) conversion to light olefins (C-2(=)-C-4(=)) via Fischer-Tropsch synthesis (FTS), the wide product distribution remains a challenge, with a theoretical limit of only 58% for C-2-C-4 hydrocarbons. We present a process that reaches C-2(=)-C-4(=) selectivity as high as 80% and C-2-C-4 94% at carbon monoxide (CO) conversion of 17%. This is enabled by a bifunctional catalyst affording two types of active sites with complementary properties. The partially reduced oxide surface (ZnCrOx) activates CO and H-2, and C-C coupling is subsequently manipulated within the confined acidic pores of zeolites. No obvious deactivation is observed within 110 hours. Furthermore, this composite catalyst and the process may allow use of coal-and biomass-derived syngas with a low H-2/CO ratio.
引用
收藏
页码:1065 / 1068
页数:4
相关论文
共 26 条
[1]   REACTIONS OF FREE METHYLENE - PHOTOLYSIS OF KETENE IN PRESENCE OF OTHER GASES [J].
CHANMUGAM, J ;
BURTON, M .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1956, 78 (03) :509-519
[2]   A methanol to olefins review: Diffusion, coke formation and deactivation SAPO type catalysts [J].
Chen, D. ;
Moljord, K. ;
Holmen, A. .
MICROPOROUS AND MESOPOROUS MATERIALS, 2012, 164 :239-250
[3]  
Chen XQ, 2015, CHEM COMMUN, V51, P217, DOI [10.3778/j.issn.1002-8331.1401-0315, 10.1039/c4cc06600f]
[4]   Selective detection of isomers with photoionization mass spectrometry for studies of hydrocarbon flame chemistry [J].
Cool, TA ;
Nakajima, K ;
Mostefaoui, TA ;
Qi, F ;
McIlroy, A ;
Westmoreland, PR ;
Law, ME ;
Poisson, L ;
Peterka, DS ;
Ahmed, M .
JOURNAL OF CHEMICAL PHYSICS, 2003, 119 (16) :8356-8365
[5]   Study of physical mixtures of Cr2O3-ZnO and ZSM-5 catalysts for the transformation of syngas into liquid hydrocarbons [J].
Erena, J ;
Arandes, JM ;
Bilbao, J ;
Aguayo, AT ;
de Lasa, HI .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 1998, 37 (04) :1211-1219
[6]   COMPOSITION OF SYNTHETIC LIQUID FUELS .1. PRODUCT DISTRIBUTION AND ANALYSIS OF C5-C8 PARAFFIN ISOMERS FROM COBALT CATALYST [J].
FRIEDEL, RA ;
ANDERSON, RB .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1950, 72 (03) :1212-1215
[7]   SYNTHESIS GAS CONVERSION UTILIZING MIXED CATALYST COMPOSED OF CO REDUCING CATALYST AND SOLID ACID .4. SELECTIVE SYNTHESIS OF C2, C-3, AND C-4 PARAFFINS FROM SYNTHESIS GAS [J].
FUJIMOTO, K ;
SAIMA, H ;
TOMINAGA, HO .
JOURNAL OF CATALYSIS, 1985, 94 (01) :16-23
[8]   Catalysts for Production of Lower Olefins from Synthesis Gas: A Review [J].
Galvis, Hirsa M. Torres ;
de Jong, Krijn P. .
ACS CATALYSIS, 2013, 3 (09) :2130-2149
[9]   Supported Iron Nanoparticles as Catalysts for Sustainable Production of Lower Olefins [J].
Galvis, Hirsa M. Torres ;
Bitter, Johannes H. ;
Khare, Chaitanya B. ;
Ruitenbeek, Matthijs ;
Dugulan, A. Iulian ;
de Jong, Krijn P. .
SCIENCE, 2012, 335 (6070) :835-838
[10]   Direct synthesis of LPG from synthesis gas over Pd-Zn-Cr/Pd-β hybrid catalysts [J].
Ge, Qingjie ;
Li, Xiaohong ;
Kaneko, Hiroshi ;
Fujimoto, Kaoru .
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 2007, 278 (1-2) :215-219