
浏览全部资源
扫码关注微信
1.上海大学 材料科学与工程学院 上海 201900
2.中国科学院上海应用物理研究所 张江园区 上海 201204
3.中国科学院大连化学物理研究所 清洁能源国家实验室 大连 116023
[ "杨若欧, 男, 1992年出生, 2015年毕业于浙江工业大学, 现为硕士研究生, 材料物理与化学专业", "YANG Ruoou, male, born in 1992, graduated from Zhejiang University of Technology in 2015, master student, major in material physics and chemistry" ]
姜政, E-mail:jiangzheng@sinap.ac.cn JIANG Zheng, E-mail:jiangzheng@sinap.ac.cn
收稿日期:2018-04-03,
修回日期:2018-05-12,
纸质出版日期:2018-10-10
移动端阅览
杨若欧, 孙凡飞, 赵子昂, 等. 费托合成制低碳烯烃中碱金属对CoMn催化剂催化性能的影响[J]. 核技术, 2018,41(10):100102
Ruoou YANG, Fanfei SUN, Ziang ZHAO, et al. Effects of alkalis on the catalytic performance of CoMn catalysts for Fischer-Tropsch to olefin reactions[J]. Nuclear techniques, 2018, 41(10): 100102
杨若欧, 孙凡飞, 赵子昂, 等. 费托合成制低碳烯烃中碱金属对CoMn催化剂催化性能的影响[J]. 核技术, 2018,41(10):100102 DOI: 10.11889/j.0253-3219.2018.hjs.41.100102.
Ruoou YANG, Fanfei SUN, Ziang ZHAO, et al. Effects of alkalis on the catalytic performance of CoMn catalysts for Fischer-Tropsch to olefin reactions[J]. Nuclear techniques, 2018, 41(10): 100102 DOI: 10.11889/j.0253-3219.2018.hjs.41.100102.
碳化钴(Co
2
C)在费托合成制低碳烯烃(Fischer-Tropsch to Olefin,FTO)中起着重要的催化作用。通过X射线衍射(X-ray Diffraction,XRD)、X射线吸收精细结构(X-ray Absorption Fine Structure,XAFS)等表征与方法,对碱金属在CoMn催化FTO中形成碳化钴的影响进行了研究。在钠(Na)、钾(K)元素的影响下,CoMn催化剂在活性评测中,低碳非饱和烃与低碳饱和烃的比例高达17.4与9.4,且仅有较低的甲烷(CH
4
)产生,而锂(Li)对CoMn催化剂的选择性影响较弱。通过XRD表征,发现Na、K对CoMn催化剂形成Co
2
C有很好的促进效果。XAFS揭示了CoMn催化剂的电子结构,催化反应后形成碳化钴的配位结构,为研究CoMn催化剂微观结构提供了基础理论。
Background
2
Cobalt carbide (Co
2
C) has recently been reported to catalyze the Fischer-Tropsch to olefin (FTO) conversion of syngas with high selectivity. However
electronic state and coordination structure of cobalt carbide is limited by its complex reaction.
Purpose
2
This study aims to clarify the effect of alkalis of CoMn catalysts for FTO and understanding the atomic structure of cobalt carbide nanoparticles in the CoMn catalyst.
Methods
2
X-ray absorption fine structure (XAFS) experimental on beamline (BL14W1) of XAFS spectroscopy at the Shanghai Synchrotron Radiation Facility (SSRF) is conducted to explore the electronic state and coordination structure of cobalt carbide with the effects of alkalis.
Results
2
X-ray absorption near-edge structures (XANES) spectra indicts that Na
K acted as electronic donors to cobalt than Li. EXAFS spectra clarified show that the atomic structure of cobalt carbide nanoparticles.
Conclusion
2
The Na
K promoter had benefited the formation of the cobalt carbide in the evolution of the FTO catalysts.
H M T Galvis , K P De Jong . Catalysts for production of lower olefins from synthesis gas:a review . ACS Catalysis , 2013 . 3 ( 9 ): 2130 - 2149 . DOI: 10.1021/cs4003436 http://doi.org/10.1021/cs4003436 .
A Corma , F V Melo , L Sauvanaud , . Light cracked naphtha processing:controlling chemistry for maximum propylene production . Catalysis Today , 2005 . 107-108 699 - 706 . DOI: 10.1016/j.cattod.2005.07.109 http://doi.org/10.1016/j.cattod.2005.07.109 .
Z Yan , Z J Wang , D B Bukur , . Fischer-Tropsch synthesis on a model Co/SiO2 catalyst . Journal of Catalysis , 2009 . 268 ( 2 ): 196 - 200 . DOI: 10.1016/j.jcat.2009.09.015 http://doi.org/10.1016/j.jcat.2009.09.015 .
A C J Koeken , H M T Galvis , T Davidian , . Suppression of carbon deposition in the iron-catalyzed production of lower olefins from synthesis gas . Angewandte Chemie-International Edition , 2012 . 51 ( 29 ): 7190 - 7193 . DOI: 10.1002/anie.201200280 http://doi.org/10.1002/anie.201200280 .
H M T Galvis , J H Bitter , C B Khare , . Supported iron nanoparticles as catalysts for sustainable production of lower olefins . Science , 2012 . 335 ( 6070 ): 835 - 838 . DOI: 10.1126/science.1215614 http://doi.org/10.1126/science.1215614 .
J Xie , J Yang , A I Dugulan , . Size and promoter effects in supported iron Fischer-Tropsch catalysts insights from experiment and theory . ACS Catalysis , 2016 . 6 ( 5 ): 3147 - 3157 . DOI: 10.1021/acscatal.6b00131 http://doi.org/10.1021/acscatal.6b00131 .
Z J Li , L S Zhong , F Yu , . Effects of sodium on the catalytic performance of CoMn catalysts for FischerTropsch to olefin reactions . ACS Catalysis , 2017 . 7 ( 5 ): 3622 - 3631 . DOI: 10.1021/acscatal.6b03478 http://doi.org/10.1021/acscatal.6b03478 .
M Janardanarao . Direct catalytic conversion of synthesis gas to lower olefins . Industrial & Engineering Chemistry Research , 1990 . 29 ( 9 ): 1735 - 1753 . DOI: 10.1021/ie00105a001 http://doi.org/10.1021/ie00105a001 .
F Jiao , J J Li , X L Pan , . Selective conversion of syngas to light olefins . Science , 2016 . 351 ( 6277 ): 1065 - 1068 . DOI: 10.1126/science.aaf1835 http://doi.org/10.1126/science.aaf1835 .
Q H Zhang , J C Kang , Y Wang . Development of novel catalysts for Fischer-Tropsch synthesis:tuning the product selectivity . Chemcatchem , 2010 . 2 ( 9 ): 1030 - 1058 . DOI: 10.1002/cctc.201000071 http://doi.org/10.1002/cctc.201000071 .
J Yang , Y C Sun , Y Tang , . Effect of magnesium promoter on iron-based catalyst for Fischer-Tropsch synthesis . Journal of Molecular Catalysis A-Chemical , 2006 . 245 ( 1-2 ): 26 - 36 . DOI: 10.1016/j.molcata.2005.08.051 http://doi.org/10.1016/j.molcata.2005.08.051 .
H M T Galvis , J H Bitter , T Davidian , . Iron particle size effects for direct production of lower olefins from synthesis gas . Journal of the American Chemical Society , 2012 . 134 ( 39 ): 16207 - 16215 . DOI: 10.1021/ja304958u http://doi.org/10.1021/ja304958u .
L S Zhong , F Yu , Y L An , . Cobalt carbide nanoprisms for direct production of lower olefins from syngas . Nature , 2016 . 538 ( 7623 ): 84 - 87 . DOI: 10.1038/nature19786 http://doi.org/10.1038/nature19786 .
Y P Pei , J X Liu , Y H Zhao , . High alcohols synthesis via Fischer-Tropsch reaction at cobalt metal/carbide interface . ACS Catalysis , 2015 . 5 ( 6 ): 3620 - 3624 . DOI: 10.1021/acscatal.5b00791 http://doi.org/10.1021/acscatal.5b00791 .
Y Z Xiang , N Kruse . Tuning the catalytic CO hydrogenation to straight-and long-chain aldehydes/alcohols and olefins/paraffins . Nature Communications , 2016 . 7 13058 DOI: 10.1038/ncomms13058 http://doi.org/10.1038/ncomms13058 .
Z Zhao , W Lu , R O Yang , . Insight into the formation of Co@Co 2 C catalysts for direct synthesis of higher alcohols and olefins from syngas . ACS Catalysis , 2018 . 8 ( 1 ): 228 - 241 . DOI: 10.1021/acscatal.7b02403 http://doi.org/10.1021/acscatal.7b02403 .
G Kwak , D E Kim , Y T Kim , . Enhanced catalytic activity of cobalt catalysts for Fischer-Tropsch synthesis via carburization and hydrogenation and its application to regeneration . Catalysis Science & Technology , 2016 . 6 ( 12 ): 4594 - 4600 . DOI: 10.1039/C5CY01399B http://doi.org/10.1039/C5CY01399B .
H S Yu , X J Wei , J Li , . The XAFS beamline of SSRF . Nuclear Science and Techniques , 2015 . 26 ( 5 ): 050102 DOI: 10.13538/j.1001-8042/nst.26.050102 http://doi.org/10.13538/j.1001-8042/nst.26.050102 .
M Newville . Ifeffit:interactive XAFS analysis and FEFF fitting . Journal of Synchrotron Radiation , 2001 . 8 322 - 324 . DOI: 10.1107/S0909049500016964 http://doi.org/10.1107/S0909049500016964 .
J C Mohandas , M K Gnanamani , G Jacobs , . Fischer-Tropsch synthesis:characterization and reaction testing of cobalt carbide . ACS Catalysis , 2011 . 1 ( 11 ): 1581 - 1588 . DOI: 10.1021/cs200236q http://doi.org/10.1021/cs200236q .
S Zhang , L J Zhang , H M Li , . Investigation of annealing-induced oxygen vacancies in the Co-doped ZnO system by Co K-edge XANES spectroscopy . Journal of Synchrotron Radiation , 2010 . 17 600 - 605 . DOI: 10.1107/S0909049510020303 http://doi.org/10.1107/S0909049510020303 .
0
浏览量
28
下载量
1
CSCD
关联资源
相关文章
相关作者
相关机构
京公网安备11010802024621