Study on the performance of F-T component modified KCuZrO<sub>2</sub> catalyst for CO hydrogenation to isobutanol

WANG Hui-jun; WU Ying-quan; TIAN Shao-peng; WANG Li-yan; GONG Na-na; XIE Hong-juan; TAN Yi-sheng

Volume 48 Issue 3

Mar. 2020

Turn off MathJax

Article Contents

Article Navigation > Journal of Fuel Chemistry and Technology > 2020 > 48(3): 302-310

WANG Hui-jun, WU Ying-quan, TIAN Shao-peng, WANG Li-yan, GONG Na-na, XIE Hong-juan, TAN Yi-sheng. Study on the performance of F-T component modified KCuZrO2 catalyst for CO hydrogenation to isobutanol[J]. Journal of Fuel Chemistry and Technology, 2020, 48(3): 302-310.

Citation:

WANG Hui-jun, WU Ying-quan, TIAN Shao-peng, WANG Li-yan, GONG Na-na, XIE Hong-juan, TAN Yi-sheng. Study on the performance of F-T component modified KCuZrO₂ catalyst for CO hydrogenation to isobutanol[J]. Journal of Fuel Chemistry and Technology, 2020, 48(3): 302-310.

Citation:

PDF( 4721 KB)

Study on the performance of F-T component modified KCuZrO₂ catalyst for CO hydrogenation to isobutanol

WANG Hui-jun^{1, 2},
WU Ying-quan^{1
,
,},
TIAN Shao-peng³,
WANG Li-yan^{1, 2},
GONG Na-na^{1, 2},
XIE Hong-juan¹,
TAN Yi-sheng^{1
,
,}

1.
State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, China
2.
University of Chinese Academy of Sciences, Beijing 100049, China
3.
School of Science Xijing University, Xi'an 710000, China

Funds:

The project was supported by the National Natural Science Foundation of China 21573269

The project was supported by the National Natural Science Foundation of China 21706218

More Information

Corresponding author: WU Ying-qaun, E-mail: wvyq@sxicc.ac.cn; TAN Yi-sheng, E-mail: tan@sxicc.ac.cn
Received Date: 2020-01-21
Rev Recd Date: 2020-03-03

Available Online: 2021-01-23

Publish Date: 2020-03-10

Abstract

Abstract

KCuZrO₂ catalysts modified with different F-T elements (Fe, Co, Ni) were prepared by co-precipitation method and then were tested for isobutanol synthesis from catalytic CO hydrogenation. The catalysts were characterized by N₂ adsorption and desorption experiments (BET), XRD, TEM, XPS, H₂-TPR, CO-TPD and in situ DRIFTS. The results showed that the addition of F-T components promoted the formation of ethanol and propanol, and had different effects on the selectivity of isobutanol. The characterization results showed that Fe promoted the dispersion of catalyst components, and enriched the active component Cu on the catalyst surface, which improved the active adsorption of H₂ and CO. In addition, more C₁ species were formed on the KFeCuZrO₂ catalyst surface, and these C₁ species could further react with ethanol and propanol to produce isobutanol. However, the catalysts modified by Co and Ni lacked sufficient C₁ species, so the selectivity of isobutanol did not increase significantly. The introduction of Co had little effect on the structure of catalyst and the dispersion of Cu, but the activity of catalyst decreased after Co addition, which might be due to the deactivation of catalyst. After adding Ni to the catalyst, the specific surface area decreased and the particle size increased, and the Cu/Zr molar ratio on the catalyst surface also decreased to 0.19. The interaction between Cu-Zr was weakened, and the isobutanol selectivity was also reduced.
- CO hydrogenation,
- F-T elements,
- Cu/ZrO₂,
- isobutanol

FullText(HTML)

References(35)

References

[1]	李明阳.合成气制异丁醇的催化剂研究[D].上海: 华东理工大学, 2015. LI Ming-yang. Study on the catalyst for isobutanol synthesis from syngas[D]. Shanghai: East China University of Science and Technology, 2015.
[2]	SLATING T A, KESAN J P. Making regulator innovation keep pace with technological innovation[J]. Wis Law Rev, 2011, 1109-1179. http://papers.ssrn.com/sol3/papers.cfm?abstract_id=1805008
[3]	田宇, 王义强, 王启业.异丁醇生物合成的研究进展[J].生物技术通报, 2013, 1(5):40-44. http://d.old.wanfangdata.com.cn/Periodical/swjstb201305007 TIAN Yu, WANG Yi-qiang, WANG Qi-ye. Research progress of isobutanol biosynthesis[J]. Biotechnol Bull, 2013, 1(5):40-44. http://d.old.wanfangdata.com.cn/Periodical/swjstb201305007
[4]	寇永利, 解红娟, 刘广波, 张欣悦, 韩怡卓, Noritatsu Tsubaki, 谭猗生. ZnCr基催化剂煅烧温度对异丁醇合成性能的影响[J].燃料化学学报, 2013, 41(6):703-709. http://www.ccspublishing.org.cn/article/id/100032923 KOU Yong-li, XIE Hong-juan, LIU Guang-bo, ZHANG Xin-yue, HAN Yi-zhuo, NORITATSU Tsubaki, TAN Yi-sheng. Effect of calcination temperature on the performance of ZnCr based catalyst in isobutanol synthesis[J]. J Fuel Chem Technol, 2013, 41(6):703-709. http://www.ccspublishing.org.cn/article/id/100032923
[5]	GAO X F, WU Y Q, ZHANG T, WANG L Y, LI X L, TAN Y S. Binary ZnO/Zn-Cr nanospinel catalysts prepared by a hydrothermal method for isobutanol synthesis from syngas[J]. Cat Sci Technol, 2018, 8:2975-2986. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=226b723dcf76346db9b42eba5a2c714b
[6]	KOU J W, CHENG S Y, GAO Z H, CHENG F Q, HUANG W. Synergistic effects of potassium promoter and carbon fibers on direct synthesis of isobutanol from syngas over Cu/ZnO/Al₂O₃ catalysts obtained from hydrotalcite-like compounds[J]. Solid State Sci, 2019, 87:138-145. doi: 10.1016/j.solidstatesciences.2018.11.007
[7]	谭理, 武应全, 张涛, 解红娟, 陈建刚.沉淀温度对K-CuLaZrO₂催化剂上合成气直接合成异丁醇的影响[J].燃料化学学报, 2019, 47(9):1096-1102. http://www.ccspublishing.org.cn/article/id/2fda3d52-f899-42f6-bc1f-9e4ac30af8a9 TAN Li, WU Ying-quan, ZHANG Tao, XIE Hong-juan, CHEN Jian-gang. Effect of precipitation temperature on the performance of K-CuLaZrO₂ catalyst for isobutanol synthesis from syngas[J]. J Fuel Chem Technol, 2019, 47(9):1096-1102. http://www.ccspublishing.org.cn/article/id/2fda3d52-f899-42f6-bc1f-9e4ac30af8a9
[8]	何代平.二氧化锆基催化剂上合成低碳醇和酮的研究[D].北京: 中国科学院大学, 2004. HE Dai-ping. Higher alcohol and ketone synthesis study on ZrO₂-based catalysts[D]. Beijing: University of Chinese Academy of Science, 2004.
[9]	ARTYUKH Y N, LUNEY N K, VERKHGRADSKII O P, ZELENKOV G A, OEVA L A, LIMOVICH E A. Effect of the introduction of certain additives to the CO+H₂ mixture and the scheme for the formation of alcohols higher than C₁[J]. Theor Exp Chem, 1990, 26:476-479. doi: 10.1007/BF00530266
[10]	BERETTA A, LIETTI L, TRONCONI E, FORZATTI P, PASQUON I. Development of a mechanistic kinetic model of the higher alcohol synthesis over a Cs-doped Zn/Cr/O catalyst 2. Analysis of chemical enrichment experiments[J]. Ind Eng Chem Res, 1996, 35:2154-2160. http://cn.bing.com/academic/profile?id=1e02bcc2e1fa846d77613980e5ce6f37&encoded=0&v=paper_preview&mkt=zh-cn
[11]	WU Y Q, XIE H J, KOU Y L, NORITASTU T, HAN Y Z, TAN Y S. The mechanism of higher alcohol formation on ZrO₂-based catalyst from syngas[J]. Korean J Chem Eng, 2015, 32:406-412. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=09529b8232223a919a67b18e74c6f8cb
[12]	XU X, DOESBURG E B M, SCHOLTEN J J F. Synthesis of higher alcohols from syngas recent patented catalysts and tentative on the mechanism[J]. Catal Today, 1987, 2:125-170. doi: 10.1016/0920-5861(87)80002-0
[13]	AO M, PHAM G H, SUNARSO J, TADE M O, LIU S. Active centers of catalysts for higher alcohol synthesis from syngas:A review[J]. ACS Catal, 2018, 8:7025-7050. http://cn.bing.com/academic/profile?id=05159d839423c235a4a24f794f0c8f0d&encoded=0&v=paper_preview&mkt=zh-cn
[14]	LUK H T, MONDELI C, FERRE D C, STEWART J A, PEREZ-RAMIREZ J. Status and prospects in higher alcohols synthesis from syngas[J]. Chem Soc Rev, 2017, 46:1358-1426. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=cb9b83963a9d190538889e1e6504dd9f
[15]	WANG P, CHEN S Y, BAI Y X, GAO X F, LI X L, SUN K, XIE H J, YANG G H, HAN Y Z, TAN Y S. Effect of the promoter and support on cobalt-based catalysts for higher alcohols synthesis through CO hydrogenation[J]. Fuel, 2017, 195:69-81. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=8e0383f680d04082ad7dbc676b216ca4
[16]	SPIVEY J J, EGBEBI A. Heterogeneous catalytic synthesis of ethanol from biomass-derived syngas[J]. Chem Soc Rev, 2007, 36:1514-1528. http://cn.bing.com/academic/profile?id=7ef6fbd5fc9f8ff0c4a525e4bed428ed&encoded=0&v=paper_preview&mkt=zh-cn
[17]	XIAO K, BAO Z, QI X, WANG X, ZHONG L, FANG K, LIN M, SUN Y. Advances in bifunctional catalysis for higher alcohol synthesis from syngas[J]. Chin J Catal, 2013, 34:116-129. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=cuihuaxb201301010
[18]	XIAO K, QI X, BAO Z, WANG X, ZHONG L, FANG K, LIN M, SUN Y. CuFe, CuCo and CuNi nanoparticles as catalysts for higher alcohol synthesis from syngas:a comparative study[J]. Catal Sci Technol, 2013, 3:1591-1602. http://cn.bing.com/academic/profile?id=f9e7c76f3ed9ed8a0f2ffb8293ec622c&encoded=0&v=paper_preview&mkt=zh-cn
[19]	SUN X, YU Y, ZHANG M. Insight into the effect of promoter Co on C₂ oxygenate formation from syngas on CoCu(100) and Cu(100):a comparative DFT study[J]. Appl Surf Sci, 2018, 434:28-39. doi: 10.1016/j.apsusc.2017.10.164
[20]	AO M, PHAM G H, SAGE V, PAREEK V. Selectivity enhancement for higher alcohols synthesis product in Fischer-Tropsch synthesis over nickel-substituted La_0.9Sr_0.1CoO₃ perovskite catalysts[J]. Fuel, 2017, 206:390-400. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=7dd22d52b5bd2d0ca3cc88393c35ed59
[21]	AO M, PHAM G H, SAGE V, PAREEK V, LIU S M. Perovskite-derived trimetallic Co-Ni-Cu catalyst for higher alcohol synthesis from syngas[J]. Fuel Process Technol, 2019, 193:141-148. http://cn.bing.com/academic/profile?id=eeed1464c5ec4e18522192fbdf918ac1&encoded=0&v=paper_preview&mkt=zh-cn
[22]	陈小平. F-T合成组元改性Cu/Mn/ZrO₂甲醇催化剂用于低碳醇合成的研究[D].北京: 中国科学院大学, 1999. CHEN Xiao-ping. Study on F-T element modified Cu/Mn/ZrO₂ methanol catalysts for higher alcohol synthesis[D]. Beijing: University of Chinese Academy of Science, 1999.
[23]	XU R, YANG C, WEI W, LI W H, SUN Y H, HU T D. Influence of promoter on catalytic properties of Cu-Mn-Fe/ZrO₂ catalysts for alcohols synthesis[J]. React Kinet Catal Lett, 2004, 81:91-98. https://www.researchgate.net/publication/229307965_Fe-modified_CuMnZrO2_catalysts_for_higher_alcohols_synthesis_from_syngas
[24]	LI W Z, HUANG H, LI H J, ZHANG W, LIU H C. Facile synthesis of pure monoclinic and tetragonal zirconia nanoparticles and their phase effects on the behavior of supported molybdena catalysts for methanol-selective oxidation[J]. Langmuir, 2008, 24:8358-8366. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=cee0b513bef781546d5210b8717e74d8
[25]	LI G R, LI W, ZHANG M H, TAO K Y. Characterization and catalytic application of homogeneous nano-composite oxides ZrO₂-Al₂O₃[J]. Catal Today, 2004, 93(5):95-601. doi: 10.1016/j.cattod.2004.06.010
[26]	SUN K, WU Y Q, TAN M H, WANG L Y, YANG G H, ZHANG M, ZHANG W, TAN YS. Ethanol and higher alcohols synthesis from syngas over CuCoM (M=Fe, Cr, Ga and Al) nanoplates derived from hydrotalcite-like precursors[J]. ChemCatChem, 2019, 11:2695-2706. doi: 10.1002/cctc.201900096
[27]	AVGOUROPOULOS G, IOANNIDES T, MATRALIS H. Influence of the preparation method on the performance of CuO-CeO₂ catalysts for the selective oxidation of CO[J]. Appl Catal B:Environ, 2005, 56:87-93. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=3887d474fb479182a25d534d11f5c3ba
[28]	WU Y Q, XIE H J, TIAN S P, NORITATSU T, HAN Y Z, TAN Y S. Isobutanol synthesis from syngas over K-Cu/ZrO₂-La₂O₃(x) catalysts:Effect of La-loading[J]. J Mol Catal A:Chem, 2015, 396:254-260. doi: 10.1016/j.molcata.2014.10.003
[29]	YU Q, YAO X J, ZHANG H L, GAO F, DONG L. Effect of ZrO₂ addition method on the activity of Al₂O₃-supported CuO for NO reduction with CO:Impregnation vs. co-precipitation[J]. Appl Catal A:Gen, 2012, 423/424:42-51. doi: 10.1016/j.apcata.2012.02.017
[30]	RIBEIRO N F P, SOUZA M M V M, SCHMAL M. Combustion synthesis of copper catalysts for selective CO oxidation[J]. J Power Sources, 2008, 179:329-330. doi: 10.1016/j.jpowsour.2007.12.096
[31]	WU Y Q, WANG S C, XIE H J, GAO J W, TIAN S P, HAN Y Z, TAN Y S. Influence of Cu on the K-LaZrO₂ Catalyst for Isobutanol Synthesis[J]. Acta Phys Chim Sin, 2015, 31(1):166-172. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=wlhxxb201501027
[32]	JUNG K T, BELL A T. An in situ infrared study of dimethyl carbonate synthesis from carbon dioxide and methanol over zirconia[J]. J Catal, 2001, 204:339-347. http://www.wanfangdata.com.cn/details/detail.do?_type=perio&id=7474d7a365d9e184f2579bb6375b8233
[33]	POKROVSKI K, JUNG K T, BELL A T. Investigation of CO and CO₂ adsorption on tetragonal and monoclinic zirconia[J]. Langmuir, 2001, 17:4297-4300. doi: 10.1016/j.jpowsour.2007.12.096
[34]	SANTOS V P, VANDER L B, CHOJECKI A, BUDRONI G, CORTHALS S, SHIBATA H, MEIMA G R, KAPTEIJIN F, MAKKEE M, GASCON J. Mechanistic insight into the synthesis of higher alcohols from syngas:The role of K promotion on MoS₂ catalysts[J]. ACS Catal. 2013, 3:1634-1637. doi: 10.1021/cs4003518
[35]	WU Y Q, GONG N N, ZHANG M, ZHANG W, ZHANG T, ZHANG J F, WANG L Y, XIE H J, TAN Y S. Insight into the branched alcohol formation mechanism on K-ZnCr catalysts from syngas[J]. Catal Sci Technol, 2019, 9(10):2592-2600. doi: 10.1039/C9CY00542K