Ethanol to distillate-range molecules using Cu/MgxAlOy catalysts with low Cu loadings

被引：26

作者：

Cuello-Penaloza, Paolo A. ^{[1
]}

Dastidar, Raka G. ^{[1
]}

Wang, Shao-Chun ^{[2
]}

Du, Yi ^{[3
]}

Lanci, Michael P. ^{[3
]}

Wooler, Bradley ^{[3
]}

Kliewer, Christine E. ^{[3
]}

Hermans, Ive ^{[2
]}

Dumesic, James A. ^{[1
]}

Huber, George W. ^{[1
]}

机构：

[1] Univ Wisconsin, Dept Chem & Biol Engn, 1415 Engn Dr, Madison, WI 53706 USA

[2] Univ Wisconsin Madison, Dept Chem, 1101 Univ Ave, Madison, WI 53706 USA

[3] ExxonMobil Res & Engn Co, 3545 Route 22 East Clinton Township, Annandale, NJ 08801 USA

来源：

APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY | 2022年 / 304卷

关键词：

Alcohol coupling reactions; Esterification; Mixed metal oxides; Schultz-Flory distribution; Catalyst stability; SUPERCRITICAL METHANOL DEPOLYMERIZATION; CONDENSATION-REACTIONS; HYDROXYAPATITE CATALYSTS; ETHYL-ACETATE; ALCOHOLS; CONVERSION; BUTANOL; OXIDES; COPPER; SITES;

D O I：

10.1016/j.apcatb.2021.120984

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：

A series of calcined MgAl mixed metal oxide catalysts with low Cu loadings (0.1-1.5 wt%) were tested for ethanol oligomerization to distillate-range molecules. The low Cu loading catalysts (0.1-0.6 wt%) had high selectivity to linear chain C4+ alcohols (49-63% selectivity) and C6+ esters (45-66% of total esters). More specifically, the diesel fuel precursor selectivities were over 75% for low Cu loading catalysts (0.1-0.6 wt%), with a decrease to 49% for a higher Cu loading catalyst (> 1.2 wt% Cu) due to increased ethyl acetate and acetone formation. Alcohol and ester product selectivities follow a Schultz-Flory distribution. Alcohol selectivity was found to vary inversely with BET surface areas of the catalysts, whereas ester selectivity was found to increase with higher base site counts. However, Cu wt% loading was found to have a stronger impact in overall catalyst activity. The catalysts deactivated proportionally to the number of turnovers mainly due to coking, but could be regenerated by calcination.

引用

页数：12

共 45 条

[31] Theoretical insights into the sites and mechanisms for base catalyzed esterification and aldol condensation reactions over Cu [J].

Neurock, Matthew ;

Tao, Zhiyuan ;

Chemburkar, Ashwin ;

Hibbitts, David D. ;

Iglesia, Enrique .

FARADAY DISCUSSIONS, 2017, 197 :59-86

[32] 1-Butanol synthesis from ethanol over strontium phosphate hydroxyapatite catalysts with various Sr/P ratios [J].

Ogo, Shuhei ;

Onda, Ayumu ;

Iwasa, Yukina ;

Hara, Kenji ;

Fukuoka, Atsushi ;

Yanagisawa, Kazumichi .

JOURNAL OF CATALYSIS, 2012, 296 :24-30

[33]

Osakada K, 2014, LECT N CHEM, V85, P169, DOI 10.1007/978-3-662-43539-7_5

[34] Upgrading ethanol to n-butanol over highly dispersed Ni-MgAlO catalysts [J].

Pang, Jifeng ;

Zheng, Mingyuan ;

He, Lei ;

Li, Lin ;

Pan, Xiaoli ;

Wang, Aiqin ;

Wang, Xiaodong ;

Zhang, Tao .

JOURNAL OF CATALYSIS, 2016, 344 :184-193

[35] Ethanol condensation at elevated pressure over copper on AlMgO and AlCaO porous mixed-oxide supports [J].

Petrolini, Davi D. ;

Eagan, Nathaniel ;

Ball, Madelyn R. ;

Burt, Samuel P. ;

Hermans, Ive ;

Huber, George W. ;

Dumesic, James A. ;

Martins, Leandro .

CATALYSIS SCIENCE & TECHNOLOGY, 2019, 9 (08) :2032-2042

[36]

Ramasamy K.K., 2020, Method of converting ethanol to higher alcohols, Patent No. 10745330

[37] Tunable catalytic properties of bi-functional mixed oxides in ethanol conversion to high value compounds [J].

Ramasamy, Karthikeyan K. ;

Gray, Michel ;

Job, Heather ;

Smith, Colin ;

Wang, Yong .

CATALYSIS TODAY, 2016, 269 :82-87

[38] Role of Calcination Temperature on the Hydrotalcite Derived MgO-Al2O3 in Converting Ethanol to Butanol [J].

Ramasamy, Karthikeyan K. ;

Gray, Michel ;

Job, Heather ;

Santosa, Daniel ;

Li, Xiaohong Shari ;

Devaraj, Arun ;

Karkamkar, Abhi ;

Wang, Yong .

TOPICS IN CATALYSIS, 2016, 59 (01) :46-54

[39] Role of the Cu-ZrO2 Interfacial Sites for Conversion of Ethanol to Ethyl Acetate and Synthesis of Methanol from CO2 and H2 [J].

Ro, Insoo ;

Liu, Yifei ;

Ball, Madelyn R. ;

Jackson, David H. K. ;

Chada, Joseph Paul ;

Sener, Canan ;

Kuech, Thomas F. ;

Madon, Rostam J. ;

Huber, George W. ;

Dumesic, James A. .

ACS CATALYSIS, 2016, 6 (10) :7040-7050

[40] Formation of C-C and C-O Bonds and Oxygen Removal in Reactions of Alkanediols, Alkanols, and Alkanals on Copper Catalysts [J].

Sad, Maria E. ;

Neurock, Matthew ;

Iglesia, Enrique .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2011, 133 (50) :20384-20398

← 1 2 3 4 5 →