Acid-Base Promoted Dehydrogenation Coupling of Ethanol on Supported Ag Particles

被引：37

作者：

Zhang, Jian ^{[1
,2
]}

Shi, Kai ^{[1
,2
]}

An, Zhe ^{[1
,2
]}

Zhu, Yanru ^{[1
,2
]}

Shu, Xin ^{[1
,2
]}

Song, Hongyan ^{[1
,2
]}

Xiang, Xu ^{[1
,2
]}

He, Jing ^{[1
,2
]}

机构：

[1] Beijing Univ Chem Technol, State Key Lab Chem Resource Engn, Beijing 100029, Peoples R China

[2] Beijing Univ Chem Technol, Beijing Adv Innovat Ctr Soft Matter Sci & Engn, Beijing 100029, Peoples R China

来源：

INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH | 2020年 / 59卷 / 08期

基金：

国家重点研发计划;

关键词：

OXIDANT-FREE DEHYDROGENATION; N-BUTANOL; CATALYTIC CONVERSION; SELECTIVE SYNTHESIS; TRANSITION-METAL; ALCOHOLS; CONDENSATION; 1-BUTANOL; SITES; MG;

D O I：

10.1021/acs.iecr.9b06778

中图分类号：

TQ [化学工业];

学科分类号：

0817 ;

摘要：

Dehydrogenation coupling of ethanol to n-butanol has received much attention due to the wide application of n-butanol. Highly selective butanol production from ethanol remains a challenge due to competitive reactions in the dehydrogenation and/or condensation and great difficulty in ethanol dehydrogenation. This work reports a synergistic catalysis between layered double hydroxide (LDO), an acidic-basic support, and supported Ag particles for the dehydrogenation coupling of ethanol to n-butanol. A selectivity of up to 77% toward n-butanol with an ethanol conversion of 23.2%, among impressive levels reported till now, has been achieved at 350 degrees C, 0.1 MPa. A selectivity of up to 60% toward n-butanol with an ethanol conversion of 45%, the highest selectivity at an ethanol conversion of >45% reported till now, has been achieved at 250 degrees C, 2 MPa. A synergistic catalysis between the acid-base sites of the LDO surface and supported Ag particles have been revealed to contribute the excellent butanol selectivity: basic sites promote adsorption and subsequent dehydrogenation of ethanol on Ag particles; in addition to the promotion from Ag, the following aldol condensation is boosted by acid-base cooperation.

引用

页码：3342 / 3350

页数：9

共 66 条

[1] Homogeneous Ethanol to Butanol Catalysis-Guerbet Renewed [J].

Aitchison, Hope ;

Wingad, Richard L. ;

Wass, Duncan F. .

ACS CATALYSIS, 2016, 6 (10) :7125-7132

[2] Ex Situ and Operando Studies on the Role of Copper in Cu-Promoted SiO2-MgO Catalysts for the Lebedev Ethanol-to-Butadiene Process [J].

Angelici, Carlo ;

Meirer, Florian ;

van der Eerden, Ad M. J. ;

Schaink, Herrick L. ;

Goryachev, Andrey ;

Hofmann, Jan P. ;

Hensen, Emiel J. M. ;

Weckhuysen, Bert M. ;

Bruijnincx, Pieter C. A. .

ACS CATALYSIS, 2015, 5 (10) :6005-6015

[3]

[Anonymous], 1957, GB, Patent No. [GB815566A, 815566]

[4] ETHANOL DEHYDRATION ON ALUMINA CATALYSTS .2. INFRARED STUDY ON ADSORPTION OF DIETHYL ETHER OVER ALUMINA [J].

ARAI, H ;

SAITO, Y ;

YONEDA, Y .

JOURNAL OF CATALYSIS, 1968, 10 (02) :128-&

[5] Importance of the Nature of the Active Acid/Base Pairs of Hydroxyapatite Involved in the Catalytic Transformation of Ethanol to n-Butanol Revealed by Operando DRIFTS [J].

Ben Osman, Manel ;

Krafft, Jean-Marc ;

Thomas, Cyril ;

Yoshioka, Tetsuya ;

Kubo, Jun ;

Costentin, Guylene .

CHEMCATCHEM, 2019, 11 (06) :1765-1778

[6] Isotopic transient analysis of the ethanol coupling reaction over magnesia [J].

Birky, Theodore W. ;

Kozlowski, Joseph T. ;

Davis, Robert J. .

JOURNAL OF CATALYSIS, 2013, 298 :130-137

[7] Mg and Al mixed oxides and the synthesis of n-butanol from ethanol [J].

Carvalho, Debora L. ;

de Avillez, Roberto R. ;

Rodrigues, Michelly T. ;

Borges, Luiz E. P. ;

Appel, Lucia G. .

APPLIED CATALYSIS A-GENERAL, 2012, 415 :96-100

[8] HYDROTALCITE-TYPE ANIONIC CLAYS: PREPARATION, PROPERTIES AND APPLICATIONS [J].

Cavani, F. ;

Trifiro, F. ;

Vaccari, A. .

CATALYSIS TODAY, 1991, 11 (02) :173-301

[9] Highly Selective Formation of n-Butanol from Ethanol through the Guerbet Process: A Tandem Catalytic Approach [J].

Chakraborty, Sumit ;

Piszel, Paige E. ;

Hayes, Cassandra E. ;

Baker, R. Tom ;

Jones, William D. .

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 2015, 137 (45) :14264-14267

[10] Promoted Synergic Catalysis between Metal Ni and Acid-Base Sites toward Oxidant-Free Dehydrogenation of Alcohols [J].

Chen, Hao ;

He, Shan ;

Xu, Ming ;

Wei, Min ;

Eyans, David G. ;

Duan, Xue .

ACS CATALYSIS, 2017, 7 (04) :2735-2743

← 1 2 3 4 5 6 7 →