On the effect of Alkaline Earth Metal Cations in the Hydrogenolysis of Glycerol over Pt/C - an Experimental and Theoretical Study

被引：2

作者：

Beine, Anna Katharina ^{[1
]}

Wang, Xinde ^{[2
]}

Vennewald, Maurice ^{[2
]}

Schmidt, Regina U. S. ^{[2
]}

Glotzbach, Christoph ^{[3
]}

Palkovits, Regina ^{[1
,2
]}

Hausoul, Peter J. C. ^{[2
]}

机构：

[1] Max Planck Inst Chem Energy Convers, Grp Solid Mol Catalysts, Striftstr 34-36, D-45470 Mulheim, Germany

[2] Rhein Westfal TH Aachen, Inst Tech & Macromol Chem, Worringerweg 2, D-52074 Aachen, Germany

[3] Thyssenkrupp Ind Solut AG, Friedrich Uhde Str 15, D-44141 Dortmund, Germany

来源：

CHEMCATCHEM | 2022年 / 14卷 / 08期

关键词：

barium; cations; glycerol; hydrogenolysis; Pt/C; SELECTIVE HYDROGENOLYSIS; PROPYLENE-GLYCOL; TUNGSTEN-OXIDE; CATALYSTS; 1,3-PROPANEDIOL; FORMALDEHYDE; BASE;

D O I：

10.1002/cctc.202101940

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：

Glycerol can be converted to propylene glycol via metal and base catalyzed hydrogenolysis. The nature of the base has a profound influence on the outcome of the reaction. We have tested a range of alkaline (LiOH, NaOH and CsOH) and alkaline earth (Mg(OH)(2), Ca(OH)(2), Sr(OH)(2) and Ba(OH)(2)) metal hydroxides in combination with Pt/C. The data reveal that alkaline earth metal hydroxides exhibit a much higher activity and improved selectivity. DFT calculations confirm that the coordination of reactive intermediates to divalent cations is responsible for the observed behavior. In the study, the effect of the cation on hydrogenolysis was elucidated for the first time.

引用

页数：6

共 42 条

[1]

[Anonymous], 1985, HDB CHEM PHYS

[2] Unravelling the Mechanism of Glycerol Hydrogenolysis over Rhodium Catalyst through Combined Experimental-Theoretical Investigations [J].

Auneau, Florian ;

Michel, Carine ;

Delbecq, Francoise ;

Pinel, Catherine ;

Sautet, Philippe .

CHEMISTRY-A EUROPEAN JOURNAL, 2011, 17 (50) :14288-14299

[3] Selective hydrogenolysis of glycerol to 1,2-propanediol on Nb-modified Pd - Zr - Al catalysts [J].

Cai, Fufeng ;

Jin, Feikai ;

Hao, Jie ;

Xiao, Guomin .

CATALYSIS COMMUNICATIONS, 2019, 131

[4] Photocatalytic reforming of aqueous formaldehyde with hydrogen generation over TiO2 nanotubes loaded with Pt or Au nanoparticles [J].

Dalcin Fornari, Ana Maria ;

de Araujo, Mariele Brambilla ;

Duarte, Cesar Bergamin ;

Machado, Giovanna ;

Teixeira, Sergio R. ;

Weibel, Daniel Eduardo .

INTERNATIONAL JOURNAL OF HYDROGEN ENERGY, 2016, 41 (27) :11599-11607

[5] Low-pressure hydrogenolysis of glycerol to propylene glycol [J].

Dasari, MA ;

Kiatsimkul, PP ;

Sutterlin, WR ;

Suppes, GJ .

APPLIED CATALYSIS A-GENERAL, 2005, 281 (1-2) :225-231

[6] The activated complex in chemical reactions [J].

Eyring, H .

JOURNAL OF CHEMICAL PHYSICS, 1935, 3 (02) :107-115

[7] Effect of base additives on the selective hydrogenolysis of glycerol over Ru/TiO2 catalyst [J].

Feng, Jian ;

Wang, Jinbo ;

Zhou, Yafen ;

Fu, Haiyan ;

Chen, Hua ;

Li, Xianjun .

CHEMISTRY LETTERS, 2007, 36 (10) :1274-1275

[8] Hydrogenolysis of glycerol over Pt/C catalyst in combination with alkali metal hydroxides [J].

Feng, Jian ;

Xiong, Wei ;

Ding, Hao ;

He, Bai .

OPEN CHEMISTRY, 2016, 14 (01) :279-286

[9] Hydrogenolysis of glycerol to propanediols over a Pt/ASA catalyst: The role of acid and metal sites on product selectivity and the reaction mechanism [J].

Gandarias, I. ;

Arias, P. L. ;

Requies, J. ;

Guemez, M. B. ;

Fierro, J. L. G. .

APPLIED CATALYSIS B-ENVIRONMENTAL, 2010, 97 (1-2) :248-256

[10] The role of tungsten oxide in the selective hydrogenolysis of glycerol to 1,3-propanediol over Pt/WOx/Al2O3 [J].

Garcia-Fernandez, Sara ;

Gandarias, Inaki ;

Requies, Jesus ;

Soulimani, Fouad ;

Arias, Pedro L. ;

Weckhuysen, Bert M. .

APPLIED CATALYSIS B-ENVIRONMENTAL, 2017, 204 :260-272

← 1 2 3 4 5 →