Tailoring of Hydrotalcite-Derived Cu-Based Catalysts for CO2 Hydrogenation to Methanol

被引:20
作者
Frusteri, Leone [1 ]
Cannilla, Catia [2 ]
Todaro, Serena [3 ]
Frusteri, Francesco [2 ]
Bonura, Giuseppe [2 ]
机构
[1] Univ Messina, Dip Ingn Elettron Chim & Ingn Ind, Contrada Dio 1, I-98166 Messina, Italy
[2] CNR ITAE, Ist Tecnol Avanzate Energia Nicola Giordano, Via S Lucia Contesse 5, I-98126 Messina, Italy
[3] Univ Calabria, Dip Ingn Ambiente Terr & Ingn Chim, Via P Bucci, I-87036 Arcavacata Di Rende, Italy
关键词
CO2; hydrogenation; methanol synthesis; hydrotalcite; copper catalysts; CU/ZNO CATALYSTS; ZNO; PERFORMANCE; PRECURSORS; CONVERSION; ZR; GA; AL;
D O I
10.3390/catal9121058
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
Ternary CuxZnyAlz catalysts were prepared using the hydrotalcite (HT) method. The influence of the atomic x:y:z ratio on the physico-chemical and catalytic properties under CO2 hydrogenation conditions was probed. The characterization data of the investigated catalysts were obtained by XRF, XRD, BET, TPR, CO2-TPD, N2O chemisorption, SEM, and TEM techniques. In the "dried" catalyst, the typical structure of a hydrotalcite phase was observed. Although the calcination and subsequent reduction treatments determined a clear loss of the hydrotalcite structure, the pristine phase addressed the achievement of peculiar physico-chemical properties, also affecting the catalytic activity. Textural and surface effects induced by the zinc concentration conferred a very interesting catalyst performance, with a methanol space time yield (STY) higher than that of commercial systems operated under the same experimental conditions. The peculiar behavior of the hydrotalcite-like samples was related to a high dispersion of the active phase, with metallic copper sites homogeneously distributed among the oxide species, thereby ensuring a suitable activation of H-2 and CO2 reactants for a superior methanol production.
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页数:15
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共 30 条
[1]   Methanol synthesis from CO2 hydrogenation over copper based catalysts [J].
Ahouari, Hania ;
Soualah, Ahcene ;
Le Valant, Anthony ;
Pinard, Ludovic ;
Magnoux, Patrick ;
Pouilloux, Yannick .
REACTION KINETICS MECHANISMS AND CATALYSIS, 2013, 110 (01) :131-145
[2]   Effects of oxide carriers on surface functionality and process performance of the Cu-ZnO system in the synthesis of methanol via CO2 hydrogenation [J].
Arena, Francesco ;
Mezzatesta, Giovanni ;
Zafarana, Giovanni ;
Trunfio, Giuseppe ;
Frusteri, Francesco ;
Spadaro, Lorenzo .
JOURNAL OF CATALYSIS, 2013, 300 :141-151
[3]   Correlations between synthesis, precursor, and catalyst structure and activity of a large set of CuO/ZnO/Al2O3 catalysts for methanol synthesis [J].
Baltes, C. ;
Vukojevic, S. ;
Schueth, F. .
JOURNAL OF CATALYSIS, 2008, 258 (02) :334-344
[4]   Significant Advances in C1 Catalysis: Highly Efficient Catalysts and Catalytic Reactions [J].
Bao, Jun ;
Yang, Guohui ;
Yoneyama, Yoshiharu ;
Tsubaki, Noritatsu .
ACS CATALYSIS, 2019, 9 (04) :3026-3053
[5]   Heterogeneous Catalysis of CO2 Conversion to Methanol on Copper Surfaces [J].
Behrens, Malte .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2014, 53 (45) :12022-12024
[6]   Knowledge-based development of a nitrate-free synthesis route for Cu/ZnO methanol synthesis catalysts via formate precursors [J].
Behrens, Malte ;
Kissner, Stefan ;
Girsgdies, Frank ;
Kasatkin, Igor ;
Hermerschmidt, Felix ;
Mette, Katharina ;
Ruland, Holger ;
Muhler, Martin ;
Schloegl, Robert .
CHEMICAL COMMUNICATIONS, 2011, 47 (06) :1701-1703
[7]   Meso- and nano-structuring of industrial Cu/ZnO/(Al2O3) catalysts [J].
Behrens, Malte .
JOURNAL OF CATALYSIS, 2009, 267 (01) :24-29
[8]   Structure control on kinetics of copper reduction in Zr-containing mixed oxides during catalytic hydrogenation of carbon oxides to methanol [J].
Bonura, G. ;
Khassin, A. A. ;
Yurieva, T. M. ;
Cannilla, C. ;
Frusteri, F. ;
Frusteri, L. .
CATALYSIS TODAY, 2020, 342 :39-45
[9]   The changing nature of the active site of Cu-Zn-Zr catalysts for the CO2 hydrogenation reaction to methanol [J].
Bonura, G. ;
Cordaro, M. ;
Cannilla, C. ;
Arena, F. ;
Frusteri, F. .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2014, 152 :152-161
[10]   CO2 Recycling to Dimethyl Ether: State-of-the-Art and Perspectives [J].
Catizzone, Enrico ;
Bonura, Giuseppe ;
Migliori, Massimo ;
Frusteri, Francesco ;
Giordano, Girolamo .
MOLECULES, 2018, 23 (01)