Porosity and Structure of Hierarchically Porous Ni/Al2O3 Catalysts for CO2 Methanation

被引：29

作者：

Weber, Sebastian ^{[1
,2
]}

Abel, Ken L. ^{[3
]}

Zimmermann, Ronny T. ^{[4
]}

Huang, Xiaohui ^{[5
,6
]}

Bremer, Jens ^{[7
]}

Rihko-Struckmann, Liisa K. ^{[7
]}

Batey, Darren ^{[8
]}

Cipiccia, Silvia ^{[8
]}

Titus, Juliane ^{[3
]}

Poppitz, David ^{[3
]}

Kuebel, Christian ^{[5
,6
,9
]}

Sundmacher, Kai ^{[4
,7
]}

Glaeser, Roger ^{[3
]}

Sheppard, Thomas L. ^{[1
,2
]}

机构：

[1] Karlsruhe Inst Technol KIT, Inst Catalysis Res & Technol, Hermann Von Helmholtz Pl 1, D-76344 Eggenstein Leopoldshafen, Germany

[2] Karlsruhe Inst Technol KIT, Inst Chem Technol & Polymer Chem, Engesserstr 20, D-76131 Karlsruhe, Germany

[3] Univ Leipzig, Inst Chem Technol, Linnestr 3, D-04103 Leipzig, Germany

[4] Otto von Guericke Univ, Inst Proc Engn, Chair Proc Syst Engn, Univ Pl 2, D-39106 Magdeburg, Germany

[5] Karlsruhe Inst Technol KIT, Inst Nanotechnol INT, Hermann Von Helmholtz Pl 1, D-76344 Eggenstein Leopoldshafen, Germany

[6] Tech Univ Darmstadt, Dept Mat & Earth Sci, Alarich Weiss Str 2, D-64287 Darmstadt, Germany

[7] Max Planck Inst Magdeburg, Dept Proc Syst Engn, Sandtorstr 1, D-39106 Magdeburg, Germany

[8] Diamond Light Source, Harwell Sci & Innovat Campus,Fermi Ave, Didcot OX11 0DE, Oxon, England

[9] Karlsruhe Inst Technol KIT, Karlsruhe Nano Micro Facil, Hermann Von Helmholtz Pl 1, D-76344 Eggenstein Leopoldshafen, Germany

来源：

CATALYSTS | 2020年 / 10卷 / 12期

关键词：

methanation; carbon dioxide; hierarchical porosity; nickel; alumina; tomography; porosity analysis; COMPUTED-TOMOGRAPHY; PARTIAL OXIDATION; NIAL2O4; SPINEL; ELECTRON; NICKEL; ALUMINA; RECONSTRUCTION; HYDROGENATION; DISTRIBUTIONS; DIFFRACTION;

D O I：

10.3390/catal10121471

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：

CO2 methanation is often performed on Ni/Al2O3 catalysts, which can suffer from mass transport limitations and, therefore, decreased efficiency. Here we show the application of a hierarchically porous Ni/Al2O3 catalyst for methanation of CO2. The material has a well-defined and connected meso- and macropore structure with a total porosity of 78%. The pore structure was thoroughly studied with conventional methods, i.e., N-2 sorption, Hg porosimetry, and He pycnometry, and advanced imaging techniques, i.e., electron tomography and ptychographic X-ray computed tomography. Tomography can quantify the pore system in a manner that is not possible using conventional porosimetry. Macrokinetic simulations were performed based on the measures obtained by porosity analysis. These show the potential benefit of enhanced mass-transfer properties of the hierarchical pore system compared to a pure mesoporous catalyst at industrially relevant conditions. Besides the investigation of the pore system, the catalyst was studied by Rietveld refinement, diffuse reflectance ultraviolet-visible (DRUV/vis) spectroscopy, and H-2-temperature programmed reduction (TPR), showing a high reduction temperature required for activation due to structural incorporation of Ni into the transition alumina. The reduced hierarchically porous Ni/Al2O3 catalyst is highly active in CO2 methanation, showing comparable conversion and selectivity for CH4 to an industrial reference catalyst.

引用

页码：1 / 22

页数：22

共 69 条

[11] Enhanced activity of CO2 methanation over mesoporous nanocrystalline Ni-Al2O3 catalysts prepared by ultrasound-assisted co-precipitation method [J].