Probing surface-sensitive redox properties of VOx/TiO2 catalyst nanoparticles

被引:10
作者
Ek, Martin [1 ,2 ,3 ]
Arnarson, Logi [1 ]
Moses, Poul Georg [1 ]
Rasmussen, Soren B. [1 ]
Skoglundh, Magnus [2 ,4 ]
Olsson, Eva [2 ,3 ]
Helveg, Stig [1 ,5 ]
机构
[1] Haldor Topsoe Res Labs, Haldor Topsoes Alle 1, DK-2800 Lyngby, Denmark
[2] Chalmers Univ Technol, Competence Ctr Catalysis, S-41296 Gothenburg, Sweden
[3] Chalmers Univ Technol, Dept Phys, S-41296 Gothenburg, Sweden
[4] Chalmers Univ Technol, Dept Chem & Chem Engn, S-41296 Gothenburg, Sweden
[5] Tech Univ Denmark, Ctr Visualizing Catalyt Proc VISION, Dept Phys, DK-2800 Lyngby, Denmark
基金
新加坡国家研究基金会;
关键词
Electron energy loss spectroscopy;
D O I
10.1039/d0nr08943e
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Redox processes of oxide materials are fundamental in catalysis. These processes depend on the surface structure and stoichiometry of the oxide and are therefore expected to vary between surface facets. However, there is a lack of direct measurements of redox properties on the nanoscale for analysing the importance of such faceting effects in technical materials. Here, we address the facet-dependent redox properties of vanadium-oxide-covered anatase nanoparticles of relevance to, e.g., selective catalytic reduction of nitrogen oxides. The vanadium oxidation states at individual nanoscale facets are resolved in situ under catalytically relevant conditions by combining transmission electron microscopy imaging and electron energy loss spectroscopy. The measurements reveal that vanadium on {001} facets consistently retain higher oxidation states than on {10l} facets. Insight into such structure-sensitivity of surface redox processes opens prospects of tailoring oxide nanoparticles with enhanced catalytic functionalities.
引用
收藏
页码:7266 / 7272
页数:7
相关论文
共 40 条
[1]   A complete reaction mechanism for standard and fast selective catalytic reduction of nitrogen oxides on low coverage VOx/TiO2(001) catalysts [J].
Arnarson, Logi ;
Falsig, Hanne ;
Rasmussen, Soren B. ;
Lauritsen, Jeppe V. ;
Moses, Poul Georg .
JOURNAL OF CATALYSIS, 2017, 346 :188-197
[2]   Coexistence of Square Pyramidal Structures of Oxo Vanadium (+5) and (+4) Species Over Low-Coverage VOX/TiO2 (101) and (001) Anatase Catalysts [J].
Arnarson, Logi ;
Rasmussen, Soren B. ;
Falsig, Hanne ;
Lauritsen, Jeppe V. ;
Moses, Poul Georg .
JOURNAL OF PHYSICAL CHEMISTRY C, 2015, 119 (41) :23445-23452
[3]   Optimizing EELS acquisition [J].
Bosman, Michel ;
Keast, Vicki J. .
ULTRAMICROSCOPY, 2008, 108 (09) :837-846
[4]   Nature of active layer in vanadium oxide supported on titanium oxide and control of its reactivity in the selective oxidation and ammoxidation of alkylaromatics [J].
Centi, G .
APPLIED CATALYSIS A-GENERAL, 1996, 147 (02) :267-298
[5]   Revealing Surface Elemental Composition and Dynamic Processes Involved in Facet-Dependent Oxidation of Pt3Co Nanoparticles via in Situ Transmission Electron Microscopy [J].
Dai, Sheng ;
Hou, Yusheng ;
Onoue, Masatoshi ;
Zhang, Shuyi ;
Gao, Wenpei ;
Yan, Xingxu ;
Graham, George W. ;
Wu, Ruqian ;
Pan, Xiaoqing .
NANO LETTERS, 2017, 17 (08) :4683-4688
[6]   The surface science of titanium dioxide [J].
Diebold, U .
SURFACE SCIENCE REPORTS, 2003, 48 (5-8) :53-229
[7]   SOLID-STATE V-51 NMR STRUCTURAL STUDIES OF VANADIUM(V) OXIDE CATALYSTS SUPPORTED ON TIO2(ANATASE) AND TIO2(RUTILE) - THE INFLUENCE OF SURFACE IMPURITIES ON THE VANADIUM(V) COORDINATION [J].
ECKERT, H ;
DEO, G ;
WACHS, IE ;
HIRT, AM .
COLLOIDS AND SURFACES, 1990, 45 :347-359
[8]   Visualizing atomic-scale redox dynamics in vanadium oxide-based catalysts [J].
Ek, Martin ;
Ramasse, Quentin M. ;
Arnarson, Logi ;
Moses, Poul Georg ;
Helveg, Stig .
NATURE COMMUNICATIONS, 2017, 8
[9]   Electronic structure calculations with GPAW: a real-space implementation of the projector augmented-wave method [J].
Enkovaara, J. ;
Rostgaard, C. ;
Mortensen, J. J. ;
Chen, J. ;
Dulak, M. ;
Ferrighi, L. ;
Gavnholt, J. ;
Glinsvad, C. ;
Haikola, V. ;
Hansen, H. A. ;
Kristoffersen, H. H. ;
Kuisma, M. ;
Larsen, A. H. ;
Lehtovaara, L. ;
Ljungberg, M. ;
Lopez-Acevedo, O. ;
Moses, P. G. ;
Ojanen, J. ;
Olsen, T. ;
Petzold, V. ;
Romero, N. A. ;
Stausholm-Moller, J. ;
Strange, M. ;
Tritsaris, G. A. ;
Vanin, M. ;
Walter, M. ;
Hammer, B. ;
Hakkinen, H. ;
Madsen, G. K. H. ;
Nieminen, R. M. ;
Norskov, J. K. ;
Puska, M. ;
Rantala, T. T. ;
Schiotz, J. ;
Thygesen, K. S. ;
Jacobsen, K. W. .
JOURNAL OF PHYSICS-CONDENSED MATTER, 2010, 22 (25)
[10]  
Ertl G., 2008, Handbook of Heterogeneous Catalysis, V1