Structural selectivity of supported Pd nanoparticles for catalytic NH3 oxidation resolved using combined operando spectroscopy

被引：109

作者：

Dann, Ellie K. ^{[1
,2
]}

Gibson, Emma K. ^{[2
,3
]}

Blackmore, Rachel H. ^{[2
,4
]}

Catlow, C. Richard A. ^{[1
,2
,5
]}

Collier, Paul ^{[6
]}

Chutia, Arunabhiram ^{[2
,7
]}

Erden, Tugce Eralp ^{[6
]}

Hardacre, Christopher ^{[2
,8
]}

Kroner, Anna ^{[9
]}

Nachtegaal, Maarten ^{[10
]}

Raj, Agnes ^{[6
]}

Rogers, Scott M. ^{[1
,2
]}

Taylor, S. F. Rebecca ^{[8
]}

Thompson, Paul ^{[11
]}

Tierney, George F. ^{[2
,4
]}

Zeinalipour-Yazdi, Constantinos D. ^{[2
,12
]}

Goguet, Alexandre ^{[2
,13
]}

Wells, Peter P. ^{[2
,4
,9
]}

机构：

[1] UCL, Dept Chem, London, England

[2] Rutherford Appleton Lab, UK Catalysis Hub, Res Complex Harwell, Didcot, Oxon, England

[3] Univ Glasgow, Sch Chem, Glasgow, Lanark, Scotland

[4] Univ Southampton, Sch Chem, Southampton, Hants, England

[5] Cardiff Univ, Cardiff Catalysis Inst, Sch Chem, Cardiff, S Glam, Wales

[6] Sonning Common, Johnson Matthey Technol Ctr, Reading, Berks, England

[7] Univ Lincoln, Sch Chem, Lincoln, England

[8] Univ Manchester, Sch Chem Engn & Analyt Sci, Manchester, Lancs, England

[9] Diamond Light Source, Didcot, Oxon, England

[10] Paul Scherrer Inst, Villigen, Switzerland

[11] European Synchrotron Radiat Facil, XMaS, Grenoble, France

[12] Univ Greenwich, Sch Sci, Chatham, England

[13] Queens Univ Belfast, Sch Chem & Chem Engn, Belfast, Antrim, North Ireland

来源：

NATURE CATALYSIS | 2019年 / 2卷 / 02期

基金：

英国工程与自然科学研究理事会;

关键词：

INITIO MOLECULAR-DYNAMICS; WET AIR OXIDATION; AB-INITIO; PALLADIUM NANOPARTICLES; FT-IR; EXCHANGED ZEOLITES; AMMONIA OXIDATION; L-3; EDGE; NITROGEN; METAL;

D O I：

10.1038/s41929-018-0213-3

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：

The selective catalytic oxidation of NH3 to N-2 presents a promising solution for the abatement of unused NH3-based reductants from diesel exhaust after treatment. Supported Pd nanoparticle catalysts show selectivity to N-2 rather than NOx, which is investigated in this work. The link between Pd nanoparticle structure and surface reactivity was found using operando X-ray absorption fine structure spectroscopy, diffuse reflectance infrared Fourier-transformed spectroscopy and on-line mass spectrometry. Nitrogen insertion into the metallic Pd nanoparticle structure at low temperatures (<200 degrees C) was found to be responsible for high N-2 selectivity, whereas the unfavourable formation of NO is linked to adsorbed nitrates, which form at the surface of bulk PdO nanoparticles at high temperatures (>280 degrees C). Our work demonstrates the ability of combined operando spectroscopy and density functional theory calculations to characterize a previously unidentified PdNx species, and clarify the selectivitydirecting structure of supported Pd catalysts for the selective catalytic oxidation of NH3 to N-2.

引用

页码：157 / 163

页数：7

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