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      Simultaneous NO x and Particulate Matter Removal from Diesel Exhaust by Hierarchical Fe-Doped Ce–Zr Oxide

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          Abstract

          Particulate matter and NO x emissions from diesel exhaust remains one of the most pressing environmental problems. We explore the use of hierarchically ordered mixed Fe–Ce–Zr oxides for the simultaneous capture and oxidation of soot and reduction of NO x by ammonia in a single step. The optimized material can effectively trap the model soot particles in its open macroporous structure and oxidize the soot below 400 °C while completely removing NO in the 285–420 °C range. Surface characterization and DFT calculations emphasize the defective nature of Fe-doped ceria. The isolated Fe ions and associated oxygen vacancies catalyze facile NO reduction to N 2. A mechanism for the reduction of NO with NH 3 on Fe-doped ceria is proposed involving adsorbed O 2. Such adsorbed O 2 species will also contribute to the oxidation of soot.

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          Most cited references69

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          Generalized Gradient Approximation Made Simple.

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            Is Open Access

            A linear response approach to the calculation of the effective interaction parameters in the LDA+U method

            In this work we reexamine the LDA+U method of Anisimov and coworkers in the framework of a plane-wave pseudopotential approach. A simplified rotational-invariant formulation is adopted. The calculation of the Hubbard U entering the expression of the functional is discussed and a linear response approach is proposed that is internally consistent with the chosen definition for the occupation matrix of the relevant localized orbitals. In this way we obtain a scheme whose functionality should not depend strongly on the particular implementation of the model in ab-initio calculations. We demonstrate the accuracy of the method, computing structural and electronic properties of a few systems including transition and rare-earth correlated metals, transition metal monoxides and iron-silicate.
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              Exceptional activity for methane combustion over modular Pd@CeO2 subunits on functionalized Al2O3.

              There is a critical need for improved methane-oxidation catalysts to both reduce emissions of methane, a greenhouse gas, and improve the performance of gas turbines. However, materials that are currently available either have low activity below 400°C or are unstable at higher temperatures. Here, we describe a supramolecular approach in which single units composed of a palladium (Pd) core and a ceria (CeO(2)) shell are preorganized in solution and then homogeneously deposited onto a modified hydrophobic alumina. Electron microscopy and other structural methods revealed that the Pd cores remained isolated even after heating the catalyst to 850°C. Enhanced metal-support interactions led to exceptionally high methane oxidation, with complete conversion below 400°C and outstanding thermal stability under demanding conditions.
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                Author and article information

                Journal
                ACS Catal
                ACS Catal
                cs
                accacs
                ACS Catalysis
                American Chemical Society
                2155-5435
                26 April 2017
                02 June 2017
                : 7
                : 6
                : 3883-3892
                Affiliations
                []State Key Laboratory of Heavy Oil Processing, China University of Petroleum , 18 Fuxue Road, Chang Ping, Beijing 102249, China
                []Schuit Institute of Catalysis, Department of Chemical Engineering and Chemistry, Eindhoven University of Technology , P.O. Box 513, 5600 MB Eindhoven, The Netherlands
                [§ ]Institute of Catalysis for Energy and Environment, Shenyang Normal University , Shenyang 110034, China
                Author notes
                [* ]Tel: (+86) 10-89732778; e-mail: liujian@ 123456cup.edu.cn .
                [* ]Tel: (+86) 10-89732326; e-mail: zhaozhen@ 123456synu.edu.cn .
                [* ]Tel: (+31) 40-2455054; e-mail: E.J.M.Hensen@ 123456TUE.nl .
                Article
                10.1021/acscatal.6b03387
                5460666
                0750db84-f291-4dfa-aa7e-788e8e30cff8
                Copyright © 2017 American Chemical Society

                This is an open access article published under a Creative Commons Non-Commercial No Derivative Works (CC-BY-NC-ND) Attribution License, which permits copying and redistribution of the article, and creation of adaptations, all for non-commercial purposes.

                History
                : 29 November 2016
                : 22 April 2017
                Categories
                Research Article
                Custom metadata
                cs6b03387
                cs-2016-03387r

                soot oxidation,nox reduction,ceria,doping,macropores
                soot oxidation, nox reduction, ceria, doping, macropores

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