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      The effect of milling parameters on the mechanochemical synthesis of Pd–CeO 2 methane oxidation catalysts

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          Abstract

          Pd–ceria interaction can be tuned by suitable milling intensity to obtain highly active methane oxidation catalysts.

          Abstract

          The preparation of catalytic materials via mechanochemical routes is a very promising alternative to complex wet chemical syntheses due to its simplicity, versatility and ecological advantages. The mechanical mixing of Pd nanoparticles and CeO 2 results in very active methane oxidation catalysts; here we explore the effect of milling parameters on the overall performance of Pd–ceria catalysts. The high methane combustion activity is the result of nanoscale interaction between palladium and cerium oxide and it is shown to be strongly dependent on the intensity of milling. This was investigated through methane combustion tests up to 1173 K and characterized by means of temperature programmed oxidation and reduction experiments. The morphological features of the obtained materials were investigated by HRTEM analysis and correlated to the catalytic behavior.

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          Most cited references49

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          Hallmarks of mechanochemistry: from nanoparticles to technology.

          The aim of this review article on recent developments of mechanochemistry (nowadays established as a part of chemistry) is to provide a comprehensive overview of advances achieved in the field of atomistic processes, phase transformations, simple and multicomponent nanosystems and peculiarities of mechanochemical reactions. Industrial aspects with successful penetration into fields like materials engineering, heterogeneous catalysis and extractive metallurgy are also reviewed. The hallmarks of mechanochemistry include influencing reactivity of solids by the presence of solid-state defects, interphases and relaxation phenomena, enabling processes to take place under non-equilibrium conditions, creating a well-crystallized core of nanoparticles with disordered near-surface shell regions and performing simple dry time-convenient one-step syntheses. Underlying these hallmarks are technological consequences like preparing new nanomaterials with the desired properties or producing these materials in a reproducible way with high yield and under simple and easy operating conditions. The last but not least hallmark is enabling work under environmentally friendly and essentially waste-free conditions (822 references).
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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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              Mechanochemistry: A Force of Synthesis

              The past decade has seen a reawakening of solid-state approaches to chemical synthesis, driven by the search for new, cleaner synthetic methodologies. Mechanochemistry, i.e., chemical transformations initiated or sustained by mechanical force, has been advancing particularly rapidly, from a laboratory curiosity to a widely applicable technique that not only enables a cleaner route to chemical transformations but offers completely new opportunities in making and screening for molecules and materials. This Outlook provides a brief overview of the recent achievements and opportunities created by mechanochemistry, including access to materials, molecular targets, and synthetic strategies that are hard or even impossible to access by conventional means.
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                Author and article information

                Contributors
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                Journal
                CSTAGD
                Catalysis Science & Technology
                Catal. Sci. Technol.
                Royal Society of Chemistry (RSC)
                2044-4753
                2044-4761
                August 12 2019
                2019
                : 9
                : 16
                : 4232-4238
                Affiliations
                [1 ]Dipartimento Politecnico
                [2 ]Università di Udine
                [3 ]and INSTM
                [4 ]33200 Udine
                [5 ]Italy
                [6 ]Institute of Energy Technologies
                [7 ]Department of Chemical Engineering and Barcelona Research Center in Multiscale Science and Engineering
                [8 ]Universitat Politècnica de Catalunya
                [9 ]08019 Barcelona
                [10 ]Spain
                Article
                10.1039/C9CY01098J
                899783bc-da4c-428b-b64c-fa19ae1a4fde
                © 2019

                http://rsc.li/journals-terms-of-use

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