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      Atomically dispersed cobalt on graphitic carbon nitride as a robust catalyst for selective oxidation of ethylbenzene by peroxymonosulfate

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          Abstract

          A Co single-atom catalyst on g-C 3N 4 support was prepared for the selective oxidation of ethylbenzene (EB) to acetophenone (AcPO) by peroxymonosulfate (PMS). The Co atoms bonded with N were robust active sites for EB oxidation via the radical pathway.

          Abstract

          The development of a highly efficient strategy for the activation of the C–H bond in hydrocarbons is one of the most challenging tasks facing the chemical industries. The synthesis of novel catalysts with atomically dispersed active centers is highly desirable to achieve the maximized atom efficiency. Here we report the controllable preparation of a Co-based single-atom catalyst anchored on a graphitic carbon nitride support (SACo@g-C 3N 4) with 3.17 wt% Co content, which is successfully applied for the selective oxidation of ethylbenzene (EB) to derive acetophenone (AcPO) via the activated peroxymonosulfate (PMS) oxidant. The Co atoms are chemically bonded with the N atoms of g-C 3N 4 and present exceptional stability and reusability to resist the applied acidic-oxidative environment. Both the EB conversion and AcPO selectivity were over 95% in this highly selective SACo@g-C 3N 4/PMS system under mild reaction conditions. The selective conversion of EB into AcPO is attributed to the oxidative radicals generated from the decomposition of PMS molecules via the electron transfer between Co atoms and PMS. Sulfate radicals (SO 4˙ ) make a greater contribution than others to activate the C–H bond in EB oxidation. This work uncovers a facile and scalable approach for the synthesis of a robust Co-based single atom catalyst (SAC) on a g-C 3N 4 support and unveils its potential in the oxidation of hydrocarbons via a highly efficient and environmentally benign PMS activation.

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          Single-atom catalysts: a new frontier in heterogeneous catalysis.

          Supported metal nanostructures are the most widely used type of heterogeneous catalyst in industrial processes. The size of metal particles is a key factor in determining the performance of such catalysts. In particular, because low-coordinated metal atoms often function as the catalytically active sites, the specific activity per metal atom usually increases with decreasing size of the metal particles. However, the surface free energy of metals increases significantly with decreasing particle size, promoting aggregation of small clusters. Using an appropriate support material that strongly interacts with the metal species prevents this aggregation, creating stable, finely dispersed metal clusters with a high catalytic activity, an approach industry has used for a long time. Nevertheless, practical supported metal catalysts are inhomogeneous and usually consist of a mixture of sizes from nanoparticles to subnanometer clusters. Such heterogeneity not only reduces the metal atom efficiency but also frequently leads to undesired side reactions. It also makes it extremely difficult, if not impossible, to uniquely identify and control the active sites of interest. The ultimate small-size limit for metal particles is the single-atom catalyst (SAC), which contains isolated metal atoms singly dispersed on supports. SACs maximize the efficiency of metal atom use, which is particularly important for supported noble metal catalysts. Moreover, with well-defined and uniform single-atom dispersion, SACs offer great potential for achieving high activity and selectivity. In this Account, we highlight recent advances in preparation, characterization, and catalytic performance of SACs, with a focus on single atoms anchored to metal oxides, metal surfaces, and graphene. We discuss experimental and theoretical studies for a variety of reactions, including oxidation, water gas shift, and hydrogenation. We describe advances in understanding the spatial arrangements and electronic properties of single atoms, as well as their interactions with the support. Single metal atoms on support surfaces provide a unique opportunity to tune active sites and optimize the activity, selectivity, and stability of heterogeneous catalysts, offering the potential for applications in a variety of industrial chemical reactions.
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            g-C3 N4 -Based Heterostructured Photocatalysts

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              A universal principle for a rational design of single-atom electrocatalysts

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                Author and article information

                Contributors
                Journal
                JMCAET
                Journal of Materials Chemistry A
                J. Mater. Chem. A
                Royal Society of Chemistry (RSC)
                2050-7488
                2050-7496
                February 9 2021
                2021
                : 9
                : 5
                : 3029-3035
                Affiliations
                [1 ]WA School of Mines: Minerals, Energy and Chemical Engineering
                [2 ]Curtin University
                [3 ]WA 6102
                [4 ]Australia
                [5 ]Eyring Materials Center
                [6 ]Arizona State University
                [7 ]Tempe
                [8 ]USA
                [9 ]School of Chemical Engineering
                [10 ]The University of Adelaide
                [11 ]Adelaide
                [12 ]School of Engineering
                [13 ]Edith Cowan University
                [14 ]WA 6027
                [15 ]Australian Synchrotron
                [16 ]Victoria 3168
                [17 ]Beijing Advanced Innovation Centre for Soft Matter Science and Engineering
                Article
                10.1039/D0TA11503G
                7524929f-d3a3-461b-9054-26f9dc4164d1
                © 2021

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

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