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      Enhanced oxygen reduction with single-atomic-site iron catalysts for a zinc-air battery and hydrogen-air fuel cell

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          Abstract

          Efficient, durable and inexpensive electrocatalysts that accelerate sluggish oxygen reduction reaction kinetics and achieve high-performance are highly desirable. Here we develop a strategy to fabricate a catalyst comprised of single iron atomic sites supported on a nitrogen, phosphorus and sulfur co-doped hollow carbon polyhedron from a metal-organic framework@polymer composite. The polymer-based coating facilitates the construction of a hollow structure via the Kirkendall effect and electronic modulation of an active metal center by long-range interaction with sulfur and phosphorus. Benefiting from structure functionalities and electronic control of a single-atom iron active center, the catalyst shows a remarkable performance with enhanced kinetics and activity for oxygen reduction in both alkaline and acid media. Moreover, the catalyst shows promise for substitution of expensive platinum to drive the cathodic oxygen reduction reaction in zinc-air batteries and hydrogen-air fuel cells.

          Abstract

          Development of fuel cells and metal-air batteries is hindered by electrocatalyst performance, which can be enhanced with uniform and atomically dispersed active sites. Here the authors report an iron-based electrocatalyst for oxygen reduction in cathodes for a zinc-air battery and a hydrogen-air fuel cell.

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          Generalized Gradient Approximation Made Simple

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            Efficient iterative schemes forab initiototal-energy calculations using a plane-wave basis set

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              Identification of catalytic sites for oxygen reduction in iron- and nitrogen-doped graphene materials.

              While platinum has hitherto been the element of choice for catalysing oxygen electroreduction in acidic polymer fuel cells, tremendous progress has been reported for pyrolysed Fe-N-C materials. However, the structure of their active sites has remained elusive, delaying further advance. Here, we synthesized Fe-N-C materials quasi-free of crystallographic iron structures after argon or ammonia pyrolysis. These materials exhibit nearly identical Mössbauer spectra and identical X-ray absorption near-edge spectroscopy (XANES) spectra, revealing the same Fe-centred moieties. However, the much higher activity and basicity of NH3-pyrolysed Fe-N-C materials demonstrates that the turnover frequency of Fe-centred moieties depends on the physico-chemical properties of the support. Following a thorough XANES analysis, the detailed structures of two FeN4 porphyrinic architectures with different O2 adsorption modes were then identified. These porphyrinic moieties are not easily integrated in graphene sheets, in contrast with Fe-centred moieties assumed hitherto for pyrolysed Fe-N-C materials. These new insights open the path to bottom-up synthesis approaches and studies on site-support interactions.
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                Author and article information

                Contributors
                wangdingsheng@mail.tsinghua.edu.cn
                Journal
                Nat Commun
                Nat Commun
                Nature Communications
                Nature Publishing Group UK (London )
                2041-1723
                21 December 2018
                21 December 2018
                2018
                : 9
                : 5422
                Affiliations
                [1 ]ISNI 0000 0001 0662 3178, GRID grid.12527.33, Department of Chemistry, , Tsinghua University, ; 100084 Beijing, China
                [2 ]ISNI 0000 0000 9040 3743, GRID grid.28703.3e, Beijing Guyue New Materials Research Institute, , Beijing University of Technology, ; 100124 Beijing, China
                [3 ]ISNI 0000000119573309, GRID grid.9227.e, Beijing Synchrotron Radiation Facility, Institute of High Energy Physics, , Chinese Academy of Sciences, ; 100049 Beijing, China
                [4 ]ISNI 0000000119573309, GRID grid.9227.e, State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, , Chinese Academy of Sciences, ; 030001 Taiyuan, China
                [5 ]ISNI 0000000119573309, GRID grid.9227.e, Mössbauer Effect Data Center, Dalian Institute of Chemical Physics, , Chinese Academy of Sciences, ; 116023 Dalian, China
                [6 ]ISNI 0000 0000 9291 3229, GRID grid.162110.5, State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, , Wuhan University of Technology, ; 430070 Wuhan, China
                [7 ]ISNI 0000 0000 9931 8406, GRID grid.48166.3d, State Key Lab of Organic-Inorganic Composites and Beijing Advanced Innovation Center for Soft Matter Science and Engineering, , Beijing University of Chemical Technology, ; 100029 Beijing, China
                Author information
                http://orcid.org/0000-0001-8860-093X
                http://orcid.org/0000-0003-0074-7633
                Article
                7850
                10.1038/s41467-018-07850-2
                6303331
                30575726
                7f2ed139-ca60-4e9a-ae9a-365727aec16f
                © The Author(s) 2018

                Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/.

                History
                : 17 March 2018
                : 30 November 2018
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