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      Potential‐Cycling Synthesis of Single Platinum Atoms for Efficient Hydrogen Evolution in Neutral Media

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          Abstract

          Single‐atom catalysts (SACs) have exhibited high activities for the hydrogen evolution reaction (HER) electrocatalysis in acidic or alkaline media, when they are used with binders on cathodes. However, to date, no SACs have been reported for the HER electrocatalysis in neutral media. We demonstrate a potential‐cycling method to synthesize a catalyst comprising single Pt atoms on CoP‐based nanotube arrays supported by a Ni foam, termed PtSA‐NT‐NF. This binder‐free catalyst is centimeter‐scale and scalable. It is directly used as HER cathodes, whose performances at low and high current densities in phosphate buffer solutions (pH 7.2) are comparable to and better than, respectively, those of commercial Pt/C. The Pt mass activity of PtSA‐NT‐NF is 4 times of that of Pt/C, and its electrocatalytic stability is also better than that of Pt/C. This work provides a large‐scale production strategy for binder‐free Pt SAC electrodes for efficient HER in neutral media.

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          Thermally stable single-atom platinum-on-ceria catalysts via atom trapping

          J. Jones, H Xiong, A. T. DeLaRiva … (2016)
          Catalysts based on single atoms of scarce precious metals can lead to more efficient use through enhanced reactivity and selectivity. However, single atoms on catalyst supports can be mobile and aggregate into nanoparticles when heated at elevated temperatures. High temperatures are detrimental to catalyst performance unless these mobile atoms can be trapped. We used ceria powders having similar surface areas but different exposed surface facets. When mixed with a platinum/aluminum oxide catalyst and aged in air at 800°C, the platinum transferred to the ceria and was trapped. Polyhedral ceria and nanorods were more effective than ceria cubes at anchoring the platinum. Performing synthesis at high temperatures ensures that only the most stable binding sites are occupied, yielding a sinter-resistant, atomically dispersed catalyst.
          Article 0 comments Cited 531 times – based on 0 reviews     Review now
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            Molecule-Level g-C3N4 Coordinated Transition Metals as a New Class of Electrocatalysts for Oxygen Electrode Reactions.

            Yao Zheng, Yan Jiao, Yihan Zhu … (2017)
            Organometallic complexes with metal-nitrogen/carbon (M-N/C) coordination are the most important alternatives to precious metal catalysts for oxygen reduction and evolution reactions (ORR and OER) in energy conversion devices. Here, we designed and developed a range of molecule-level graphitic carbon nitride (g-C3N4) coordinated transition metals (M-C3N4) as a new generation of M-N/C catalysts for these oxygen electrode reactions. As a proof-of-concept example, we conducted theoretical evaluation and experimental validation on a cobalt-C3N4 catalyst with a desired molecular configuration, which possesses comparable electrocatalytic activity to that of precious metal benchmarks for the ORR and OER in alkaline media. The correlation of experimental and computational results confirms that this high activity originates from the precise M-N2 coordination in the g-C3N4 matrix. Moreover, the reversible ORR/OER activity trend for a wide variety of M-C3N4 complexes has been constructed to provide guidance for the molecular design of this promising class of catalysts.
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              Identification of active sites in CO oxidation and water-gas shift over supported Pt catalysts.

              Kunlun Ding, Ahmet Gulec, Alexis Johnson … (2015)
              Identification and characterization of catalytic active sites are the prerequisites for an atomic-level understanding of the catalytic mechanism and rational design of high-performance heterogeneous catalysts. Indirect evidence in recent reports suggests that platinum (Pt) single atoms are exceptionally active catalytic sites. We demonstrate that infrared spectroscopy can be a fast and convenient characterization method with which to directly distinguish and quantify Pt single atoms from nanoparticles. In addition, we directly observe that only Pt nanoparticles show activity for carbon monoxide (CO) oxidation and water-gas shift at low temperatures, whereas Pt single atoms behave as spectators. The lack of catalytic activity of Pt single atoms can be partly attributed to the strong binding of CO molecules.
              Article 0 comments Cited 310 times – based on 0 reviews     Review now
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                Author and article information

                Contributors
                Dr. Xijun Liu: xjliu@tjut.edu.cn
                Prof. Jun Luo: jluo@tjut.edu.cn
                Journal
                Journal ID (nlm-ta): Angew Chem Int Ed Engl
                Journal ID (iso-abbrev): Angew. Chem. Int. Ed. Engl
                Journal ID (doi): 10.1002/(ISSN)1521-3773
                Journal ID (publisher-id): ANIE
                Title: Angewandte Chemie (International Ed. in English)
                Publisher: John Wiley and Sons Inc. (Hoboken )
                ISSN (Print): 1433-7851
                ISSN (Electronic): 1521-3773
                Publication date (Electronic): 23 August 2017
                Publication date (Print): 23 October 2017
                Volume: 56
                Issue: 44 ( doiID: 10.1002/anie.v56.44 )
                Pages: 13694-13698
                Affiliations
                [ 1 ] Center for Electron Microscopy TUT-FEI Joint Laboratory Tianjin Key Laboratory of Advanced Functional Porous Materials Institute for New Energy Materials & Low-Carbon Technologies School of Materials Science and Engineering Tianjin University of Technology Tianjin 300384 China
                Author notes
                [†]

                These authors contributed equally to this work.

                Article
                Publisher ID: ANIE201706921
                DOI: 10.1002/anie.201706921
                PMC ID: 5659130
                PubMed ID: 28787544
                SO-VID: 6de67851-368a-42dd-a578-2b94b441be55
                Copyright © © 2017 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA.
                License:

                This is an open access article under the terms of the Creative Commons Attribution‐NonCommercial License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited and is not used for commercial purposes.

                History
                Date received : 07 July 2017
                Page count
                Figures: 5, Tables: 0, References: 59, Pages: 5, Words: 0
                Funding
                Funded by: National Program for Thousand Young Talents of China
                Funded by: Tianjin Municipal Education Commission
                Funded by: Tianjin Municipal Science and Technology Commission
                Award ID: 15JCYBJC52600
                Funded by: National Natural Science Foundation of China
                Award ID: 21601136
                Award ID: 51572016
                Categories
                Subject: Communication
                Subject: Communications
                Subject: Hydrogen Evolution | Very Important Paper
                Custom metadata
                source-schema-version-number 2.0
                component-id anie201706921
                cover-date October 23, 2017
                details-of-publishers-convertor Converter:WILEY_ML3GV2_TO_NLMPMC version:5.2.1 mode:remove_FC converted:26.10.2017

                ScienceOpen disciplines: Chemistry
                Keywords: electrode materials,hydrogen evolution reaction,platinum,potential cycling,single-atom catalysis
                Data availability:
                ScienceOpen disciplines: Chemistry
                Keywords: electrode materials, hydrogen evolution reaction, platinum, potential cycling, single-atom catalysis

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