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      A Co-Doped Nanorod-like RuO 2 Electrocatalyst with Abundant Oxygen Vacancies for Acidic Water Oxidation

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          Summary

          Active and highly stable electrocatalysts for oxygen evolution reaction (OER) in acidic media are currently in high demand as a cleaner alternative to the combustion of fossil fuels. Herein, we report a Co-doped nanorod-like RuO 2 electrocatalyst with an abundance of oxygen vacancies achieved through the facile, one-step annealing of a Ru-exchanged ZIF-67 derivative. The compound exhibits ultra-high OER performance in acidic media, with a low overpotential of 169 mV at 10 mA cm −2 while maintaining excellent activity, even when exposed to a 50-h galvanostatic stability test at a constant current of 10 mA cm −2. The dramatic enhancement in OER performance is mainly attributed to the abundance of oxygen vacancies and modulated electronic structure of the Co-doped RuO 2 that rely on a vacancy-related lattice oxygen oxidation mechanism (LOM) rather than adsorbate evolution reaction mechanism (AEM), as revealed and supported by experimental characterizations as well as density functional theory (DFT) calculations.

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          Highlights

          • •

            A Co-doped RuO 2 electrocatalyst with an abundance of oxygen vacancies was synthesized

          • •

            The compound exhibits ultra-high OER performance in acidic media

          • •

            The oxygen vacancies contribute to the high OER performance

          Abstract

          Catalysis; Electrochemical Energy Production; Nanomaterials

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          Most cited references36

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          Double perovskites as a family of highly active catalysts for oxygen evolution in alkaline solution.

          Alexis Grimaud, Kevin J May, Christopher Carlton … (2013)
          The electronic structure of transition metal oxides governs the catalysis of many central reactions for energy storage applications such as oxygen electrocatalysis. Here we exploit the versatility of the perovskite structure to search for oxide catalysts that are both active and stable. We report double perovskites (Ln₀.₅Ba₀.₅)CoO(₃-δ) (Ln=Pr, Sm, Gd and Ho) as a family of highly active catalysts for the oxygen evolution reaction upon water oxidation in alkaline solution. These double perovskites are stable unlike pseudocubic perovskites with comparable activities such as Ba₀.₅Sr₀.₅Co₀.₈Fe₀.₂O(₃-δ) which readily amorphize during the oxygen evolution reaction. The high activity and stability of these double perovskites can be explained by having the O p-band centre neither too close nor too far from the Fermi level, which is computed from ab initio studies.
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            High Electrocatalytic Hydrogen Evolution Activity of an Anomalous Ruthenium Catalyst.

            Yan Jiao, Ying Chen, Yao Zheng … (2016)
            Hydrogen evolution reaction (HER) is a critical process due to its fundamental role in electrocatalysis. Practically, the development of high-performance electrocatalysts for HER in alkaline media is of great importance for the conversion of renewable energy to hydrogen fuel via photoelectrochemical water splitting. However, both mechanistic exploration and materials development for HER under alkaline conditions are very limited. Precious Pt metal, which still serves as the state-of-the-art catalyst for HER, is unable to guarantee a sustainable hydrogen supply. Here we report an anomalously structured Ru catalyst that shows 2.5 times higher hydrogen generation rate than Pt and is among the most active HER electrocatalysts yet reported in alkaline solutions. The identification of new face-centered cubic crystallographic structure of Ru nanoparticles was investigated by high-resolution transmission electron microscopy imaging, and its formation mechanism was revealed by spectroscopic characterization and theoretical analysis. For the first time, it is found that the Ru nanocatalyst showed a pronounced effect of the crystal structure on the electrocatalytic activity tested under different conditions. The combination of electrochemical reaction rate measurements and density functional theory computation shows that the high activity of anomalous Ru catalyst in alkaline solution originates from its suitable adsorption energies to some key reaction intermediates and reaction kinetics in the HER process.
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              Systematic XPS studies of metal oxides, hydroxides and peroxides

              Jean-Charles Dupin, Danielle Gonbeau, Philippe Vinatier … (2000)
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                Author and article information

                Contributors
                Yichao Lin
                Qiuju Zhang
                Liang Chen
                Journal
                Journal ID (nlm-ta): iScience
                Journal ID (iso-abbrev): iScience
                Title: iScience
                Publisher: Elsevier
                ISSN (Electronic): 2589-0042
                Publication date PMC-release: 04 December 2019
                Publication date Collection: 24 January 2020
                Publication date (Electronic): 04 December 2019
                Volume: 23
                Issue: 1
                Electronic Location Identifier: 100756
                Affiliations
                [1 ]Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Sciences, Ningbo, Zhejiang 315201, P.R. China
                [2 ]University of Chinese Academy of Sciences, Beijing 100049, P. R. China
                [3 ]School of Materials Science and Chemical Engineering, Ningbo University, Ningbo 315211, P. R. China
                [4 ]Department of Chemistry and Chemical Biology, Rutgers, The State University of New Jersey, Piscataway, NJ 08854, USA
                [5 ]State Grid Ningbo Electric Power Supply Company, Ningbo, Zhejiang 315000, P.R. China
                [6 ]Department of Materials Science and Engineering, Southern University of Science and Technology, Shenzhen 518055, P. R. China
                [7 ]Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai 201800, P.R. China
                Author notes
                [∗ ]Corresponding author yclin@ 123456nimte.ac.cn
                [∗∗ ]Corresponding author zhangqj@ 123456nimte.ac.cn
                [∗∗∗ ]Corresponding author chenliang@ 123456nimte.ac.cn
                [8]

                These authors contributed equally

                [9]

                Lead Contact

                Article
                Publisher ID: S2589-0042(19)30501-2 Publisher ID: 100756
                DOI: 10.1016/j.isci.2019.100756
                PMC ID: 6941840
                PubMed ID: 31887659
                SO-VID: 232ab701-f6b1-4213-9389-900a94d2231e
                Copyright © © 2019 The Author(s)
                License:

                This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).

                History
                Date received : 21 July 2019
                Date revision received : 26 September 2019
                Date accepted : 28 November 2019
                Categories
                Subject: Article

                Keywords: catalysis,electrochemical energy production,nanomaterials
                Data availability:
                Keywords: catalysis, electrochemical energy production, nanomaterials

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