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      A spongy nickel-organic CO 2 reduction photocatalyst for nearly 100% selective CO production

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          Abstract

          A spongy nickel-organic photocatalyst with nearly 100% selective CO 2 to CO conversion.

          Abstract

          Solar-driven photocatalytic conversion of CO 2 into fuels has attracted a lot of interest; however, developing active catalysts that can selectively convert CO 2 to fuels with desirable reaction products remains a grand challenge. For instance, complete suppression of the competing H 2 evolution during photocatalytic CO 2-to-CO conversion has not been achieved before. We design and synthesize a spongy nickel-organic heterogeneous photocatalyst via a photochemical route. The catalyst has a crystalline network architecture with a high concentration of defects. It is highly active in converting CO 2 to CO, with a production rate of ~1.6 × 10 4 μmol hour −1 g −1. No measurable H 2 is generated during the reaction, leading to nearly 100% selective CO production over H 2 evolution. When the spongy Ni-organic catalyst is enriched with Rh or Ag nanocrystals, the controlled photocatalytic CO 2 reduction reactions generate formic acid and acetic acid. Achieving such a spongy nickel-organic photocatalyst is a critical step toward practical production of high-value multicarbon fuels using solar energy.

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          Most cited references43

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          Water photolysis at 12.3% efficiency via perovskite photovoltaics and Earth-abundant catalysts.

          Although sunlight-driven water splitting is a promising route to sustainable hydrogen fuel production, widespread implementation is hampered by the expense of the necessary photovoltaic and photoelectrochemical apparatus. Here, we describe a highly efficient and low-cost water-splitting cell combining a state-of-the-art solution-processed perovskite tandem solar cell and a bifunctional Earth-abundant catalyst. The catalyst electrode, a NiFe layered double hydroxide, exhibits high activity toward both the oxygen and hydrogen evolution reactions in alkaline electrolyte. The combination of the two yields a water-splitting photocurrent density of around 10 milliamperes per square centimeter, corresponding to a solar-to-hydrogen efficiency of 12.3%. Currently, the perovskite instability limits the cell lifetime.
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            Photocatalytic Reduction of CO2on TiO2and Other Semiconductors

            Rising atmospheric levels of carbon dioxide and the depletion of fossil fuel reserves raise serious concerns about the ensuing effects on the global climate and future energy supply. Utilizing the abundant solar energy to convert CO2 into fuels such as methane or methanol could address both problems simultaneously as well as provide a convenient means of energy storage. In this Review, current approaches for the heterogeneous photocatalytic reduction of CO2 on TiO2 and other metal oxide, oxynitride, sulfide, and phosphide semiconductors are presented. Research in this field is focused primarily on the development of novel nanostructured photocatalytic materials and on the investigation of the mechanism of the process, from light absorption through charge separation and transport to CO2 reduction pathways. The measures used to quantify the efficiency of the process are also discussed in detail.
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              The teraton challenge. A review of fixation and transformation of carbon dioxide

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                Author and article information

                Journal
                Sci Adv
                Sci Adv
                SciAdv
                advances
                Science Advances
                American Association for the Advancement of Science
                2375-2548
                July 2017
                28 July 2017
                : 3
                : 7
                : e1700921
                Affiliations
                [1 ]Department of Materials Science and Engineering, University of California, Berkeley, Berkeley, CA 94720, USA.
                [2 ]Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA.
                [3 ]School of Chemical and Biomedical Engineering, Nanyang Technological University, 62 Nanyang Drive, Singapore 637459, Singapore.
                [4 ]SinBeRISE (Singapore-Berkeley Research Initiative for Sustainable Energy) CREATE, 1 Create Way, Singapore 138602, Singapore.
                [5 ]National Center for Materials Service Safety, University of Science and Technology Beijing, Beijing 100083, P. R. China.
                [6 ]Department of Chemistry, University of California, Berkeley, Berkeley, CA 94720, USA.
                [7 ]Center for Functional Nanomaterials, Brookhaven National Laboratory, Upton, NY 11973, USA.
                [8 ]Department of Chemistry, Virginia Tech, Blacksburg, VA 24061, USA.
                [9 ]Energy Storage and Distributed Resources Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA.
                [10 ]National Center for Electron Microscopy, Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA.
                [11 ]Leiden Institute of Chemistry, Leiden University, 2300 RA Leiden, Netherlands.
                Author notes
                [*]

                These authors contributed equally to this work.

                []Corresponding author. Email: rxu@ 123456ntu.edu.sg (R.X.); hmzheng@ 123456lbl.gov (H.Z.)
                Author information
                http://orcid.org/0000-0003-3289-1322
                http://orcid.org/0000-0003-0735-201X
                http://orcid.org/0000-0002-8238-8728
                http://orcid.org/0000-0002-4171-5964
                http://orcid.org/0000-0002-6521-868X
                http://orcid.org/0000-0002-3729-3148
                http://orcid.org/0000-0001-6427-5677
                http://orcid.org/0000-0002-2096-6078
                http://orcid.org/0000-0002-2148-8047
                http://orcid.org/0000-0001-6777-4594
                http://orcid.org/0000-0001-9334-9751
                http://orcid.org/0000-0002-7562-2627
                Article
                1700921
                10.1126/sciadv.1700921
                5533539
                28782031
                483908cb-3d28-46c2-955e-59025504774b
                Copyright © 2017 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution NonCommercial License 4.0 (CC BY-NC).

                This is an open-access article distributed under the terms of the Creative Commons Attribution-NonCommercial license, which permits use, distribution, and reproduction in any medium, so long as the resultant use is not for commercial advantage and provided the original work is properly cited.

                History
                : 24 March 2017
                : 27 June 2017
                Funding
                Funded by: doi http://dx.doi.org/10.13039/100000015, U.S. Department of Energy;
                Award ID: award320760
                Award ID: #DE-AC02-05CH11231
                Funded by: doi http://dx.doi.org/10.13039/100000015, U.S. Department of Energy;
                Award ID: award320761
                Award ID: #DE-AC02-76SF00515
                Categories
                Research Article
                Research Articles
                SciAdv r-articles
                Chemical Physics
                Custom metadata
                Florcloven Cruz

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