Highly Selective Au/ZnO via Colloidal Deposition for CO2 Hydrogenation to Methanol: Evidence of AuZn Role

License URL: http://creativecommons.org/licenses/by-sa/4.0

Gold, Au nanoparticles were deposited on ZnO, Al2O3, and Ga2O3 via colloidal method in order to investigate the role of support for CO2 hydrogenation to methanol. Au/ZnO was also produced using impregnation method to investigate the effect of colloidal method to improve methanol selectivity. Au/ZnO produced via sol immobilization showed high selectivity towards methanol meanwhile impregnation method produced Au/ZnO catalyst with high selectivity towards CO. The CO2 conversion was also influenced by the amount of Au weight loading. Au nanoparticles with average diameter of 3.5 nm exhibited 4% of CO2 conversion with 72% of methanol selectivity at 250 °C and 20 bar. The formation of AuZn alloy was identified as active sites for selective CO2 hydrogenation to methanol. Segregation of Zn from ZnO to form AuZn alloy increased the number of surface oxygen vacancy for CO2 adsorption to form formate intermediates. The formate was stabilized on AuZn alloy for further hydrogenation to form methanol. The use of Al2O3 and Ga2O3 inhibited the formation of Au alloy, and therefore reduced methanol production. Au/Al2O3 showed 77% selectivity to methane, meanwhile Au/Ga2O3 produced 100% selectivity towards CO. Copyright © 2021 by Authors, Published by BCREC Group. This is an open access article under the CC BY-SA License (https://creativecommons.org/licenses/by-sa/4.0).
Article Metrics:
- Olah, G.A. (2005). Beyond Oil and Gas: The Methanol Economy. Angewandte Chemie International Edition, 44(18), 2636–2639, doi: 10.1002/anie.200462121
- Behrens, M., Studt, F., Kasatkin, I., Kühl, S., Hävecker, M., Abild-Pedersen, F., Zander, S., Girgsdies, F., Kurr, P., Kniep, B.-L., Tovar, M., Fischer, R.W., Nørskov, J.K., Schlögl, R. (2012). The Active Site of Methanol Synthesis over Cu/ZnO/Al2O3 Industrial Catalysts. Science, 336(6083), 893, doi: 10.1126/science.1219831
- Speight, J.G. (2011). Chapter 8 - Hydrocarbons from Synthesis Gas. In J.G. Speight (Ed.), Handbook of Industrial Hydrocarbon Processes (pp. 281-323). Gulf Professional Publishing. doi: 10.1016/B978-0-7506-8632-7.10008-8
- Kattel, S., Ramírez, P.J., Chen, J.G., Rodriguez, J.A., Liu, P. (2017). Active sites for CO2 hydrogenation to methanol on Cu/ZnO catalysts. Science, 355(6331), 1296, doi: 10.1126/science.aal3573
- Jiang, X., Koizumi, N., Guo, X., Song, C. (2015). Bimetallic Pd–Cu catalysts for selective CO2 hydrogenation to methanol. Applied Catalysis B: Environmental, 170–171, 173–185, doi: 10.1016/j.apcatb.2015.01.010
- Edwards, J.H. (1995). Potential sources of CO2 and the options for its large-scale utilisation now and in the future. Catalysis Today, 23(1), 59–66, doi: 10.1016/0920-5861(94)00081-C
- Bahruji, H., Guan, S., Puthiyapura, V.K. (2016). Precious Metal Catalysts for Sustainable Energy and Environmental Remediation. In Modern Developments in Catalysis (pp. 211-251). World Scientific (Europe). doi: 10.1142/9781786341228_0007
- Saeidi, S., Najari, S., Fazlollahi, F., Nikoo, M.K., Sefidkon, F., Klemeš, J.J., Baxter, L.L. (2017). Mechanisms and kinetics of CO2 hydrogenation to value-added products: A detailed review on current status and future trends. Renewable and Sustainable Energy Reviews, 80, 1292–1311, doi: 10.1016/j.rser.2017.05.204
- Zhang, X., Liu, J.-X., Zijlstra, B., Filot, I.A.W., Zhou, Z., Sun, S., Hensen, E.J.M. (2018). Optimum Cu nanoparticle catalysts for CO2 hydrogenation towards methanol. Nano Energy, 43, 200–209, doi: 10.1016/j.nanoen.2017.11.021
- Bahruji, H., Bowker, M., Jones, W., Hayward, J., Ruiz Esquius, J., Morgan, D.J., Hutchings, G.J. (2017). PdZn catalysts for CO2 hydrogenation to methanol using chemical vapour impregnation (CVI). Faraday Discussions, 197, 309–324, doi: 10.1039/C6FD00189K
- Bond, G.C. (2016). Hydrogenation by gold catalysts: an unexpected discovery and a current assessment. Gold Bulletin, 49(3), 53–61, doi: 10.1007/s13404-016-0182-8
- Bahruji, H., Bowker, M., Hutchings, G., Dimitratos, N., Wells, P., Gibson, E., Jones, W., Brookes, C., Morgan, D., Lalev, G. (2016). Pd/ZnO catalysts for direct CO2 hydrogenation to methanol. Journal of Catalysis, 343, 133–146, doi: 10.1016/j.jcat.2016.03.017
- Hartadi, Y., Widmann, D., Behm, R.J. (2015). CO2 Hydrogenation to Methanol on Supported Au Catalysts under Moderate Reaction Conditions: Support and Particle Size Effects. ChemSusChem, 8(3), 456–465, doi: 10.1002/cssc.201402645
- Abdel-Mageed, A.M., Klyushin, A., Knop-Gericke, A., Schlögl, R., Behm, R.J. (2019). Influence of CO on the Activation, O-Vacancy Formation, and Performance of Au/ZnO Catalysts in CO2 Hydrogenation to Methanol. The Journal of Physical Chemistry Letters, 10(13), 3645–3653, doi: 10.1021/acs.jpclett.9b00925
- Pawinrat, P., Mekasuwandumrong, O., Panpranot, J. (2009). Synthesis of Au–ZnO and Pt–ZnO nanocomposites by one-step flame spray pyrolysis and its application for photocatalytic degradation of dyes. Catalysis Communications, 10(10), 1380–1385, doi: 10.1016/j.catcom.2009.03.002
- Derrouiche, S., La Fontaine, C., Thrimurtulu, G., Casale, S., Delannoy, L., Lauron-Pernot, H., Louis, C. (2016). Unusual behaviour of Au/ZnO catalysts in selective hydrogenation of butadiene due to the formation of a AuZn nanoalloy. Catalysis Science & Technology, 6(18), 6794–6805, doi: 10.1039/C5CY01664A
- Borissov, D., Pareek, A., Renner, F.U., Rohwerder, M. (2010). Electrodeposition of Zn and Au–Zn alloys at low temperature in an ionic liquid. Physical Chemistry Chemical Physics, 12(9), 2059–2062, doi: 10.1039/B919669B
- Wang, T., Jin, B., Jiao, Z., Lu, G., Ye, J., Bi, Y. (2014). Photo-directed growth of Au nanowires on ZnO arrays for enhancing photoelectrochemical performances. Journal of Materials Chemistry A, 2(37), 15553–15559, doi: 10.1039/C4TA02960G
- Bahruji, H., Armstrong, R.D., Ruiz Esquius, J., Jones, W., Bowker, M., Hutchings, G.J. (2018). Hydrogenation of CO2 to Dimethyl Ether over Brønsted Acidic PdZn Catalysts. Industrial & Engineering Chemistry Research, 57(20), 6821–6829, doi: 10.1021/acs.iecr.8b00230
- Bahruji, H., Esquius, J.R., Bowker, M., Hutchings, G., Armstrong, R.D., Jones, W. (2018). Solvent Free Synthesis of PdZn/TiO2 Catalysts for the Hydrogenation of CO2 to Methanol. Topics in Catalysis, 61(3), 144–153, doi: 10.1007/s11244-018-0885-6
- Shen, W.J., Jun, K.W., Choi, H.S., Lee, K.W. (2000). Thermodynamic Investigation of Methanol and Dimethyl Ether Synthesis from CO2 Hydrogenation. Korean Journal of Chemical Engineering, 17(2), 210–216, doi: 10.1007/BF02707145
- Sholeha, N.A., Jannah, L., Rohma, H.N., Widiastuti, N., Prasetyoko, D., Jalil, A.A., Bahruji, H. (2020). Synthesis of Zeolite Nay from Dealuminated Metakaolin as Ni Support for CO2 Hydrogenation to Methane. Clays and Clay Minerals, 68(5), 513–523, doi: 10.1007/s42860-020-00089-3
- Guilera, J., del Valle, J., Alarcón, A., Díaz, J.A., Andreu, T. (2019). Metal-oxide promoted Ni/Al2O3 as CO2 methanation micro-size catalysts. Journal of CO2 Utilization, 30, 11–17, doi: 10.1016/j.jcou.2019.01.003
- Strunk, J., Kähler, K., Xia, X., Comotti, M., Schüth, F., Reinecke, T., Muhler, M. (2009). Au/ZnO as catalyst for methanol synthesis: The role of oxygen vacancies. Applied Catalysis A: General, 359(1), 121–128, doi: 10.1016/j.apcata.2009.02.030
Last update: 2021-04-20 17:23:53
Last update: 2021-04-20 17:23:55
License URL: http://creativecommons.org/licenses/by-sa/4.0
Journal Author(s) Rights
In order for BCREC Group to publish and disseminate research articles, we need publishing rights (transfered from author(s) to publisher). This is determined by a publishing agreement between the Author(s) and BCREC Group. This agreement deals with the transfer or license of the copyright of publishing to BCREC Group, while Authors still retain significant rights to use and share their own published articles. BCREC Group supports the need for authors to share, disseminate and maximize the impact of their research and these rights, in any databases.
As a journal Author, you have rights for a large range of uses of your article, including use by your employing institute or company. These Author rights can be exercised without the need to obtain specific permission. Authors publishing in BCREC journals have wide rights to use their works for teaching and scholarly purposes without needing to seek permission, including:
- use for classroom teaching by Author or Author's institution and presentation at a meeting or conference and distributing copies to attendees;
- use for internal training by author's company;
- distribution to colleagues for their reseearch use;
- use in a subsequent compilation of the author's works;
- inclusion in a thesis or dissertation;
- reuse of portions or extracts from the article in other works (with full acknowledgement of final article);
- preparation of derivative works (other than commercial purposes) (with full acknowledgement of final article);
- voluntary posting on open web sites operated by author or author’s institution for scholarly purposes,
Authors/Readers/Third Parties can copy and redistribute the material in any medium or format, as well as remix, transform, and build upon the material for any purpose, even commercially, but they must give appropriate credit (the name of the creator and attribution parties (authors detail information), a copyright notice, an open access license notice, a disclaimer notice, and a link to the material), provide a link to the license, and indicate if changes were made (Publisher indicates the modification of the material (if any) and retain an indication of previous modifications using a CrossMark Policy and information about Erratum-Corrigendum notification).
Authors/Readers/Third Parties can read, print and download, redistribute or republish the article (e.g. display in a repository), translate the article, download for text and data mining purposes, reuse portions or extracts from the article in other works, sell or re-use for commercial purposes, remix, transform, or build upon the material, they must distribute their contributions under the same license as the original Creative Commons Attribution-ShareAlike (CC BY-SA).
Copyright Transfer Agreement for Publishing (Publishing Right)
The Authors submitting a manuscript do so on the understanding that if accepted for publication, copyright for publishing (publishing right) of the article shall be assigned/transferred to Publisher of Bulletin of Chemical Reaction Engineering & Catalysis journal and Department of Chemical Engineering Diponegoro University/Masyarakat Katalis Indonesia - Indonesian Catalyst Society (MKICS) (or BCREC Group).
Upon acceptance of an article, authors will be asked to complete a 'Copyright Transfer Agreement for Publishing (CTAP)'. An e-mail will be sent to the Corresponding Author confirming receipt of the manuscript together with a 'Copyright Transfer Agreement for Publishing' form by online version of this agreement.
Bulletin of Chemical Reaction Engineering & Catalysis journal and Department of Chemical Engineering Diponegoro University/Masyarakat Katalis Indonesia-Indonesian Catalyst Society (MKICS), the Editors and the Advisory International Editorial Board make every effort to ensure that no wrong or misleading data, opinions or statements be published in the journal. In any way, the contents of the articles and advertisements published in the Bulletin of Chemical Reaction Engineering & Catalysis are sole and exclusive responsibility of their respective authors and advertisers.
Remember, even though we ask for a transfer of copyright for publishing (CTAP), our journal Author(s) retain (or are granted back) significant scholarly rights as mentioned before.
The Copyright Transfer Agreement for Publishing (CTAP) Form can be downloaded here: [Copyright Transfer Agreement for Publishing (CTAP) Form BCREC 2020]
The copyright form should be signed electronically and send to the Editorial Office in the form of original e-mail below:
Prof. Dr. I. Istadi (Editor-in-Chief)
Editorial Office of Bulletin of Chemical Reaction Engineering & Catalysis
Laboratory of Plasma-Catalysis (R3.5), UPT Laboratorium Terpadu, Universitas Diponegoro
Jl. Prof. Soedarto, Semarang, Central Java, Indonesia 50275
Telp/Whatsapp: +62-81-316426342
E-mail: bcrec[at]live.undip.ac.id
(This policy statements has been updated at 24th December 2020)