Ratnadip De1, Sabrina Gonglach2, Shounik Paul1, Michael Haas2, S S Sreejith1, Philipp Gerschel3, Ulf-Peter Apfel3,4, Thanh Huyen Vuong5, Jabor Rabeah5, Soumyajit Roy1, Wolfgang Schöfberger2. 1. Eco-Friendly Applied Materials Laboratory (EFAML), Materials Science Centre, Department of Chemical Sciences, Mohanpur Campus, Indian Institute of Science Education and Research, Kolkata, 741246, West Bengal, India. 2. Institute of Organic Chemistry, Johannes Kepler University Linz, Altenberger Straße 69, 4040, Linz, Austria. 3. Inorganic Chemistry I, Ruhr-Universität Bochum, Universitätsstraße 150, 44801, Bochum, Germany. 4. Fraunhofer UMSICHT, Osterfelder Straße 3, 46047, Oberhausen, Germany. 5. Leibniz-Institut für Katalyse e. V., Albert-Einstein-Straße 29a, 18059, Rostock, Germany.
Abstract
The controlled electrochemical reduction of carbon dioxide to value added chemicals is an important strategy in terms of renewable energy technologies. Therefore, the development of efficient and stable catalysts in an aqueous environment is of great importance. In this context, we focused on synthesizing and studying a molecular MnIII -corrole complex, which is modified on the three meso-positions with polyethylene glycol moieties for direct and selective production of acetic acid from CO2 . Electrochemical reduction of MnIII leads to an electroactive MnII species, which binds CO2 and stabilizes the reduced intermediates. This catalyst allows to electrochemically reduce CO2 to acetic acid in a moderate acidic aqueous medium (pH 6) with a selectivity of 63 % and a turn over frequency (TOF) of 8.25 h-1 , when immobilized on a carbon paper (CP) electrode. In terms of high selectivity towards acetate, we propose the formation and reduction of an oxalate type intermediate, stabilized at the MnIII -corrole center.
The controlled electrochemical reduction of n class="Chemical">carbon dioxide to value added chemicals is an important strategy in terms of renewable energy technologies. Therefore, the development of efficient and stable catalysts in an aqueous environment is of great importance. In this context, we focused on synthesizing and studying a molecularMnIII -corrole complex, which is modified on the three meso-positions with polyethylene glycol moieties for direct and selective production of acetic acid from CO2 . Electrochemical reduction of MnIII leads to an electroactive MnII species, which binds CO2 and stabilizes the reduced intermediates. This catalyst allows to electrochemically reduce CO2 to acetic acid in a moderate acidic aqueous medium (pH 6) with a selectivity of 63 % and a turn over frequency (TOF) of 8.25 h-1 , when immobilized on a carbon paper (CP) electrode. In terms of high selectivity towards acetate, we propose the formation and reduction of an oxalate type intermediate, stabilized at the MnIII -corrole center.
Authors: James Shipp; Simon Parker; Steven Spall; Samantha L Peralta-Arriaga; Craig C Robertson; Dimitri Chekulaev; Peter Portius; Simon Turega; Alastair Buckley; Rachael Rothman; Julia A Weinstein Journal: Inorg Chem Date: 2022-08-12 Impact factor: 5.436
Authors: Jessica Michalke; Kirill Faust; Thomas Bögl; Stephan Bartling; Nils Rockstroh; Christoph Topf Journal: Int J Mol Sci Date: 2022-08-05 Impact factor: 6.208