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Biomimetic CO Oxidation Below – 100 ⁰C by a Nitrate-Containing Metal-Free Microporous System

preprint
submitted on 26.05.2020 and posted on 27.05.2020 by Konstantin Khivantsev, Nicholas R. Jaegers, Hristiyan A. Aleksandrov, Libor Kovarik, Miroslaw A. Derewinski, Yong Wang, Georgi N. Vayssilov, János Szanyi

CO oxidation is of importance both for organic and inorganic systems. Transition and precious metals on various supports can oxidize CO to CO2. Among them, few systems, like Au/TiO2, can perform CO oxidation at the low temperature of -70 ⁰C. Living (an)aerobic organisms perform CO oxidation with nitrate using complex enzymes under ambient temperatures which is an important pathway of their living cycle that enables them to “breathe”/produce energy in the absence of oxygen and leads to the carbonate mineral formation. Herein, we report that CO can be oxidized to CO2 by nitrate at –140 ⁰C in completely inorganic system (zeolite) without metals. The transformation of NOx and CO species in zeolite as well as the origin of this unique activity (catalyzed by Bronsted acid sites) are clarified using spectroscopic and computational approach.

Funding

HAA and GNV are grateful for the support by the European Regional Development Fund and the Operational Program "Science and Education for Smart Growth" under contract UNITe № BG05M2OP001-1.001-0004 -С01 (2018-2023). The research at PNNL was supported by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Biosciences, and Geosciences Catalysis Program (DEAC05-RL01830, FW-47319). Experiments were conducted in the Environmental Molecular Sciences Laboratory (EMSL), a national scientific user facility sponsored by the Department of Energy’s Office of Biological and Environmental Research at Pacific Northwest National Laboratory (PNNL). PNNL is a multi-program national laboratory operated for the DOE by Battelle Memorial Institute under Contract DE-AC06-76RL01830.

History

Email Address of Submitting Author

Konstantin.Khivantsev@pnnl.gov

Institution

Pacific Northwest National Laboratory

Country

United States

ORCID For Submitting Author

0000-0002-4810-586X

Declaration of Conflict of Interest

No conflicts of interest to declare

Version Notes

Version 1.0

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