Direct single-enzyme biomineralization of catalytically active ceria and ceria-zirconia nanocrystals

Curran, Christopher D., Lu, Li, Jia, Yue, Kiely, Christopher J. ORCID: https://orcid.org/0000-0001-5412-0970, Berger, Bryan W. and McIntosh, Steven 2017. Direct single-enzyme biomineralization of catalytically active ceria and ceria-zirconia nanocrystals. ACS Nano 11 (3) , pp. 3337-3346. 10.1021/acsnano.7b00696

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Abstract

Biomineralization is an intriguing approach to the synthesis of functional inorganic materials for energy applications whereby biological systems are engineered to mineralize inorganic materials and control their structure over multiple length scales under mild reaction conditions. Herein we demonstrate a single-enzyme-mediated biomineralization route to synthesize crystalline, catalytically active, quantum-confined ceria (CeO2–x) and ceria–zirconia (Ce1–yZryO2–x) nanocrystals for application as environmental catalysts. In contrast to typical anthropogenic synthesis routes, the crystalline oxide nanoparticles are formed at room temperature from an otherwise inert aqueous solution without the addition of a precipitant or additional reactant. An engineered form of silicatein, rCeSi, as a single enzyme not only catalyzes the direct biomineralization of the nanocrystalline oxides but also serves as a templating agent to control their morphological structure. The biomineralized nanocrystals of less than 3 nm in diameter are catalytically active toward carbon monoxide oxidation following an oxidative annealing step to remove carbonaceous residue. The introduction of zirconia into the nanocrystals leads to an increase in Ce(III) concentration, associated catalytic activity, and the thermal stability of the nanocrystals.

Item Type:	Article
Date Type:	Publication
Status:	Published
Schools:	Chemistry Cardiff Catalysis Institute (CCI)
Publisher:	American Chemical Society
ISSN:	1936-0851
Date of First Compliant Deposit:	4 December 2017
Date of Acceptance:	17 February 2017
Last Modified:	21 Nov 2024 04:15
URI:	https://orca.cardiff.ac.uk/id/eprint/107226

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