Abstract
AbstractPalladium promotion and deposition on monoclinic zirconia are effective strategies to boost the performance of bulk In2O3 in CO2-to-methanol and could unlock superior reactivity if well integrated into a single catalytic system. However, harnessing synergic effects of the individual components is crucial and very challenging as it requires precise control over their assembly. Herein, we present ternary Pd-In2O3-ZrO2 catalysts prepared by flame spray pyrolysis (FSP) with remarkable methanol productivity and improved metal utilization, surpassing their binary counterparts. Unlike established impregnation and co-precipitation methods, FSP produces materials combining low-nuclearity palladium species associated with In2O3 monolayers highly dispersed on the ZrO2 carrier, whose surface partially transforms from a tetragonal into a monoclinic-like structure upon reaction. A pioneering protocol developed to quantify oxygen vacancies using in situ electron paramagnetic resonance spectroscopy reveals their enhanced generation because of this unique catalyst architecture, thereby rationalizing its high and sustained methanol productivity.
Funder
Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschung
Agency for Science, Technology and Research
Publisher
Springer Science and Business Media LLC
Subject
General Physics and Astronomy,General Biochemistry, Genetics and Molecular Biology,General Chemistry,Multidisciplinary
Cited by
68 articles.
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