Water and carbon oxides on monoclinic zirconia: experimental and computational insights

文献情報

出版日 2014-08-13

DOI 10.1039/C4CP02742F

インパクトファクター 3.676

著者

Sonja Kouva, Jenni Andersin, Karoliina Honkala, Juha Lehtonen, Jaana Kanervo

原文を見る

要旨

Zirconium oxide (ZrO2, zirconia) is an interesting catalytic material to be used in biomass conversion, e.g., gasification and reforming. In this work, we show that reducing and hydrating pretreatments affect the surface sites on monoclinic zirconia. The multitechnique approach comprises temperature-programmed surface reactions (TPSR) under CO and CO2 at 100–550 °C, in situ DRIFTS investigations of the surface species and density functional theory (DFT) calculations. The key findings of the work are: (1) formates are formed either directly from gas-phase CO on terminal surface hydroxyls or via the linear CO surface species that are found exclusively on the reduced zirconia without water treatment; (2) formates are able to decompose at high temperature either reversibly to CO or reductively to CO2 and H2via surface reaction between formates and multicoordinated hydroxyls; and (3) a new weak reversible binding state of CO is found exclusively on ZrO2 that is first reduced and subsequently hydrated.

掲載誌

Physical Chemistry Chemical Physics

CiteScore: 5.5

自己引用率: 10.3%

年間論文数: 3036

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.