Cobalt Catalysts Decorated with Platinum Atoms Supported on Barium Zirconate Provide Enhanced Activity and Selectivity for CO2 Methanation

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• 作者：Hyun Ho Shin ; Li Lu ; Zhou Yang ; Christopher J. Kiely ; Steven McIntosh
• 刊名：ACS Catalysis
• 出版年：2016
• 出版时间：May 6, 2016
• 年：2016
• 卷：6
• 期：5
• 页码：2811-2818
• 全文大小：508K
• 年卷期：0
• ISSN：2155-5435

文摘

A perovskite-structured barium zirconate, BaZrO₃ (BZ), support is demonstrated to enhance the activity, relative to γ-Al₂O₃, of Co nanoparticle catalysts decorated with Pt for CO₂ methanation. The CO₂ methanation reaction may play a central role in both CO₂ utilization and energy storage strategies for renewable energy. These catalysts require cooperative hydrogen transport between the supported Pt and Co species to provide the desired functionality, as CO₂ preferentially dissociates on Co with H₂ dissociating primarily on Pt. In this work, this interaction is enhanced through an atomic decoration of Pt on the Co nanoparticle surface. This morphology is achieved through immobilization of colloidal Pt particles on the Co/BaZrO₃ support followed by selected catalyst pretreatment conditions to atomically disperse the Pt. Furthermore, at the same loading of Co and Pt (1 and 0.2 wt %, respectively), the barium zirconate support provides a more than 6-fold increase in CH₄ formation rate in comparison to previously studied γ-Al₂O₃ supports at 325 °C. This was accompanied by a CH₄ selectivity of over 70%, which was maintained over the measured temperature range of 250–350 °C; in fact, the selectivity was 80% at 325 °C, in comparison to only 43% for γ-Al₂O₃ support. This enhancement is attributed to a strong interaction between the Co particles and the BaZrO₃ support. Yttria doping at 5 and 30 atom % levels on the zirconia site led to a reduction of the catalytic performance relative to BaZrO₃, although the activity displayed at low levels of substitution was still higher than that over the γ-Al₂O₃ support.