Gold supported on zirconia polymorphs for dehydrogenation of formic acid in base-free aqueous medium
首发时间:2015-06-24
Abstract:It is highly desirable to develop an efficient heterogeneous catalyst for selective formic acid (FA) decomposition for ultraclean H2 gas in the absence of any organic/inorganic alkalis or extra additives under mild conditions. Au/ZrO2 has been proven to be a robust and efficient catalyst for FA dehydrogenation. Yet, there is a lack of understanding of the crystallite phase effect of ZrO2 for supporting active Au in target process. We report here ZrO2 with different polymorphs supported Au nanoparticles (NPs) can achieve near completion of FA dehydrogenation at 80 oC, and Au/m-ZrO2 catalyst with the largest amount of surface basic sites exhibited the highest catalytic activity. Basic sites in Au catalyst surface can substantially facilitate crucial FA deprotonation process in base-free aqueous medium which appears to be a key factor for achieving high dehydrogenation performance.
keywords: gold catalysis zirconia polymorphs formic acid base-free hydrogen
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ZrO2晶相对负载纳米金催化无碱水相甲酸分解制氢的影响
摘要:发展一种多相催化剂能在温和条件下高效选择性分解无碱甲酸制备纯净氢气对以甲酸为储氢原料的清洁能源非常重要。研究表明,Au/ZrO2对该反应展示出很好的催化性能。然而,关于ZrO2晶相对Au/ZrO2催化剂的整体影响却无报道。本研究发现,不同晶相ZrO2负载金催化剂,即Au/a-ZrO2、Au/m-ZrO2和Au/t-ZrO2,在80 oC时可完成甲酸脱氢转化,而拥有最多数量表面碱性位的Au/m-ZrO2显示出最高活性。在无碱水溶液中,金催化剂的表面碱性位可显著促进甲酸脱质子过程这一关键步骤。
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No.4647162972468143****
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