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Low-Temperature Dehydrogenation of Ethanol on Atomically Dispersed Gold Supported on ZnZrOx
ACS Catalysis ( IF 11.3 ) Pub Date : 2015-12-08 00:00:00 , DOI: 10.1021/acscatal.5b01593 Chongyang Wang 1 , Gabriella Garbarino 1, 2 , Lawrence F. Allard 3 , Faith Wilson 1 , Guido Busca 2 , Maria Flytzani-Stephanopoulos 1
ACS Catalysis ( IF 11.3 ) Pub Date : 2015-12-08 00:00:00 , DOI: 10.1021/acscatal.5b01593 Chongyang Wang 1 , Gabriella Garbarino 1, 2 , Lawrence F. Allard 3 , Faith Wilson 1 , Guido Busca 2 , Maria Flytzani-Stephanopoulos 1
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Atomically dispersed gold supported on nanoscale ZnZrOx composite oxides was prepared and investigated in this work as a catalyst for the low-temperature ethanol dehydrogenation reactions. The composite ZnZrOx support disperses gold atomically and stabilizes it against growth much better than either of the neat oxides. Sequential ethanol conversion reactions to acetaldehyde and acetone take place on the Au/ZnZrOx catalysts within well-separated temperature windows over the range of tested temperatures (30–400 °C). ZnO modulates the acidity of the ZrO2 surface, and the extent of this was followed by isopropanol temperature-programmed desorption with online mass spectrometry (IPA-TPD/MS; and by diffuse reflectance UV−Vis−IR). Catalyst activity and selectivity were tested by temperature-programmed surface reaction (TPSR) and under steady-state reaction conditions. The work has demonstrated that ZnZrOx with optimized ZnO distribution preserves the active Au–Ox surface species under reaction conditions and suppresses undesired dehydration reactions. Addition of gold on the bare zirconia support passivates the acid sites catalyzing ethanol dehydration and introduces desired dehydrogenation sites at low temperatures (∼200 °C).
中文翻译：
ZnZrO x负载原子分散金对乙醇的低温脱氢
制备了分散在纳米级ZnZrO x复合氧化物上的原子分散金，并在这项工作中进行了研究，以作为低温乙醇脱氢反应的催化剂。复合ZnZrO x载体比任何一种纯氧化物都原子分散金，并使金的生长稳定化。在Au / ZnZrO x催化剂上，在测试温度范围内（30-400°C），在适当分隔的温度窗口内，乙醇顺序转化为乙醛和丙酮。ZnO调节ZrO 2的酸度表面，然后用在线质谱（IPA-TPD / MS；以及漫反射UV-Vis-IR）对异丙醇进行程序升温脱附。通过程序升温表面反应（TPSR）并在稳态反应条件下测试催化剂的活性和选择性。这项工作表明，具有最佳ZnO分布的ZnZrO x在反应条件下保留了活性Au-O x表面物种，并抑制了不希望的脱水反应。在裸露的氧化锆载体上添加金会钝化催化乙醇脱水的酸位，并在低温（约200°C）下引入所需的脱氢位。
更新日期：2015-12-08
中文翻译：
ZnZrO x负载原子分散金对乙醇的低温脱氢
制备了分散在纳米级ZnZrO x复合氧化物上的原子分散金，并在这项工作中进行了研究，以作为低温乙醇脱氢反应的催化剂。复合ZnZrO x载体比任何一种纯氧化物都原子分散金，并使金的生长稳定化。在Au / ZnZrO x催化剂上，在测试温度范围内（30-400°C），在适当分隔的温度窗口内，乙醇顺序转化为乙醛和丙酮。ZnO调节ZrO 2的酸度表面，然后用在线质谱（IPA-TPD / MS；以及漫反射UV-Vis-IR）对异丙醇进行程序升温脱附。通过程序升温表面反应（TPSR）并在稳态反应条件下测试催化剂的活性和选择性。这项工作表明，具有最佳ZnO分布的ZnZrO x在反应条件下保留了活性Au-O x表面物种，并抑制了不希望的脱水反应。在裸露的氧化锆载体上添加金会钝化催化乙醇脱水的酸位，并在低温（约200°C）下引入所需的脱氢位。
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