In situ S/TEM Reactions of Ag/ZrO2/SBA-16 Catalysts for Single-Step Conversion of Ethanol to Butadiene

In situ S/TEM Reactions of Ag/ZrO2/SBA-16 Catalysts for Single-Step Conversion of Ethanol to Butadiene
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DOI:
10.1017/s1431927619008031
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发表时间:
2019-08
影响因子:
2.8
通讯作者:
K. Unocic;V. Dagle;R. Dagle;Evan C. Wegener;J. Kropf;T. Krause;Daniel A. Ruddy;L. Allard;S. Habas
K. Unocic;V. Dagle;R. Dagle;Evan C. Wegener;J. Kropf;T. Krause;Daniel A. Ruddy;L. Allard;S. Habas
中科院分区:
工程技术4区
文献类型:
--
作者:
K. Unocic;V. Dagle;R. Dagle;Evan C. Wegener;J. Kropf;T. Krause;Daniel A. Ruddy;L. Allard;S. Habas

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1,3-丁二烯(C4H6或BD)用于制造各种合成橡胶、弹性体和聚合物树脂,产品包括轮胎、高尔夫球和乐高。BD的价格波动和对未来供应短缺的担忧促使人们寻找替代来源;从可再生乙醇中生产BD是一个有希望的选择[1]。开发了一种具有可裁剪的酸和金属中心的双功能催化剂,该催化剂对乙醇制取BD具有活性和选择性。最近发现,在氢气下操作时,会产生1-丁烯和2-丁烯的混合物,而不是BD;正丁烯可以用作燃料前体[2]。通过了解催化剂在反应条件下的稳定性和选择性,设想了乙醇选择性两步转化为喷气和柴油烷烃。本研究的目的是用扫描电子显微镜(S)和X射线吸收光谱(XAS)研究Ag/ZrO_2/SBA-16催化剂的结构-功能关系以及催化剂中的银分散体对催化剂性能的影响。
1,3-Butadiene (C4H6 or BD) is used for manufacturing a variety of synthetic rubbers, elastomers, and polymer resins, with products that include tires, golf balls, and Legos. BD price swings and concerns about future supply shortages have created an incentive to find alternative sources; producing BD from renewable ethanol is one promising option [1]. A bifunctional Ag/ZrO2/SBA-16 catalyst with tailored acid and metal sites that is both active and selective for the production of BD from ethanol has been developed [2]. It was recently discovered that when operating under hydrogen, a mixture of 1and 2-butenes are produced instead of BD; n-butenes can be used as fuel precursors [2]. By understanding the catalyst stability and selectivity under reaction conditions, a selective two-step conversion of ethanol to jetand diesel-range hydrocarbons is envisioned. The aim of this research is to determine the structure-function relationships of the Ag/ZrO2/SBA-16 catalyst and the role of Ag dispersions within the catalyst on performance using operando scanning transmission electron microscopy (S/TEM) and X-ray absorption spectroscopy (XAS).