Selective formation of propan-1-ol from propylene via a chemical looping approach

Selective formation of propan-1-ol from propylene via a chemical looping approach
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通过化学循环方法从丙烯选择性形成 1-丙醇

DOI:
10.1039/d2re00222a
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发表时间:
2022
影响因子:
3.9
通讯作者:
Harrison A
Harrison A
中科院分区:
化学2区
文献类型:
--
作者:
Harrison A

文献摘要

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研究了以丙烯为原料生产丙烷-1-醇的一种新的化学环路方法。以−δ钙钛矿为催化剂载体,制备了银基和金基催化剂,并用X射线衍射仪、扫描电子显微镜和X射线光电子能谱对其进行了表征。催化剂颗粒用于在填充床反应器中进行的实验,通过在材料上传递5vol%的丙烯来生成氧化产物,并通过还原催化剂载体SrFeO_3−δ来提供氧气。随后,固体颗粒在单独的步骤中与空气再次氧化,关闭了化学循环。以−δ为载体的AgC l和AgAu合金催化剂在2 60~30 0℃温度范围内对丙烷-1-醇有高达70-80%的稳定选择性,尽管丙烯转化率较低(∼为0.5-1.5%),但几乎没有生成仲醇。讨论了在化学环条件下,丙烷-1-醇通过环氧丙烷或烯丙醇中间体生成的假设机理。
A novel chemical looping approach for propan-1-ol production from propylene was investigated. Silver- and gold-based catalysts were prepared, with SrFeO3−δ perovskite as a catalyst support, and characterised using X-ray diffraction (XRD), electron microscopy (SEM and STEM-EDS), and X-ray photoelectron spectroscopy (XPS). Particles of the catalysts were used in experiments carried out in a packed bed reactor, by passing 5 vol% propylene over the material to generate oxygenated products, with oxygen provided via reduction of the catalyst support, SrFeO3−δ. The solid particles were subsequently re-oxidised with air in a separate step, closing the chemical loop. Catalysts composed of AgCl and AgAu alloy supported on SrFeO3−δ gave up to 70–80% stable selectivity towards propan-1-ol over the temperature range 260–300 °C, with little to no formation of the secondary alcohol, propan-2-ol, albeit at low propylene conversion (∼0.5–1.5%). Postulated mechanisms for propan-1-ol formation under chemical looping conditions are discussed, via propylene oxide or allyl alcohol intermediates.