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首页> 外文期刊>Proceedings of the National Academy of Sciences of the United States of America >Design of a 'green' one-step catalytic production of epsilon-caprolactam (precursor of nylon-6)
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Design of a 'green' one-step catalytic production of epsilon-caprolactam (precursor of nylon-6)

机译：ε-己内酰胺（尼龙6的前体）“绿色”一步催化生产的设计

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摘要

The ever-increasing industrial demand for nylon-6 (polycaprolactam) necessitates the development of environmentally benign methods of producing its precursor, epsilon-caprolactam, from cyclohexanone. It is currently manufactured in two popular double-step processes, each of which uses highly aggressive reagents, and each generates substantial quantities of largely unwanted ammonium sulfate as by-product. Here we describe a viable laboratory-scale, single-step, solvent-free process of producing epsilon-caprolactam using a family of designed bifunctional, heterogeneous, nanoporous catalysts containing isolated acidic and redox sites, which smoothly convert cyclohexanone to epsilon-caprolactam with selectivities in the range 65-78% in air and ammonia at 80 degrees C. The catalysts are microporous (pore diameter 7.3 angstrom) aluminophosphates in which small fractions of the (AlO45-)-O-vertical bar vertical bar vertical bar and p(v)O(4)(3-) tetrahedra constituting the 4-connected open framework are replaced by (CoPO45-)-P-vertical bar vertical bar vertical bar and (SiO44-)-O-IV tetrahedra, which become the loci of the redox and acidic centers, respectively. The catalysts may be further optimized, and already may be so designed as to generate selectivities of approximate to 80% or the intermediate oxime, formed from NH2OH, which is produced in situ within the pore system. The advantages of such designed heterogeneous catalysts, and their application to a range of other chemical conversions, are also adumbrated.
机译：工业上对尼龙-6（聚己内酰胺）的需求不断增长，因此需要开发从环己酮生产其前体ε-己内酰胺的环境友好方法。目前，它是通过两种流行的双步工艺制造的，每个工艺都使用高度侵蚀性的试剂，并且每个工艺都会产生大量副产品大量不需要的硫酸铵。在这里，我们描述了一种可行的实验室规模，单步，无溶剂的生产ε-己内酰胺的方法，该工艺使用一系列设计的双功能，均相，纳米孔催化剂，该催化剂包含分离的酸性和氧化还原位点，可将环己酮以选择性选择性平稳地转化为ε-己内酰胺在80°C的空气和氨中浓度范围为65-78％。催化剂是微孔（孔径7.3埃）铝磷酸盐，其中小部分（AlO45-）-O-垂直棒，垂直棒和p（v构成4连接的开放框架的（O）（4）（3-）四面体被（CoPO45-）-P垂直条垂直条和（SiO44-）-O-IV四面体取代，它们成为氧化还原和酸性中心。可以进一步优化催化剂，并且可以将催化剂设计成产生约80％的选择性，或者生成由NH2OH形成的中间体肟，后者在孔隙系统中就地产生。还设计了这种设计的非均相催化剂的优点及其在一系列其他化学转化中的应用。

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