Design of a "green" one-step catalytic production of epsilon-caprolactam (precursor of nylon-6).

Abstract:

: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 A) aluminophosphates in which small fractions of the Al(III)O4(5-) and P(V)O4(3-) tetrahedra constituting the 4-connected open framework are replaced by Co(III)PO4(5-) and Si(IV)O4(4-) 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 approximately 80% for 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.

authors

Thomas JM,Raja R

doi

10.1073/pnas.0506907102

keywords:

subject

Has Abstract

pub_date

2005-09-27 00:00:00

pages

13732-6

issue

39

eissn

0027-8424

issn

1091-6490

pii

0506907102

journal_volume

102

pub_type

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