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Morphology‐Reserved Synthesis of Discrete Nanosheets of CuO@SAPO‐34 and Pore Mouth Catalysis for One‐Pot Oxidation of Cyclohexane
Author(s) -
Guo Xiangke,
Xu Mengxia,
She Minyi,
Zhu Yan,
Shi Taotao,
Chen Zhaoxu,
Peng Luming,
Guo Xuefeng,
Lin Ming,
Ding Weiping
Publication year - 2020
Publication title -
angewandte chemie international edition
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.831
H-Index - 550
eISSN - 1521-3773
pISSN - 1433-7851
DOI - 10.1002/anie.201911749
Subject(s) - cyclohexane , catalysis , molecular sieve , lamellar structure , oxide , chemical engineering , materials science , adipic acid , copper oxide , morphology (biology) , copper , inorganic chemistry , chemistry , polymer chemistry , organic chemistry , composite material , metallurgy , biology , engineering , genetics
Abstract Discrete nanosheets of silicon‐doped AlPO 4 molecular sieves (SAPO‐34) with a thickness of ≈7 nm have been prepared through morphology‐reserved synthesis with a lamellar aluminum phosphate as precursor. Cages of the nanosheets are in situ incorporated with copper oxide clusters. The CuO@SAPO‐34 nanosheets exhibit a large external surface area with a high number of (010) channel pores on the surface. Due to the thin morphology, copper oxide clusters occupy the outmost cages with a probability >50 %. The distinctive configuration facilitates a new concept of pore mouth catalysis, i.e., reactant molecules larger than the pores cannot enter the interior of the molecular sieves but can interact with the CuO clusters at “the mouth” of the pore. In heterogeneous catalysis, CuO@SAPO‐34 nanosheets have shown top performance in one‐pot oxidation of cyclohexane to adipic acid by O 2 , a key compound for the manufacture of nylon‐66, which is so far produced using non‐green nitric acid oxidation.