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Pt x 负载沸石 NaY 中受阻路易斯对的形成。

Formation of Frustrated Lewis Pairs in Ptx -Loaded Zeolite NaY.

机构信息

Neutron Science Division, Korea Atomic Energy Research Institute, 989-111, Daedeokdaero, Yuseong-gu, Daejeon (Korea).

Department of Physics, Sogang University, 35, Baekbumro, Mapo-gu, Seoul (Korea).

出版信息

Angew Chem Int Ed Engl. 2015 Oct 26;54(44):13080-4. doi: 10.1002/anie.201506790. Epub 2015 Sep 7.

Abstract

The formation of a frustrated Lewis pair consisting of sodium hydride (Na(+) H(-) ) and a framework-bound hydroxy proton O(H(+) ) is reported upon H2 treatment of zeolite NaY loaded with Pt nanoparticles (Ptx /NaY). Frustrated Lewis pair formation was confirmed using in situ neutron diffraction and spectroscopic measurements. The activity of the intrazeolite NaH as a size-selective catalyst was verified by the efficient esterification of acetaldehyde (a small aldehyde) to form the corresponding ester ethyl acetate, whereas esterification of the larger molecule benzaldehyde was unsuccessful. The frustrated Lewis pair (consisting of Na(+) H(-) and O(H(+) )) generated within zeolite NaY may be a useful catalyst for various catalytic reactions which require both H(-) and H(+) ions, such as catalytic hydrogenation or dehydrogenation of organic compounds and activation of small molecules.

摘要

报道了在负载 Pt 纳米粒子(Ptx/NaY)的沸石 NaY 经 H2 处理后形成由氢化钠(Na(+) H(-))和骨架结合的羟基质子 O(H(+))组成的受阻路易斯对。通过原位中子衍射和光谱测量证实了受阻路易斯对的形成。通过将乙醛(一种小醛)高效酯化形成相应的乙酯乙基乙酸酯,验证了沸石内 NaH 的活性作为尺寸选择性催化剂,而较大分子苯甲醛的酯化则不成功。在沸石 NaY 内生成的受阻路易斯对(由 Na(+) H(-) 和 O(H(+))组成)可能是用于需要 H(-)和 H(+)离子的各种催化反应的有用催化剂,例如有机化合物的催化加氢或脱氢以及小分子的活化。

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