Probing Interactions of γ-Alumina with Water via Multinuclear Solid-State NMR Spectroscopy.

Probing Interactions of γ-Alumina with Water via Multinuclear Solid-State NMR Spectroscopy.
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通过多核固态核磁共振波谱探测 γ-氧化铝与水的相互作用

DOI:
10.1002/cctc.201901838
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发表时间:
2020-03-19
期刊:
影响因子:
4.5
通讯作者:
Peng L
Peng L
中科院分区:
化学3区
文献类型:
--
作者:
Shen L;Wang Y;Du JH;Chen K;Lin Z;Wen Y;Hung I;Gan Z;Peng L

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γ-Al_2O_3与水的相互作用是控制其结构和催化性能的重要因素。我们应用固态多核NMR光谱,通过实时监测1H和17 O光谱来研究这种相互作用。表面选择性检测是通过将富含17 O的水吸附在γ-氧化铝纳米棒上来实现的。用~ 1H/~(17)O双共振核磁共振和~(27)Al核磁共振在~ 35.2T磁场下选择性地探测了表面的结构演化。在纳米棒表面上的羟基物质的形成是快速的,当暴露于水时,其涉及首先产生具有双桥接和隔离羟基物质的低配位铝离子。水分子中的氧原子与裸露表面位点之间发生快速交换,表明这些氧物种的高反应性。这些结果为研究γ-Al 2 O3表面的结构和动力学提供了新的思路,所采用的方法也可推广到研究其它氧化物与水的相互作用。
Interaction of γ-alumina with water are important in controlling its structure and catalytic properties. We apply solid-state multinuclear NMR spectroscopy to investigate this interaction by monitoring 1H and 17O spectra in real-time. Surface-selective detection is made possible by adsorbing 17O-enriched water on γ-alumina nanorods. Structural evolution on the surface was selectively probed by 1H/17O double resonance NMR and 27Al NMR at ultrahigh 35.2 T magnetic field. Formation of hydroxyl species on the surface of nanorods is rapid upon the exposure of water, which involves low coordinated aluminum ions with doubly bridging and isolated hydroxyl species being generated first. Fast exchange occurs between oxygen atoms in the water molecules and bare surface sites, indicating high reactivity of these oxygen species. These results provide new insights into the structure and dynamics on the surface of γ-alumina and the methods applied here can be extended to study the interaction of other oxides with water.
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