4.8 Article

Strong Lewis Base Ga4B2O9: Ga-O Connectivity Enhanced Basicity and Its Applications in the Strecker Reaction and Catalytic Conversion of n-Propanol

Journal

ACS APPLIED MATERIALS & INTERFACES
Volume 10, Issue 18, Pages 15895-15904

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsami.8b04144

Keywords

structure properties relationships; solid bases catalysis; Lewis base sites location; heterogeneously catalyzed Strecker reaction; n-propanol catalytic conversion; gallium borates

Funding

  1. National Natural Science Foundation of China [91222106, 21671028, 21771027]
  2. Natural Science Foundation of Chongqing [CSTC 2014jcyjA50036, 2016jcyjA0291]

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Heterogeneous solid base catalysis is valuable and promising in chemical industry, however it is insufficiently developed compared to solid acid catalysis due to the lack of satisfied solid base catalysts. To gain the strong basicity, the previous strategy was to basify oxides with alkaline metals to create surficial vacancies or defects, which suffers from the instability under catalytic conditions. Monocomponent basic oxides like MgO are literally stable but deficient in electron-with drawing ability. Here we prove that a special connectivity of atoms could enhance the Lewis basicity of oxygen in monocomponent solids exemplified by Ga4B2O9. The structure-induced basicity is from the mu(3)-O linked exclusively to five-coordinated Ga3+center dot Ga4B2O9 behaved as a durable catalyst with a high yield of 81% in the base-catalyzed synthesis of aaminonitriles by Strecker reaction. In addition, several monocomponent solid bases were evaluated in the Strecker reaction, and Ga4B2O9 has the largest amount of strong base centers (23.1 mu mol/g) and the highest catalytic efficiency. Ga4B2O9 is also applicable in hightemperature solid-gas catalysis, for example, Ga4B2O9 catalyzed efficiently the dehydrogenation of n-propanol, resulting in a high selectivity to propanal (79%). In contrast, the comparison gallium borate, Ga-PKU-1, which is a Bronsted acid, preferred to catalyze the dehydration process to obtain propylene with a selectivity of 94%.

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