High photocatalytic activity of Cu 2 O embedded in hierarchically hollow SiO 2 for efficient chemoselective hydrogenatio
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High photocatalytic activity of Cu2O embedded in hierarchically hollow SiO2 for efficient chemoselective hydrogenation of nitroarenes Zhengliang Yin1, Yingguan Xiao1, Xiong Wan1, Ying Jiang2, Gang Chen1,*, Qingye Shi1, and Shunsheng Cao1,* 1 2
Research School of Polymer Materials, School of Materials Science and Engineering, Jiangsu University, Zhenjiang 212013, China School of Water, Energy and Environment, Cranfield University, Bedford MK43 0AL, UK
Received: 18 June 2020
ABSTRACT
Accepted: 13 October 2020
Photocatalytic organic conversion is a crucial process in the hydrogenation of nitroarenes, but harsh reaction conditions such as long reaction time, high hydrogen pressure, and organic medium still need to be considerably overcome under visible-light irradiation. Here, we have constructed a transition metal oxide photocatalyst by embedding low-cost Cu2O with strong visible-light absorption into hierarchically hollow SiO2 sphere (SiO2-Cu2O@SiO2) that can suppress the escape of photogenerated atomic hydrogen and promote the contact probability between hydrogen atom and nitroarene molecules due to confinement effect. Remarkably, the SiO2-Cu2O@SiO2 photocatalyst can exhibit efficient chemoselectivity toward the hydrogenation of various nitroarenes in an aqueous system at ambient conditions, successfully working out the requirement of strict hydrogenation conditions, especially for organic medium over almost all of the reported photocatalysts. Notably, quantitative aniline can be produced for the visible-light catalytic reduction of nitroarenes, suggesting a considerable potential for industrial applications.
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Handling Editor: Joshua Tong.
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https://doi.org/10.1007/s10853-020-05449-x
J Mater Sci
GRAPHIC ABSTRACT
H2
Escape
Suppress the escape of H
Cu2O (2.1 eV)
Introduction The selective hydrogenation of nitroarenes over efficient catalysts is the method of choice for the production of anilines and their derivatives that are extremely important intermediates for the manufacture of chemicals, fuels, agrochemicals, and pharmaceuticals [1–4]. Although supported metal catalysts present efficient performance for the reduction of nitroarenes, the inevitable by-products severely limit their practical applications due to stepwise reduction of nitroarenes [4–6]. Furthermore, it is a big challenge to realize perfect chemoselectivity of nitroarene over most of the supported metal catalysts when a nitroarene molecule consists of one or more reducible groups (e.g., - OOH, - Cl, - C = O, etc.) [7, 8]. In particular, the reported heterogeneous catalysts simultaneously induce the undesirable elimination of these functional groups due to harsh reaction conditions such as high temperature or high hydrogen pressure [2, 4, 9–13], which subsequently affects downstream chemical synthesis processes. Therefore, it is of significant interest for commercial and academic research to construct
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