Efficient adjustment of product selectivity using controllable Pd nanoparticles in nitroarene hydrogenation--颗粒学报PARTICUOLOGY

Zhang, J., Wang, L., Chen, F., & Xiao, F.-S. (2020). Efficient adjustment of product selectivity using controllable Pd nanoparticles in nitroarene hydrogenation. Particuology, 48, 13-18. https://doi.org/10.1016/j.partic.2018.08.011

Efficient adjustment of product selectivity using controllable Pd nanoparticles in nitroarene hydrogenation

Jian Zhang, Liang Wang, Fang Chen ^*, Feng-Shou Xiao ^*

Key Laboratory of Applied Chemistry of Zhejiang Province and Department of Chemistry, Zhejiang University, Hangzhou 310028, China

10.1016/j.partic.2018.08.011

Volume 48, February 2020, Pages 13-18

Received 17 May 2018, Revised 14 August 2018, Accepted 29 August 2018, Available online 28 March 2019, Version of Record 27 January 2020.

E-mail: kenobi@163.com; fsxiao@zju.edu.cn

Highlights

• Pd nanoparticles were rationally controlled on or inside zeolite crystals.

• Pd location affected the catalytic performance in nitroarene hydrogenation.

• Different catalytic performances were due to different Pd–reactant interactions.

• Catalyst stacking manner strongly influenced the catalytic performance.

• Catalyst stacking manner was related to Pd–reactant interaction.

Abstract

Product selectivity adjustment is a much-studied topic in mesoscience that is critical for industrial processes and strongly related to reaction intermediates formed by interactions between catalytic active sites and reactants. Herein, we report efficient adjustment of the product selectivity in the hydrogenation of substituted nitroarenes via rational reaction intermediates achieved using controllable Pd nanoparticles. Pd nanoparticles fixed within zeolite Beta crystals (Pd@Beta) afforded rational Pd–NO₂ interactions, in which the Pd nanoparticle-adsorbed substituted nitroarenes, such as nitrobenzaldehyde, were reasonably hydrogenated into the corresponding aminobenzaldehyde. However, for Pd nanoparticles supported on the external surfaces of zeolite beta crystals, various side products were obtained owing to the coexistence of Pd–NO₂ and Pd–C=O interactions. When Pd nanoparticles were artificially controlled in various positions in a fixed-bed reactor, the product selectivity was significantly affected. These results demonstrate the importance of molecular adsorption and diffusion processes in adjusting product selectivity in catalytic reactions.

Graphical abstract

Keywords

Product selectivity; Nitroarene hydrogenation; Pd nanoparticles; Zeolite crystals

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