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Research Article

3D printed hierarchical spinel monolithic catalysts for highly efficient semi-hydrogenation of acetylene

Zijian Yuan1,2Lu Liu1Wei Ru1,3Daojin Zhou1( )Yun Kuang1Junting Feng1,3( )Bin Liu2( )Xiaoming Sun1( )
State Key Laboratory of Chemical Resource Engineering, College of Chemistry, Beijing University of Chemical Technology, Beijing 100029, China
School of Chemical and Biomedical Engineering, Nanyang Technological University, 62 Nanyang Drive, Singapore 637459, Singapore
Beijing Engineering Center for Hierarchical Catalysts, Beijing University of Chemical Technology, Beijing 100029, China
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Graphical Abstract

The aluminate intercalation into Al3+-containing layered double hydroxide (LDH) enabled the phase-pure spinel formation at a low temperature with consolidated architecture and high specific surface area. Moreover, three-dimensional (3D) printed spinel monolithic catalysts from the precursor with hierarchical pores at both the macro- and microscale facilitated chemicals and heat diffusion, resulting in high activity, excellent selectivity as well as long-term stability for semi-hydrogenation of acetylene to ethylene.


Porous monolithic catalysts with high specific surface areas, which can not only facilitate heat/mass transfer, but also help to expose active sites, are highly desired in strongly exothermic or endothermic gas–solid phase reactions. In this work, hierarchical spinel monolithic catalysts with a porous woodpile architecture were fabricated via extrusion-based three-dimensional (3D) printing (direct ink writing, DIW in brief) of aluminate-intercalated layered double hydroxide (AI-LDH) followed by low temperature calcination. The intercalation of aluminate in LDH is found crucial to tailor the M2+/Al3+ ratio, integrate LDH nanosheets into monolithic catalyst, and enable the conversion of LDH to spinel at the temperature as low as 500 °C with high specific surface areas (> 350 m2/g). The rapid mass/heat transfer resulted from the versatile 3D network at macroscale and the highly dispersed and fully exposed active sites benefited from the porous structure at microscale endow the 3D-printed Pd loaded spinel MgAl-mixed metal oxide (3D-AI-Pd/MMO) catalyst with excellent catalytic performance in semi-hydrogenation of acetylene, achieving 100% conversion at 60 °C with more than 84% ethylene selectivity.

Electronic Supplementary Material

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12274_2022_4291_MOESM1_ESM.pdf (2.5 MB)
Nano Research
Pages 6010-6018
Cite this article:
Yuan Z, Liu L, Ru W, et al. 3D printed hierarchical spinel monolithic catalysts for highly efficient semi-hydrogenation of acetylene. Nano Research, 2022, 15(7): 6010-6018.






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Received: 06 February 2022
Revised: 01 March 2022
Accepted: 03 March 2022
Published: 25 April 2022
© Tsinghua University Press 2022