Accelerating syngas-to-aromatic conversion via spontaneously monodispersed Fe in ZnCr2O4 spinel

Guo Tian, Xinyan Liu, Chenxi Zhang (), Xiaoyu Fan, Hao Xiong, Xiao Chen (), Zhengwen Li, Binhang Yan, Lan Zhang, Ning Wang, Hong-Jie Peng () and Fei Wei ()
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Guo Tian: Tsinghua University
Xinyan Liu: University of Electronic Science and Technology of China
Chenxi Zhang: Tsinghua University
Xiaoyu Fan: Tsinghua University
Hao Xiong: Tsinghua University
Xiao Chen: Tsinghua University
Zhengwen Li: Tsinghua University
Binhang Yan: Tsinghua University
Lan Zhang: Beijing University of Technology
Ning Wang: Beijing University of Technology
Hong-Jie Peng: University of Electronic Science and Technology of China
Fei Wei: Tsinghua University

Nature Communications, 2022, vol. 13, issue 1, 1-11

Abstract: Abstract Spontaneous monodispersion of reducible active species (e.g., Fe, Co) and their stabilization in reductive atmospheres remain a key challenge in catalytic syngas chemistry. In this study, we present a series of catalysts including spontaneously monodispersed and enriched Fe on ZnCr2O4. Deep investigation shows remarkable performance in the syngas-to-aromatic reaction only when monodispersed Fe coupled with a H-ZSM-5 zeolite. Monodispersed Fe increases the turnover frequency from 0.14 to 0.48 s−1 without sacrificing the record high selectivity of total aromatics (80–90%) at a single pass. The increased activity is ascribed to more efficient activation of CO and H2 at oxygen vacancy nearest to the isolated Fe site and the prevention of carbide formation. Atomic precise characterization and theoretical calculations shed light on the origin and implications of spontaneous Fe monodispersion, which provide guidance to the design of next-generation catalyst for upgrading small molecules to synthetic fuels and chemicals.

Date: 2022
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DOI: 10.1038/s41467-022-33217-9

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