Tuning the crystallite size of monoclinic ZrO2 to reveal critical roles of surface defects on m-ZrO2 catalyst for direct synthesis of isobutene from syngas

Xuemei Wu; Minghui Tan; Bing Xu; Shengying Zhao; Qingxiang Ma; Yingluo He; Chunyang Zeng; Guohui Yang; Noritatsu Tsubaki; Yisheng Tan

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Tuning the crystallite size of monoclinic ZrO₂ to reveal critical roles of surface defects on m-ZrO₂ catalyst for direct synthesis of isobutene from syngas

Catalysis, Kinetics and Reaction Engineering | Updated：2026-01-06

- Tuning the crystallite size of monoclinic ZrO₂ to reveal critical roles of surface defects on m-ZrO₂ catalyst for direct synthesis of isobutene from syngas
- Tuning the crystallite size of monoclinic ZrO₂ to reveal critical roles of surface defects on m-ZrO₂ catalyst for direct synthesis of isobutene from syngas
- 中国化学工程学报（英文版） 2021年35卷第7期页码：211-219
- Affiliations：
  
  1. State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences,Taiyuan,China,030001
  2. University of Chinese Academy of Sciences,Beijing,China,100049
  3. State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering, Ningxia University,Yinchuan,China,750021
  4. Department of Applied Chemistry, School of Engineering, University of Toyama, Gofuku 3190,Toyama,Japan,930-8555
  5. China Petroleum Chemical Industry Federation,Beijing,China,100723
- Author bio：
- Funds：
- DOI：
  中图分类号：
- 纸质出版：2021
- Accepted：
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Xuemei Wu, Minghui Tan, Bing Xu, 等. Tuning the crystallite size of monoclinic ZrO₂ to reveal critical roles of surface defects on m-ZrO₂ catalyst for direct synthesis of isobutene from syngas[J]. 中国化学工程学报（英文版）, 2021,35(7):211-219.

to reveal critical roles of surface defects on
Xuemei Wu, Minghui Tan, Bing Xu, 等. Tuning the crystallite size of monoclinic ZrO₂ to reveal critical roles of surface defects on m-ZrO₂ catalyst for direct synthesis of isobutene from syngas[J]. 中国化学工程学报（英文版）, 2021,35(7):211-219. DOI：

to reveal critical roles of surface defects on DOI：

摘要

Abstract

The effects of crystallite size on the physicochemical properties and surface defects of pure monoclinic ZrO

catalysts for isobutene synthesis were studied. We prepared a series of monoclinic ZrO

catalysts with different crystallite size by changing calcination temperature and evaluated their catalytic performance for isobutene synthesis from syngas. ZrO

with small crystalline size showed higher CO conversion and isobutene selectivity

while samples with large crystalline size preferred to form dimethyl ether (DME) instead of hydrocarbons

much less to isobutene. Oxygen defects (O

Defects

) analyzed by X-ray photoelectron spectroscopy (XPS) provided evidence that more O

Defects

occupied on the surface of ZrO

catalysts with smaller crystalline size. Electron paramagnetic resonance (EPR) and ultraviolet-visible diffuse reflectance (UV-vis DRS) confirmed the presence of high concentration of surface defects and Zr

-ZrO

-5.9 sample

respectively.

In situ

diffuse reflectance infrared

Fourier transform spectroscopy (

in situ

DRIFTS) analysis indicated that the adsorption strength of formed formate species on catalyst reduced as the crystalline size decreased. These results suggested that surface defects were responsible for CO activation and further influenced the adsorption strength of surface species

and thus the products distribution changed. This study provides an in-depth insight for active sites regulation of ZrO

catalyst in CO hydrogenation reaction.

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