氧空穴ZrO<sub>2</sub>复合CuFe催化剂合成气制高级醇反应性能研究

徐浩浩; 穆晓亮; 房克功; 宋江锋

doi:10.12434/j.issn.2097-2547.20240169

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氧空穴ZrO₂复合CuFe催化剂合成气制高级醇反应性能研究

C1化学与催化转化

- 氧空穴ZrO₂复合CuFe催化剂合成气制高级醇反应性能研究
- Study on reaction performances of oxygen-vacancies ZrO₂ composite CuFe catalysts for syngas to higher alcohols
- 低碳化学与化工 2024, 49(10): 11-19.
- 作者机构：
  
  1.中北大学化学与化工学院，山西太原 030051
  2.中国科学院山西煤炭化学研究所煤炭高效低碳利用全国重点实验室，山西太原 030001
- 作者简介：
  
  徐浩浩（1999—），硕士研究生，研究方向为C1化学，E-mail：1138274265@qq.com。
  房克功（1975—），博士，研究员，研究方向为C1化学，E-mail：kgfang@sxicc.ac.cn；
  宋江锋（1978—），博士，教授，研究方向为无机化学，E-mail：jfsong0129@ nuc.edu.cn。
- 基金信息：
  
  国家重点研发计划(2023YFB4103202);国家自然科学基金面上项目(22179137)
- DOI：10.12434/j.issn.2097-2547.20240169
  中图分类号： TQ223.1;O643.3
- 纸质出版日期：2024-10-25，
  
  收稿日期：2024-04-19，
  
  修回日期：2024-05-05，
- 稿件说明：
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徐浩浩,穆晓亮,房克功等.氧空穴ZrO₂复合CuFe催化剂合成气制高级醇反应性能研究[J].低碳化学与化工,2024,49(10):11-19.

XU Haohao,MU Xiaoliang,FANG Kegong,et al.Study on reaction performances of oxygen-vacancies ZrO₂ composite CuFe catalysts for syngas to higher alcohols[J].Low-carbon Chemistry and Chemical Engineering,2024,49(10):11-19.
徐浩浩,穆晓亮,房克功等.氧空穴ZrO₂复合CuFe催化剂合成气制高级醇反应性能研究[J].低碳化学与化工,2024,49(10):11-19. DOI： 10.12434/j.issn.2097-2547.20240169.

XU Haohao,MU Xiaoliang,FANG Kegong,et al.Study on reaction performances of oxygen-vacancies ZrO₂ composite CuFe catalysts for syngas to higher alcohols[J].Low-carbon Chemistry and Chemical Engineering,2024,49(10):11-19. DOI： 10.12434/j.issn.2097-2547.20240169.

摘要

合成气制高级醇具有重要的现实意义，催化剂的构建是合成气制高级醇技术的关键。分别采用碳酸钠共沉淀法和草酸凝胶沉淀法制得CuFe和富含氧空穴氧化锆（ZrO

-OV）组分，并将两者物理研磨混合制备了一系列复合催化剂CF-Z-

（其中CF、Z和

分别代表CuFe、ZrO

-OV和两者质量比），该复合催化剂CF-Z-

可有效提高醇产物中高级醇分布。采用EPR、N

吸/脱附、XRD、TEM、XPS、H

-TPR和CO-TPSR-MS等手段表征了催化剂的物理化学性质，并考察了催化剂催化合成气转化制备高级醇的反应性能。结果表明，富含氧空穴ZrO

可促进CO活化。富含氧空穴ZrO

与CuFe催化剂物理混合后，在复合催化剂CF-Z-

的表面形成了高碳贫氢的化学环境，能促进CO的转化和高级醇的生成。复合催化剂CF-Z-

的催化性能可通过调变

值来进行优化。在260 ℃、5 MPa和空速为4000 h

-1

的反应条件下，CF-Z-8催化剂的CO转化率为23.5%，总醇选择性为15.0%，其中高级醇质量占比可达96.1%。

Abstract

The synthesis of higher alcohols from syngas is of great practical importance

and the construction of catalysts is the key to this technology. CuFe and zirconia with rich oxygen vacancies components (ZrO

-OV) were prepared by sodium carbonate co-precipitation and oxalic acid gel precipitation

respectively. A series of composite catalysts CF-Z-

(CF

Z and

stand for CuFe

ZrO

-OV and the mass ratio of the two

respectively) were prepared by physically milling and mixing the two components. The series of catalysts can effectively improve the distribution of higher alcohols in alcohol products. The physicochemical properties of the catalysts were characterized by EPR

adsorption/desorption

XRD

TEM

XPS

-TPR and CO-TPSR-MS

and the reaction performances of the catalysts for preparation of higher alcohols by syngas catalytic reforming was investigated. The results show that ZrO

with rich oxygen vacancies promotes CO activation. After physically mixing ZrO

with rich oxygen vacancies and CuFe catalyst

a high-carbon and hydrogen-poor chemical environment is formed on the catalyst surface

which facilitates the conversion of CO and generation of higher alcohols. The catalytic performance of the composite catalyst can be optimized by varying

values. Under the reaction conditions of 260 ℃

5 MPa and space velocity of 4000 h

-1

the CO conversion rate of CF-Z-8 is 23.5%

the selectivity of total alcohols of CF-Z-8 is 15.0%

and the mass proportion of higher alcohols can reach 96.1%.

关键词

CuFe催化剂氧空穴ZrO2合成气高级醇

Keywords

CuFe catalystsoxygen vacanciesZrO2syngashigher alcohols

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氧空穴ZrO2复合CuFe催化剂合成气制高级醇反应性能研究

Study on reaction performances of oxygen-vacancies ZrO2 composite CuFe catalysts for syngas to higher alcohols

DOI：10.12434/j.issn.2097-2547.20240169

摘要

Abstract

关键词

Keywords

references

氧空穴ZrO₂复合CuFe催化剂合成气制高级醇反应性能研究

Study on reaction performances of oxygen-vacancies ZrO₂ composite CuFe catalysts for syngas to higher alcohols