Effects of calcination temperatures on CH<sub>4</sub>-CO<sub>2</sub> two stepwise conversion to acetic acid over Pd/LDH catalysts

WANG Xiaoshuang; WU Yixiao; WANG Fei; ZHANG Kaiwei; LIU Yongjun; HUANG Wei

doi:10.12434/j.issn.2097-2547.20250140

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Effects of calcination temperatures on CH₄-CO₂ two stepwise conversion to acetic acid over Pd/LDH catalysts

更新时间：2025-08-25

- Effects of calcination temperatures on CH₄-CO₂ two stepwise conversion to acetic acid over Pd/LDH catalysts
- Vol. 50, Issue 8, Pages: 123-132(2025)
- 作者机构：
  
  1.太原理工大学省部共建煤基能源清洁高效利用国家重点实验室，山西太原 030024
  2.太原理工大学化学与化工学院，山西太原 030024
  3.新疆智能装备研究院，新疆阿克苏 831399
- 作者简介：
- 基金信息：
- DOI：10.12434/j.issn.2097-2547.20250140
  CLC： TQ426;O643.36
- Received：27 March 2025，
  
  Revised：16 April 2025，
  
  Published：25 August 2025
- 稿件说明：
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王小双,吴怡枭,王菲等.焙烧温度对Pd/LDH催化剂上CH₄-CO₂两步梯阶转化合成乙酸的影响[J].低碳化学与化工,2025,50(8):123-132.

WANG Xiaoshuang,WU Yixiao,WANG Fei,et al.Effects of calcination temperatures on CH₄-CO₂ two stepwise conversion to acetic acid over Pd/LDH catalysts[J].Low-Carbon Chemistry and Chemical Engineering,2025,50(8):123-132.
王小双,吴怡枭,王菲等.焙烧温度对Pd/LDH催化剂上CH₄-CO₂两步梯阶转化合成乙酸的影响[J].低碳化学与化工,2025,50(8):123-132. DOI： 10.12434/j.issn.2097-2547.20250140.

WANG Xiaoshuang,WU Yixiao,WANG Fei,et al.Effects of calcination temperatures on CH₄-CO₂ two stepwise conversion to acetic acid over Pd/LDH catalysts[J].Low-Carbon Chemistry and Chemical Engineering,2025,50(8):123-132. DOI： 10.12434/j.issn.2097-2547.20250140.

摘要

和CO

直接转化为乙酸是一种100%原子经济性的反应，但其反应条件较苛刻。水滑石（LDH）因具有比表面积大、活性组分分散性好和酸碱性可调等优点，在CH

-CO

催化转化领域具有良好的应用前景。以

(Mg)/

(Al)为5的MgAl-LDH为载体，采用离子交换法负载质量分数为5%的钯（Pd）作为活性组分，将所得前驱体在不同温度下进行焙烧制得了一系列Pd/LDH-X催化剂（X代表焙烧温度）。采用XRD、FT-IR和SEM等对催化剂的结构进行了表征，并研究了催化剂在CH

-CO

两步梯阶转化合成乙酸过程中的催化性能。结果表明，在本研究设定的CH

-CO

两步梯阶转化反应条件下反应30 min，150 ℃下焙烧所得Pd/LDH-150的催化性能最优，其乙酸时空收率为61.8 μmol/(g·h)，明显优于CH

-CO

共进料条件下的乙酸时空收率（2.4 μmol/(g·h)），且乙酸是唯一的液体产物。LDH的结构完整性是影响催化剂催化性能的关键因素，催化剂表面存在较多的中强酸性位点和中强碱性位点有利于乙酸的合成。焙烧温度过高会导致LDH的层状结构坍塌，造成表面中强酸性位点和中强碱性位点数量减少，从而对催化剂的催化性能产生不利影响。

Abstract

The direct conversion of CH

and CO

to acetic acid is a 100% atom-economical reaction

but its reaction conditions are harsh. The hydrotalcite (LDH) has good application prospects in the field of CH

-CO

catalytic conversion due to its advantages of large specific surface area

good dispersion for active components and adjustable acid-base properties. MgAl-LDH with

(Mg)/

(Al) of 5 was used as the support

and palladium (Pd) with mass fraction of 5% was loaded as the active component by ion-exchange method

and a series of Pd/LDH-X catalysts (X represents the calcinatio

n temperature) were prepared by calcinating the resultant precursors at different temperatures. The structures of catalysts were characterized by XRD

FT-IR

SEM

etc.

and the catalytic performances of the catalysts were investigated in two-step stepwise conversion of CH

-CO

to acetic acid. The results show that the catalytic performance of Pd/LDH-150 obtained under calcination temperature of 150 ℃ is the best under the CH

-CO

two-step stepwise conversion reaction conditions set in this study for 30 min

with acetic acid spatiotemporal yield of 61.8 μmol/(g·h)

which is significantly greater than acetic acid spatiotemporal yield (2.4 μmol/(g·h)) under the CH

-CO

cofeeding conditions

and acetic acid is the only liquid product. The structural integrity of LDH is a key factor affecting the catalytic performance of the catalyst

and the presence of more medium-strong acidic sites and medium-strong basic sites on the surface of catalyst is favorable for the synthesis of acetic acid. Excessively high calcination temperature can lead to the collapse of the layered structure of LDH

resulting in the decrease of the number of medium-strong acidic sites and medium-strong basic sites on the surface

which can adversely affect the catalytic performance of the catalyst.

关键词

Keywords

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Effects of calcination temperatures on CH4-CO2 two stepwise conversion to acetic acid over Pd/LDH catalysts

DOI：10.12434/j.issn.2097-2547.20250140

摘要

Abstract

关键词

Keywords

references

Effects of calcination temperatures on CH₄-CO₂ two stepwise conversion to acetic acid over Pd/LDH catalysts