Citation: Lina Guo, Ruizhe Li, Chuang Sun, Xiaoli Luo, Yiqiu Shi, Hong Yuan, Shuxin Ouyang, Tierui Zhang. 层状双金属氢氧化物的层间阴离子对衍生的Ni-Al₂O₃催化剂光热催化CO₂甲烷化反应的影响[J]. Acta Physico-Chimica Sinica, ;2025, 41(1): 230900. doi: 10.3866/PKU.WHXB202309002 shu

层状双金属氢氧化物的层间阴离子对衍生的Ni-Al₂O₃催化剂光热催化CO₂甲烷化反应的影响

Lina Guo ¹ ,
Ruizhe Li ¹ ,
Chuang Sun ¹ ,
Xiaoli Luo ¹ ,
Yiqiu Shi ¹ ,
Hong Yuan ^1,, ,
Shuxin Ouyang ^1,, ,
Tierui Zhang ^2,,

1.
Engineering Research Center of Photoenergy Utilization for Pollution Control and Carbon Reduction, Ministry of Education;Key Laboratory of Pesticide and Chemical Biology of Ministry of Education, College of Chemistry, Central China Normal University, Wuhan 430079, China;
2.
Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Beijing 100190, China

Corresponding author: Hong Yuan, Shuxin Ouyang, Tierui Zhang,
Received Date: 1 September 2023
Revised Date: 6 October 2023
Accepted Date: 19 October 2023

Fund Project: The project was supported by the National Natural Science Foundation of China (21972052, 22272061) and Foundation Project of Hubei Key Laboratory of Radiation Chemistry and Functional Materials (2021KF01).

太阳能驱动的二氧化碳(CO₂)甲烷化反应不仅有助于减少多余的碳排放，而且是生产燃料的重要途径。层状金属双氢氧化物(layered double hydroxides，LDH)可以在高温还原气(H₂/Ar)氛围中还原，转化为金属负载于氧化物(MO)的催化剂。这些催化剂在CO₂加氢反应中作为优秀的光热催化剂被广泛应用。然而，有关LDH的层间阴离子类型如何影响CO₂甲烷化活性的研究还相对有限。本文研究了包含不同层间阴离子的镍(Ni)铝(Al) LDH前驱体，通过在H₂/Ar气氛中还原处理，制备了一系列Ni负载在氧化铝(Al₂O₃)上的MO催化剂，这些催化剂被命名为NiAl-x-MO (其中x代表CO₃、NO₃、Cl和SO₄，分别代表碳酸根、硝酸根、氯离子和硫酸根等阴离子)。其中，NiAl-CO₃-MO催化剂表现出50.1%的CO₂转化率，99.9%的甲烷(CH₄)选择性以及94.4 mmol·g^-1·h^-1的CH₄产出速率。与之相比，NiAl-Cl-MO和NiAl-SO₄-MO催化剂的CO₂甲烷化活性极低。H₂程序升温脱附(temperature programmed desorption with H₂，H₂-TPD)实验和密度泛函理论计算(density functional theory，DFT)结果表明，低CO₂转化率是由于残留的氯(Cl)或硫(S)与金属Ni形成的强配位键阻碍了H₂的吸附和活化。因此，在设计LDH衍生的催化剂，特别是用于氢化反应的Ni基催化剂时，应优先考虑层间阴离子在LDH中的重要作用。
- Photothermocatalysis,
- CO₂ methanation,
- Ni-Al₂O₃ catalyst,
- Layered double hydroxides,
- Interlayer anion
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层状双金属氢氧化物的层间阴离子对衍生的Ni-Al2O3催化剂光热催化CO2甲烷化反应的影响

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层状双金属氢氧化物的层间阴离子对衍生的Ni-Al₂O₃催化剂光热催化CO₂甲烷化反应的影响