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Ni/USY催化剂金属-载体相互作用对CO2甲烷化性能的影响
Effects of metal-support interactions in Ni/USY catalysts on CO2 methanation performances
- 低碳化学与化工 2025, 50(1): 27-34.
- 作者机构：
1.太原理工大学 化学工程与技术学院，山西 太原 030024
2.中石化（大连）石油化工研究院有限公司，辽宁 大连 116045
3.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
- 作者简介：
李江涛（2000—），硕士研究生，研究方向为加氢催化剂合成，E-mail：912189231@qq.com。
秦 波（1981—），博士研究生，研究员，研究方向为分子筛催化剂工业设计，E-mail：qinbo.fshy@sinopec.com；
闫晓亮（1985—），博士，教授，研究方向为多相催化剂设计与研发，E-mail：yanxiaoliang@tyut.edu.cn。
- 基金信息：国家自然科学基金(22278286);中石化科研专项(122027)
DOI：10.12434/j.issn.2097-2547.20240084
中图分类号： TQ203纸质出版日期：2025-01-25，
收稿日期：2024-03-04，
修回日期：2024-03-21，
- 稿件说明：
移动端阅览
李江涛, 刘相洋, 黄奕晨, 等. Ni/USY催化剂金属-载体相互作用对CO2甲烷化性能的影响[J]. 低碳化学与化工, 2025,50(1):27-34.
LI JIANGTAO, LIU XIANGYANG, HUANG YICHEN, et al. Effects of metal-support interactions in Ni/USY catalysts on CO2 methanation performances. [J]. Low-carbon chemistry and chemical engineering, 2025, 50(1): 27-34.
李江涛, 刘相洋, 黄奕晨, 等. Ni/USY催化剂金属-载体相互作用对CO2甲烷化性能的影响[J]. 低碳化学与化工, 2025,50(1):27-34. DOI： 10.12434/j.issn.2097-2547.20240084.
LI JIANGTAO, LIU XIANGYANG, HUANG YICHEN, et al. Effects of metal-support interactions in Ni/USY catalysts on CO2 methanation performances. [J]. Low-carbon chemistry and chemical engineering, 2025, 50(1): 27-34. DOI： 10.12434/j.issn.2097-2547.20240084.
摘要
调控金属-载体相互作用是提升负载型Ni基催化剂CO
2
甲烷化性能的重要途径之一。采用浸渍法通过调变溶液pH值制备了系列Ni/USY-
X
（
X
= 1、3或5）催化剂，考察了各催化剂的CO
2
甲烷化性能。其中Ni/USY-3催化剂在450 ℃、20 h反应条件下的稳定性测试中表现出相对最优的CO
2
甲烷化性能，CO
2
转化率和CH
4
选择性分别达到84.5%和95.7%。采用XRD、H
2
-TPR、SEM和TEM等对催化剂的物相结构、还原性能和形貌进行了表征，从微观层面系统考察了浸渍溶液pH值对催化剂结构和CO
2
甲烷化性能的影响。结果表明，在适宜pH值调控下，金属-载体相互作用增强，活性金属Ni晶粒的粒径减小，分散度提高。进一步借助原位FT-IR对催化剂的反应路径进行了分析，发现Ni/USY-3催化剂遵循甲酸盐路径。高分散性、较小粒径的活性金属Ni晶粒为碳酸氢盐及时氢化为关键中间体单齿甲酸盐提供了丰富的活性位点，从而实现了CO
2
的高效转化。
Abstract
Tailoring of the metal-support interaction is one of the important ways to improve the CO
2
methanation performances on the supported Ni-based catalysts. A series of Ni/USY-
X
(
X
= 1
3 or 5) catalysts were prepared by impregnation by adjusting the pH value of the solution. And CO
2
methanation performances of catalysts were investigated. Ni/USY-3 catalyst showes excellent CO
2
methanation performance with CO
2
conversion rate of 84.5% and
CH
4
selectivity of 95.7% in stability test at the condition of 450 ℃ and 20 h. XRD
H
2
-TPR
SEM and TEM were used to characterize the structure and morphology of the catalyst
and the effects of impregnating solution pH value on the structure and CO
2
methanation performances of the catalysts were systematically investigated at the microscopic level. The results show that under appropriate pH value control
the metal-support interaction is enhanced
the particle size of the active metal Ni particles is reduced
and the dispersion is enhanced. Furthermore
the reaction paths of catalyst were analyzed by in situ FT-IR. The results indicate that the Ni/USY-3 catalyst follows the formate pathway. The highly dispersed and small particle size of the active metal Ni particles provide abundant active sites for the timely hydrogenation of bicarbonate into the key intermediate monodontate
leading to achieving efficient conversion of CO
2
.
关键词
CO2甲烷化金属-载体相互作用酸性
Keywords
CO2 methanationmetal-support interactionacidity
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