N含量对氮化铁催化剂CO2加氢制低碳烯烃催化性能的影响
Effects of N contents on catalytic performances of iron nitride catalysts for CO2 hydrogenation to low-carbon olefins
- 低碳化学与化工 2025: 1-9.
- 作者机构：
郑州大学 炼焦煤资源绿色开发全国重点实验室，河南 郑州 450001
- 作者简介：
孙浩淳（2003—），硕士研究生，研究方向为铁基催化剂催化CO2加氢制烯烃，E-mail：1224049116@qq.com。
涂维峰（1986—），博士，教授，研究方向为多相催化反应机理，催化剂动态-构效关系研究，E-mail：Tuweifeng@zzu.edu.cn
张振洲（1987—），博士，教授，研究方向为工业催化剂设计及其应用，E-mail：zhangzhenzhou@zzu.edu.cn。
- 基金信息：催化基础国家重点实验室开放课题(N-22-13);国家自然科学基金(22478365)
DOI：10.12434/j.issn.2097-2547.20250194
中图分类号： TQ214收稿：2025-04-22，
修回：2025-05-15，
网络出版：2025-11-20，
- 稿件说明：
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孙浩淳,廖兵兵,党闪闪等.N含量对氮化铁催化剂CO2加氢制低碳烯烃催化性能的影响[J].低碳化学与化工,
SUN Haochun,LIAO Bingbing,DANG Shanshan,et al.Effects of N contents on catalytic performances of iron nitride catalysts for CO2 hydrogenation to low-carbon olefins[J].Low-Carbon Chemistry and Chemical Engineering,
孙浩淳,廖兵兵,党闪闪等.N含量对氮化铁催化剂CO2加氢制低碳烯烃催化性能的影响[J].低碳化学与化工, DOI：10.12434/j.issn.2097-2547.20250194.
SUN Haochun,LIAO Bingbing,DANG Shanshan,et al.Effects of N contents on catalytic performances of iron nitride catalysts for CO2 hydrogenation to low-carbon olefins[J].Low-Carbon Chemistry and Chemical Engineering, DOI：10.12434/j.issn.2097-2547.20250194.
摘要
通过逆水煤气反应将CO
2
加氢制备低碳烯烃是实现CO
2
转化的有效途径之一。铁基催化剂因具有适宜的加氢活性、碳链生长能力以及较低的成本，被视为催化剂候选物。氮化铁催化剂作为铁基催化剂，为具有广阔前景的CO
2
加氢制备高价值产物的催化剂，但不同N含量的氮化铁催化剂作用下CO
2
加氢含碳产物分布规律依然不清晰。通过精确调控煅烧条件，成功制备了3种具有不同N含量的铁基催化剂（Na/Fe
2
O
3
、Na/Fe
2
N和Na/Fe
4
N），并深入研究了以上3种催化剂的CO
2
加氢制低碳烯烃催化性能。结果表明，在320 ℃、1.5 MPa、CO
2
/H
2
/Ar（体积比1:3:3）混合气和空速10000 mL/(g·h)条件下反应14 h后，Na/Fe
4
N的低碳烯烃选择性（49.4%）高于Na/Fe
2
N（32.6%）和Na/Fe
2
O
3
（33.7%），并且Na/Fe
4
N的 CO选择性、碳原子数大于等于5的重质烃（C
5+
）选择性和碳原子数为2~4的烯烃与烷烃选择性之比（O/P值）均高于Na/Fe
2
N，但CO
2
转化率低于Na/Fe
2
N。通过XPS表征发现反应后Na/Fe
2
N中，Fe物种与Fe
5
C
2
的电子云密度减小，不利于低碳烯烃生成。
Abstract
One of the effective ways to achieve CO
2
conversion is to hydrogenate CO
2
to produce low-carbon olefins through reverse water gas reaction. Iron based catalysts are considered as preferred catalyst candidates due to their suitable hydrogenation activity
carbon chain growth ability and lower cost. As iron-based catalysts
iron nitride catalysts are promising catalysts for the preparation of high-value products from CO
2
hydrogenation. However
the distribution pattern of carbon containing products in CO
2
hydrogenation catalyzed by iron nitride catalysts with different N contents is still unclear. By precisely adjusting the calcination conditions
three iron-based catalysts with different N contents (Na/Fe
2
O
3
Na/Fe
2
N and Na/Fe
4
N) were successfully prepared
and their catalytic performances for CO
2
hydrogenation to low-carbon olefins were studied. The results show that under the conditions of 320 ℃
1.5 MPa
CO
2
/H
2
/Ar (volume ratio of 1:3:3) and space velocity of 10000 mL/(g·h)
the low-carbon olefins selectivity of Na/Fe
4
N (49.4%) is higher than that of Na/Fe
2
N (32.6%) and Na/Fe
2
O
3
(33.7%)
and the CO selectivity
heavy hydrocarbons with five or more carbon atoms (C
5+
)
selectivity and ratio of olefins with two to four carbon atoms to alkanes selectivity (O/P value) of Na/Fe
4
N are higher than those of Na/Fe
2
N
but the CO
2
conversion rate is lower than that of Na/Fe
2
N after 14 h reaction. The XPS characterization results show that the electron cloud density of Fe species and Fe
5
C
2
decreases in Na/Fe
2
N after
reaction
which is not conducive to the generation of low-carbon olefins.
关键词
Keywords
references
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