Heteroatom doped iron-based catalysts prepared by urea self-combustion method for efficient CO2 hydrogenation
Heteroatom doped iron-based catalysts prepared by urea self-combustion method for efficient CO2 hydrogenation
复制标题
DOI：
10.1016/j.fuel.2020.118102
复制
发表时间：
2020-09
期刊：
影响因子：
7.4
通讯作者：
Lisheng Guo;Jie Li;Yan Zeng;Rungtiwa Kosol;Yuanyuan Cui;N. Kodama;Xiaoyu Guo;R. Prasert;
中科院分区：
文献类型：
--
作者：
Lisheng Guo;Jie Li;Yan Zeng;Rungtiwa Kosol;Yuanyuan Cui;N. Kodama;Xiaoyu Guo;R. Prasert;
这项工作描述了一种通过尿素自燃烧法制备杂原子掺杂铁基催化剂（尖晶石结构）的新路线，并详细研究了这些自燃烧催化剂的催化性能。研究发现催化性能受到掺杂金属性质的影响。由于Ni和Co的高甲烷化活性，NiFe2Ox和CoFe2Ox催化剂与Fe2O3催化剂相比表现出高CH4选择性。 MgFe2Ox表现出高烯烃加氢能力。相比之下，Cu和Zn的利用通过调节表面CO2吸附和碳化物含量来提高催化活性和烯烃选择性。在这些尖晶石催化剂中，ZnFe2Ox催化剂表现出最好的CO2加氢性能。增强的 CO2 吸附以及碳化物的活性物质导致良性氢化行为。同时，还研究了Zn/Fe摩尔比的影响。值得注意的是，无论Zn促进剂的添加量如何，催化性能都能得到改善。然而，当Zn/Fe摩尔比等于1/2时，催化性能达到最佳水平。该方法为CO2催化加氢转化为高价值产品提供了一种不同于传统催化剂制备工艺的新策略。
This work describes a novel route for the fabrication of heteroatom doped iron-based catalysts (spinel-like structure) through urea self-combustion method, and catalytic performances over these self-combustion catalysts are investigated in detail. It is found that catalytic performances are affected by the properties of doped metals. Owing to the high methanation activity of Ni and Co, NiFe2Oxand CoFe2Oxcatalysts present high CH4selectivity compared to Fe2O3catalysts. MgFe2Oxexhibits high olefin hydrogenation ability. By contrast, the utilization of Cu and Zn promotes catalytic activity and olefins selectivity via regulating surface CO2adsorption and carbides content. Among these spinel catalysts, the ZnFe2Oxcatalyst shows the best CO2hydrogenation performance. Enhanced CO2adsorptions as well as active species of carbides result in the benign hydrogenation behavior. Meanwhile, the effects of Zn/Fe molar ratio are also investigated. It is worth noting that the catalytic performance can be improved regardless of the added amount of Zn promoter. Nevertheless, the catalytic performance reaches the best level when the Zn/Fe molar ratio equals 1/2. The proposed method provides a new strategy different from traditional catalyst preparation process for catalytic hydrogenation of CO2into highly valuable products.