| 双配体CuFe@MOFs材料为前驱体的催化剂的组分调控对CO2加氢制C2+醇性能的影响 | |
| Effect of Component Control of Catalysts with Dual Ligand CuFe@MOFs as Precursor on Performance of CO2 Hydrogenation to C2+ Alcohol | |
| 摘要: 采用水热法制备了以对苯二甲酸和对氨基苯甲酸为配体的双配体Fe基MOFs材料（MIL-88B（Fe）），在浸渍一定量Cu物种后经氮气气氛焙烧得到活性组分均匀分散的CuFe基催化剂。通过改变2种配体的比例调控催化剂表面Fe活性物种的价态分布，并考察了其用于固定床反应器上CO2加氢制C2+醇的催化性能，结合X射线衍射（XRD）、H2程序升温还原（H2-TPR）、N2吸附-脱附、扫描电子显微镜（SEM）、X射线光电子能谱（XPS）等表征结果发现，对苯二甲酸与对氨基苯甲酸物质的量之比为5：2时，催化剂表面低价态铁原子占比为71.27%，催化剂展现最优的催化活性，CO2转化率为8.80%，总醇选择性为31.52%，其中C2+醇的物质的量分数达到94.70%。 | |
| 关键词: 双配体 CuFe@MOFs 组分调控 二氧化碳 加氢 C2+醇 | |
| 基金项目: 国家科技支撑计划项目（No.2013BAC14B04）、国家自然科学基金（No.21336006）、山西省重点研发计划项目（No.201803D421099，201803D121043）和山西省留学基金委资助项目（No.2017-035）资助。 | |
| Abstract: CuFe@MOFs derived catalysts were synthesized by introducing a second ligand, p-aminobenzoic acid, in the hydrothermal synthesis of MIL-88B(Fe), which was followed by impregnation with Cu species. The physicochemical properties of the catalysts were characterized by X-ray diffraction (XRD), H2-temperature programmed reduction (H2-TPR), N2 adsorption-desorption, scanning electron microscopy (SEM) and X-ray photoelectron spectroscopy (XPS). The catalytic performance of the catalysts for hydrogenation of CO2 to C2+ alcohol (C2+OH) was tested in a fixed bed reactor. The results show that the elements of active components were evenly dispersed, and the active species distribution on the catalyst surface can be controlled by adjusting the molar ratio of two ligands (terephthalic acid to p-aminobenzoic acid ligands) in the raw materials. When the molar ratio of terephthalic acid to p-aminobenzoic acid was 5:2, the proportion of low-valence iron of the as-obtained catalyst was the highest (71.27%). Accordingly, this catalyst showed the best performance for CO2 hydrogenation to C2+OH, that the conversion of CO2 was 8.80%, the selectivity of total alcohol (ROH) was 31.52% and the molar fraction of C2+OH was 94.70%. This might be due to the high proportion of low-valence iron species and the well-dispersed active components. | |
| Keywords: dual ligand CuFe@MOFs composition control carbon dioxide hydrogenation C2+ alcohol | |
| 投稿时间：2021-01-28 修订日期：2021-04-25 | |
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| 张倩,温月丽,王斌,范鹤鸣,杨晨,宋镕鹏,张维中,黄伟.双配体CuFe@MOFs材料为前驱体的催化剂的组分调控对CO2加氢制C2+醇性能的影响[J].无机化学学报,2021,37(8):1390-1398. | |
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