铈掺杂锆基金属-有机框架纳米颗粒的制备及其光催化二氧化碳环加成反应催化性能研究

doi:10.6023/cjoc202405044

有机化学 ›› 2024, Vol. 44 ›› Issue (10): 3169-3177.DOI: 10.6023/cjoc202405044 上一篇下一篇

研究论文

铈掺杂锆基金属-有机框架纳米颗粒的制备及其光催化二氧化碳环加成反应催化性能研究

赵盈喆^a^,^b, 张子瑄^a^,^b, 张建玲^a^,^b^,^*(), 张仁杰^a^,^b, 李美玲^a^,^b, 滕钰楠^a^,^b, 王昊翔^a^,^b

a 中国科学院化学研究所北京 100190
b 中国科学院大学化学科学学院北京 100049

收稿日期:2024-05-29 修回日期:2024-08-24 发布日期:2024-09-18
基金资助:
国家重点研发计划(2023YFA1507903); 国家自然科学基金(22033009); 国家自然科学基金(22121002); 国家自然科学基金(22238011)

Synthesis of Cerium Doped Zirconium-Based Metal-Organic Framework Nanoparticles and Their Photocatalytic Performance for Carbon Dioxide Cycloaddition

Yingzhe Zhao^a^,^b, Zixuan Zhang^a^,^b, Jianling Zhang^a^,^b,*(), Renjie Zhang^a^,^b, Meiling Li^a^,^b, Yunan Teng^a^,^b, Haoxiang Wang^a^,^b

a Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190
b School of Chemical Sciences, University of Chinese Academy of Sciences, Beijing 100049

Received:2024-05-29 Revised:2024-08-24 Published:2024-09-18
Contact: *E-mail: zhangjl@iccas.ac.cn
Supported by:
National Key Research and Development Program of China(2023YFA1507903); National Natural Science Foundation of China(22033009); National Natural Science Foundation of China(22121002); National Natural Science Foundation of China(22238011)

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摘要/Abstract

在离子液体1-丁基-3-甲基咪唑醋酸盐中合成了铈掺杂的锆基NH₂-UiO-66纳米颗粒, 采用X射线衍射、红外光谱、扫描电子显微镜和透射电子显微镜研究了所得材料的晶体结构和形貌, 采用X射线光电子能谱和能量色散X射线谱研究了所得材料中元素的价态和分布情况. 催化性能研究表明, 铈掺杂的NH₂-UiO-66纳米颗粒在1,2-环氧丁烷与二氧化碳的环加成反应中催化效率比NH₂-UiO-66得到显著提高. 光电性质研究表明, 该催化剂具有较强的光电流响应、较小的界面电荷转移阻抗、较窄的带隙和较低的平带电位. 该工作为光催化二氧化碳环加成反应高效催化剂的合成提供了一种新思路.

关键词: 金属-有机框架, 双金属, 纳米颗粒, 离子液体, 二氧化碳环加成

Cerium-doped zirconium-based NH₂-UiO-66 nanoparticles were synthesized in ionic liquid 1-butyl-3-methyl- imidazolium acetate at room temperature. The crystal structure and morphology were studied using X-ray diffraction, infrared spectroscopy, scanning electron microscopy and transmission electron microscopy. The valence state and distribution of elements in the obtained materials were examined using X-ray photoelectron spectroscopy and energy-dispersive X-ray spectroscopy. Catalytic performance studies show that the cerium-doped NH₂-UiO-66 exhibits improved catalytic efficiency in the cycloaddition reaction of 1,2-butylene oxide and carbon dioxide than pure NH₂-UiO-66. Studies on the photoelectric properties indicate that the cerium-doped NH₂-UiO-66 catalyst possesses strong photocurrent response, low interfacial charge transfer resistance, narrow band gap, and low flat band potential. This work provides a new approach of synthesizing high-performance catalyst for photocatalytic CO₂ cycloaddition.

Key words: metal-organic framework, bimetallic, nanoparticle, ionic liquid, CO₂ cycloaddition

引用此文

赵盈喆, 张子瑄, 张建玲, 张仁杰, 李美玲, 滕钰楠, 王昊翔. 铈掺杂锆基金属-有机框架纳米颗粒的制备及其光催化二氧化碳环加成反应催化性能研究[J]. 有机化学, 2024, 44(10): 3169-3177.

Yingzhe Zhao, Zixuan Zhang, Jianling Zhang, Renjie Zhang, Meiling Li, Yunan Teng, Haoxiang Wang. Synthesis of Cerium Doped Zirconium-Based Metal-Organic Framework Nanoparticles and Their Photocatalytic Performance for Carbon Dioxide Cycloaddition[J]. Chinese Journal of Organic Chemistry, 2024, 44(10): 3169-3177.

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图/表 10

Figure 1. XRD patterns of NU66-i-Zr0.8Ce0.2, NU66-s and NU- 66-i

Figure 2. SEM (a, b), TEM (c) and element mapping (d) images of NU66-i-Zr0.8Ce0.2

Figure 3. Infrared spectra of NU66-i-Zr0.8Ce0.2, NU66-i, NU66-s and BmimOAc

Figure 4. XPS spectra of NU66-i-Zr0.8Ce0.2, NU66-i and NU66-s (a) Survey scan; (b) C1s scan; (c) N1s scan; (d) O1s scan; (e) Zr3d scan; (f) Ce3d scan

Figure 5. Catalytic performances of NU66-i-Zr0.8Ce0.2, NU66-s and NU66-i

Scheme 1. Substrate universality test of NU66-i-Zr0.8Ce0.2

Entry	Atmosphere	Light irradiation	Catalyst	Co-catalyst	Yield/%	Selectivity/%
1	101 kPa CO₂	300 W Xe lamp	30 mg NU66-i-Zr_0.8Ce_0.2	0.5 mmol TBAB	86	>99
2	101 kPa Ar	300 W Xe lamp	30 mg NU66-i-Zr_0.8Ce_0.2	0.5 mmol TBAB	0	—
3	101 kPa CO₂	Dark	30 mg NU66-i-Zr_0.8Ce_0.2	0.5 mmol TBAB	13	>99
4	101 kPa CO₂	300 W Xe lamp	—	0.5 mmol TBAB	38	>99
5	101 kPa CO₂	300 W Xe lamp	30 mg NU66-i-Zr_0.8Ce_0.2	—	1.0	>99

Table 1. Control experiments for the CO2 cycloaddition reaction with 1,2-epoxybutane

Figure 6. Photoelectric properties of NU66-i-Zr0.8Ce0.2, NU66-s and NU66-i (a) Photocurrent response; (b) Ultraviolet-visible diffused reflectance spectra; (c) Tauc plot; (d) Mott-Schottky plot

Figure 7. Calculated adsorption configuration of NU66-i (a) and NU66-i-Zr0.8Ce0.2 (b)

Scheme 2. Reaction mechanism proposed

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铈掺杂锆基金属-有机框架纳米颗粒的制备及其光催化二氧化碳环加成反应催化性能研究

Synthesis of Cerium Doped Zirconium-Based Metal-Organic Framework Nanoparticles and Their Photocatalytic Performance for Carbon Dioxide Cycloaddition

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