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Fabrication of UiO-66-NH2/Ce(HCOO)3 heterojunction with enhanced photocatalytic reduction of CO2 to CH4
Journal of CO2 Utilization ( IF 7.2 ) Pub Date : 2022-08-01 , DOI: 10.1016/j.jcou.2022.102151
Nicui Yuan , Yuxin Mei , Yuwei Liu , Yating Xie , Baining Lin , Yonghua Zhou

The development of efficient and highly selective photocatalysts is a key point for the photocatalytic conversion of CO2. In this paper, a composite catalyst UiO-66-NH2/Ce(HCOO)3 (simplified to UNH/Ce(HCOO)3) was fabricated by one pot method with CeCO3OH as the precursor. Scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction (XRD), and X-ray photoelectron spectroscopy (XPS) characterizations results confirmed that UNH was dispersed on the surface of Ce(HCOO)3 and strongly interacted with it via Ce-N bond. The yield of CH4 on the optimal UNH/Ce(HCOO)3 catalyst reached 3 times of that on pristine UNH, up to 128.81 μmol g−1, with the CH4 selectivity of 71.9 %, and the Relectron reached 286.46 μmol g−1 h−1. The UV–vis diffuse reflection spectra and photoelectrochemical tests results confirmed that the improved photocatalytic CO2 reduction performance and high CH4 selectivity could be attributed to the formation of the type-Ⅱheterojunction of UNH/Ce(HCOO)3 with abundant Ce3+, which expanded the visible light absorption range, accelerated the separation and transfer rates of photogenerated charges, and thus efficiently promoted the multi-electron reduction reaction of CO2 to CH4. In addition, the reaction temperature affected profoundly the cycle performance of the catalyst. The results presented here illustrated the possibility for improving the stability of UNH/Ce(HCOO)3-1.80 by decreasing reaction temperature.



中文翻译:

制备 UiO-66-NH2/Ce(HCOO)3 异质结,增强光催化 CO2 还原为 CH4

开发高效、高选择性的光催化剂是CO 2光催化转化的关键。本文以CeCO 3 OH为前驱体,采用一锅法制备了复合催化剂UiO-66-NH 2 /Ce(HCOO) 3(简化为UNH/Ce(HCOO) 3 )。扫描电子显微镜(SEM)、透射电子显微镜(TEM)、X射线衍射(XRD)和X射线光电子能谱(XPS)表征结果证实UNH分散在Ce(HCOO) 3的表面并与强相互作用通过Ce-N键与它。最佳UNH/Ce(HCOO) 3上的CH 4产率催化剂达到原始UNH的3倍,达到128.81 μmol g -1,CH 4选择性为71.9 %,R电子达到286.46 μmol g -1 h -1。UV-vis漫反射光谱和光电化学测试结果证实,光催化CO 2还原性能的提高和CH 4的高选择性可归因于UNH/Ce(HCOO) 3与丰富的Ce 3+形成Ⅱ型异质结。,扩大了可见光吸收范围,加快了光生电荷的分离和转移速率,从而有效地促进了CO 2到CH 4的多电子还原反应。此外,反应温度对催化剂的循环性能影响很大。这里给出的结果说明了通过降低反应温度来提高 UNH/Ce(HCOO) 3 -1.80 稳定性的可能性。

更新日期:2022-08-01
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