| 三维Cu-MOF对亚甲蓝的吸附和光催化降解及其机理 |
| Adsorption, photocatalytic degradation, and their mechanisms of methylene blue on three-dimensional Cu-MOF |
| 作者 | 单位 | E-mail | | 鲁雪莹 | 延安大学化学与化工学院, 新能源与新功能材料实验室, 延安 716000 | | | 张美丽 | 延安大学化学与化工学院, 新能源与新功能材料实验室, 延安 716000 | ydzml2332041@163.com | | 任宜霞 | 延安大学化学与化工学院, 新能源与新功能材料实验室, 延安 716000 | | | 王记江 | 延安大学化学与化工学院, 新能源与新功能材料实验室, 延安 716000 | | | 杨晓刚 | 洛阳师范大学化学与化学工程学院, 河南省功能多孔材料重点实验室, 洛阳 471934 | yxg2233@126.com |
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| 摘要: 本文报道了[Cu3(ppda)3(tib)2(H2O)4]·6H2O (Cu-MOF)的合成、结构、吸附和光催化降解性能。在Cu-MOF中，1，4-苯二乙酸(H2ppda)和1，3，5-三(1-咪唑基)苯(tib)配体交替连接Cu离子形成二维层，层与层之间通过trans-ppda2-相互穿插形成稳定的三维结构。Cu-MOF对亚甲蓝(MB)的催化效率为97%，最高反应速率常数为0.019 7 min-1。光催化降解机理：在光的激发下，催化剂表面的光生电子和空穴对发生分离，并与O2、H2O、H2O2反应生成活性物质，将染料降解为CO2和H2O。在MB溶液中加入NaCl (200 g·L-1)后，Cu-MOF的吸附量有所提升(87.23 mg·g-1)，准二级动力学模型和Langmuir等温线模型的实验数据拟合程度较好，该吸附的主要过程为单层化学吸附。 |
| 关键词: 金属有机骨架 染料污染物 光催化活性 吸附性能 |
| 基金项目: 国家自然科学基金(No.21971100)、陕西省自然科学基金(No.2022JM-095)和榆林市科学技术局项目(No.CXY-2021-126)资助。 |
| Abstract: Herein, we report the synthesis, structure, adsorption and photocatalytic degradation properties of a novel metal-organic framework [Cu3(ppda)3(tib)2(H2O)4]·6H2O (Cu-MOF) by the selection of the flexible 1,4-phenylenedi- acetic acid (H2ppda) and the rigid 1,3,5-tris(1-imidazolyl) benzene (tib). In Cu-MOF, ppda2- and tib ligands alternately link Cu ions to form 2D polymeric layers, the layer and layer interpenetrate each other by trans-ppda2- to form a stable 3D structure. Cu-MOF has excellent thermal stability and semiconductor properties, so it can be used as a catalyst. Cu-MOF had the best catalytic effect on methylene blue (MB), with a catalytic efficiency of up to 97% and the highest reaction rate constant of 0.019 7 min-1. The main photocatalytic degradation mechanism is the separation of the photogenerated electron and hole pair of the catalyst under the light excitation, and the redox reaction occurs to produce the active species to degrade the dye and eventually decompose into carbon dioxide and water. Cu - MOF exhibited high adsorption capacity after adding NaCl (200 g·L-1) to MB solution (87.23 mg·g-1). The adsorption process is a spontaneous monolayer chemisorption process illustrated by the pseudo-second-order kinetic and Langmuir isotherm models and thermodynamic studies. |
| Keywords: metal-organic framework dye contaminant photocatalytic activity adsorption property |
| 投稿时间：2023-03-17 修订日期：2023-09-02 |
| 摘要点击次数: 5413 |
| 全文下载次数: 799 |
| 鲁雪莹,张美丽,任宜霞,王记江,杨晓刚.三维Cu-MOF对亚甲蓝的吸附和光催化降解及其机理[J].无机化学学报,2023,39(10):1991-2002. |
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| Support information: 相关附件： 230087_附件3：ESI修改稿_编号230087.docx |
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