Construction of a stable porous composite with tunable graphene oxide in Ce-based-MOFs for enhanced solar-photocatalytic degradation of sulfamethoxazole in water
Construction of a stable porous composite with tunable graphene oxide in Ce-based-MOFs for enhanced solar-photocatalytic degradation of sulfamethoxazole in water
复制标题
在 Ce 基 MOF 中构建具有可调氧化石墨烯的稳定多孔复合材料，以增强水中磺胺甲恶唑的太阳能光催化降解
DOI：
10.1016/j.seppur.2022.122006
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发表时间：
2022
影响因子：
8.6
通讯作者：
Xiang Li
中科院分区：
文献类型：
--
作者：
Xin Mi;Xiang Li
·Ce-MOFs中的可调GO促进了光催化性能。·该复合物促进了电子束中的电荷转移。· ·O2-被确定为主要的活性氧物种。·计算了ROS的稳态浓度。·该复合材料显示出比原始Ce-MOF更好的水稳定性。药物活性化合物（PhAC）在水体中的存在引起了越来越多的关注。有效消除这些有毒环境污染物具有挑战性，但非常重要。铈基MOFs被认为是一种新型的金属有机骨架光催化剂。然而，有限的光吸收能力、光生载流子的快速复合以及水稳定性限制了其进一步的应用。在此，成功地将UiO-66（Ce）原位构建到一系列氧化石墨烯（GO）（lmg 〜 7.5mg）的表面上。含氧官能团的GO（OCFGs）可提高界面对200 μg/L磺胺甲恶唑（SMX）的吸附量（约45%），提高SMX的降解效率。具有最佳配比（GO@ UiO-66（Ce）-5）的复合物显著提高了电荷分离能力并产生了大量活性氧（ROS）。·O2-是SMX降解的主要驱动反应物，其稳态浓度为2.5×10 - 9 M（鼓氧条件下的1.37倍），远高于·OH的稳态浓度（1.62×10 - 14）.系统地考察了溶解氧、初始溶液pH和催化剂用量等主要操作参数。通过高效液相色谱-三重四极杆质谱联用（HPLC-MS/MS）鉴定了几种中间体。通过选择该策略，MOFs与GO基体表面紧密结合，使水处理过程中Ce离子的泄漏得到明显抑制（约3倍）。该研究为改善现有光催化材料去除水中苯乙酸的性能提供了有益的指导。
• Tunable GO in Ce-MOFs promoted the photocatalytic performance. • The composite facilitates the charge transfer in photocatalysis. • •O 2 - has been identified as the major reactive oxygen species. • Steady-state concentrations of ROS have been calculated. • This composite shows better water stability than the pristine Ce-MOFs. Pharmaceutically active compounds (PhACs) are ubiquitously detected in water matrices, arousing growing concern. Effective abatement of these toxic environmental contaminants is challenging but of great importance. Ce-based MOFs have been considered novel metal-organic framework (MOFs)-based photocatalysts in water treatment. However, limited light absorption ability, fast recombination of photogenerated carriers, and water stability limited the further application. Here, the UiO-66 (Ce) was successfully constructed onto the surface of a series of graphene oxide (GO) (1 mg∼7.5 mg) in situ. GO with oxygen-containing functional groups (OCFGs) increased the adsorption (∼45%) of the trace amount of sulfamethoxazole (SMX) (200 μg/L) over the interfaces and enhanced the degradation efficiency of SMX. The composite with the optimal ratio (GO@ UiO-66 (Ce)-5) significantly increased the charge separation ability and produced a large number of reactive oxygen species (ROS). •O 2 - was proved to be the major driving reactive substance for SMX degradation with the calculated steady-state concentration of 2.5×10 -9 M (∼1.37 times higher with bubbled oxygen), which is much higher than that of detected •OH (1.62×10 -14 ). Major operational parameters including dissolved oxygen, initial solution pH, and catalyst dosages were investigated systematically. Several intermediates were identified by high-performance liquid chromatography coupled with triple quadrupole mass spectrometry (HPLC-MS/MS). By choosing the strategy, MOFs were closely bonded to the surface of the GO matrix, making the leakage of Ce ions inhibited obviously (∼3 times) in the water treatment process. This study offers useful guidance for improving the performance of existing photocatalytic materials for PhACs removal.