Simulated solar driven catalytic degradation of psychiatric drug carbamazepine with binary BiVO4 heterostructures sensitized by graphene quantum dots

Simulated solar driven catalytic degradation of psychiatric drug carbamazepine with binary BiVO4 heterostructures sensitized by graphene quantum dots
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石墨烯量子点敏化二元 BiVO4 异质结构模拟太阳能驱动催化降解精神科药物卡马西平

DOI:
10.1016/j.apcatb.2016.10.067
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发表时间:
2017-05-15
影响因子:
22.1
通讯作者:
Wu, Ming-hong
Wu, Ming-hong
中科院分区:
化学1区
文献类型:
--
作者:
Tang, Liang;Wang, Jia-jun;Wu, Ming-hong

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本论文制备了负载BiVO4的太阳能驱动GQD催化剂,并将其用于模拟太阳光下降解卡马西平(CBZ)。所制备的三元催化剂(GQD/m-BiVO4/t-BiVO4)用透射电子显微镜、高分辨电子显微镜、X射线衍射仪、X射线光电子能谱、紫外可见光谱、拉曼光谱和荧光光谱对催化剂进行了表征。表征结果表明,GQD在二元BiVO_4载体上分散良好,负载GQD后复合材料的光学性能得到改善。通过在原始BiVO4半导体表面引入GQD,新型复合催化剂的光催化活性显著提高。其中,负载量为1.0wt%的GQD催化剂对CBZ的光催化活性最高,其矿化度可达95%以上。此外,对CBZ在催化过程中的转化产物(TP)进行了初步鉴定,认为羟基自由基是其主要活性物种。从密度泛函理论(DFT)计算和TPS的演化来看,在GQD/BiVO4的催化下,杂环上酰胺基团的羟基化和裂解可能是CBZ的主要初始光催化降解通道。(C)2016年,由爱思唯尔出版。
Herein, solar-driven GQDs loaded BiVO4 heterostructure catalysts were fabricated and employed to degradate carbamazepine (CBZ) under simulated solar light. The as-prepared ternary catalysts (GQD/m-BiVO4/t-BiVO4) were thoroughly characterized by TEM, HRTEM, XRD, XPS, UV-vis, Raman and PL. The characterization results demonstrated that GQDs are well-dispersed on binary BiVO4 support, and the optical properties of the composites are improved with GQDs loaded. The photocatalytic activities of the novel composite catalysts were significantly increased by incorporation of GQDs on original BiVO4 semiconductor. In particular, the 1.0 wt% GQD loaded catalysts exhibited the highest photocatalytic activity for CBZ, and the mineralization degree of CBZ with the catalysts could achieve more than 95%. In addition, the transformation products (TPs) of CBZ during the catalysis processes were tentatively identified, and hydroxyl radicals were regarded as the predominant active species. From the results of density functional theory (DFT) calculations and evolution of TPs, hydroxylation and cleavage of amide group on the heterocycle may be the main initial photocatalytic degradation channels for CBZ under the catalysis of GQD/BiVO4. (C) 2016 Published by Elsevier B.V.