Visible-light-driven photocatalytic and photoelectrocatalytic debromination of BDE-47 on a macroporous silicon/graphene heterostructure

Visible-light-driven photocatalytic and photoelectrocatalytic debromination of BDE-47 on a macroporous silicon/graphene heterostructure
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大孔硅/石墨烯异质结构上 BDE-47 的可见光驱动光催化和光电催化脱溴

DOI:
10.1016/j.seppur.2012.06.007
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发表时间:
2012-08
影响因子:
8.6
通讯作者:
Zhao, Qian
Zhao, Qian
中科院分区:
工程技术1区
文献类型:
--
作者:
Su, Jingyang;Yu, Hongtao;Chen, Shuo;Quan, Xie;Zhao, Qian

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采用电泳沉积法在大孔硅(MPSi)表面沉积石墨烯(Gr)片层,然后对样品进行退火处理,以提高附着力和电化学性能,制备了MPSi/Gr异质结构。在光电化学测试中,MPSi/Gr异质结显示出稳定的高光电流。MPSi/Gr异质结的稳定性得益于Gr层的保护,光电流的增强归因于MPSi/Gr异质结的有效光生电荷分离。对BDE-47的光催化和光电催化脱溴实验结果表明,MPSi/Gr具有良好的光催化性能,外加偏压可以提高MPSi/Gr的光催化性能。MPSi/Gr(1.13 h −1)异质结构的光电催化动力学常数是MPSi/碳膜异质结构(0.22 h −1)的5倍,表明Gr作为电荷收集体,能促进光生载流子的分离和转移,是构建异质结构的上级碳材料。通过比较氙灯照射下的反应效率和通过422 nm滤光片在相同灯照射下的反应效率,证实了大部分(87.1%)的脱溴是由可见光诱导的。根据O2和N2鼓泡光催化脱溴实验结果,提出BDE-47的脱溴机理为光生电子还原脱溴。
Macroporous silicon/graphene (MPSi/Gr) heterostructure was fabricated by electrophoresis depositing Gr sheets on the surface of MPSi and then annealing the samples to improve adhesion and electrochemical property. In the photoelectrochemical measurements, MPSi/Gr heterostructure displayed stable and high photocurrent compared with MPSi. The stability profits from protection of Gr layer, and the enhancement of photocurrent is ascribed to effective photogenerated charge separation of MPSi/Gr heterostructure. The results of photocatalytic and photoelectrocatalytic debromination of BDE-47 showed MPSi/Gr possesses excellent photocatalytic capability, and this capability can be enhanced by applying a bias potential. The kinetic constant of MPSi/Gr (1.13h−1) heterostructure in photoelectrocatalytic process was five times as much as that of MPSi/carbon film heterostructure (0.22h−1), indicating Gr, as a charge collector which can promote separation and transfer of photogenerated carries, is superior to other carbon materials for building heterostructures. The majority (87.1%) of debromination was induced by visible light which was confirmed by comparing reaction efficiency under xenon lamp irradiation to that under the same lamp irradiation via a 422nm filter. According to the results of photocatalytic debromination experiments with O2or N2bubbling, debromination mechanism of BDE-47 was proposed as a reductive debromination by photogenerated electrons.
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