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构建具有高机械稳定性和吸附能力的三维血红素功能化石墨烯水凝胶,用于增强亚甲基蓝的光降解。

Construction of Three-Dimensional Hemin-Functionalized Graphene Hydrogel with High Mechanical Stability and Adsorption Capacity for Enhancing Photodegradation of Methylene Blue.

机构信息

Key Laboratory of Environmental Medicine Engineering, Ministry of Education, Jiangsu Engineering Laboratory of Smart Carbon-Rich Materials and Device, School of Chemistry and Chemical Engineering, Southeast University , Nanjing 211189, China.

出版信息

ACS Appl Mater Interfaces. 2017 Feb 1;9(4):4006-4014. doi: 10.1021/acsami.6b10959. Epub 2017 Jan 23.

DOI:10.1021/acsami.6b10959
PMID:28078884
Abstract

A three-dimensional hemin-functionalized graphene hydrogel (Hem/GH) was prepared by a facile self-assembly approach. The as-prepared Hem/GH showed good mechanical strength with a storage modulus of 609-642 kPa and a high adsorption capacity to organic dye contaminants (341 mg g for rhodamine B). Moreover, Hem/GH could be used as a photosensitizer for the photocatalytic degradation of organic dyes and displayed superior photodegradation activity of methylene blue (MB). This result was better than that of counterparts such as graphene hydrogel (GH) and commercial catalyst P25. The excellent cycling performance of the Hem/GH was well maintained even after multiple cycles on adsorption process and photocatalytic reaction. Interestingly, after the photodegradation of MB, a light-induced pH change of the solution from alkaline pH 8.99 to acidic pH 3.82 was observed, and 10 wt % total organic carbon remained. The liquid chromatography/time-of-flight mass spectrometry (LC/TOF-MS) analysis confirmed the generation of acidic degradation products. The photocatalytic mechanism was further investigated by trapping experiments, which revealed that the MB degradation was driven mainly by the participation of O radicals in the photocatalytic reaction. As an extended application, visually intuitive observation showed the as-prepared Hem/GH also had strong antibacterial properties. These results suggest that Hem/GH could be potentially used for practical application due to its high adsorption ability, excellent photocatalytic activity, and strong antibacterial properties.

摘要

通过一种简便的自组装方法制备了三维血红素功能化石墨烯水凝胶(Hem/GH)。所制备的 Hem/GH 具有良好的机械强度,其储能模量为 609-642 kPa,对有机染料污染物具有高吸附能力(对罗丹明 B 的吸附量为 341 mg g)。此外,Hem/GH 可用作光催化剂,用于有机染料的光催化降解,并显示出对亚甲基蓝(MB)的优越光降解活性。该结果优于石墨烯水凝胶(GH)和商业催化剂 P25 等对照物。即使在多次吸附过程和光催化反应后,Hem/GH 的出色循环性能也得到了很好的保持。有趣的是,在 MB 的光降解后,观察到溶液的光诱导 pH 值从碱性 pH 8.99 变为酸性 pH 3.82,且仍残留 10 wt %的总有机碳。液相色谱/飞行时间质谱(LC/TOF-MS)分析证实了酸性降解产物的生成。通过捕获实验进一步研究了光催化机制,结果表明,MB 的降解主要是由光催化反应中 O 自由基的参与驱动的。作为扩展应用,直观观察表明,所制备的 Hem/GH 还具有很强的抗菌性能。这些结果表明,由于其高吸附能力、优异的光催化活性和强抗菌性能,Hem/GH 可能有潜力用于实际应用。

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