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硅酞菁共价功能化的、用铂纳米粒子修饰的氮掺杂超小还原氧化石墨烯用于水制氢

Silicon phthalocyanine covalently functionalized N-doped ultrasmall reduced graphene oxide decorated with Pt nanoparticles for hydrogen evolution from water.

作者信息

Huang Jie, Wu Yijie, Wang Dandan, Ma Yufei, Yue Zongkuan, Lu Yongtao, Zhang Mengxin, Zhang Zhijun, Yang Ping

机构信息

College of Chemistry, Chemical Engineering and Materials Science, Soochow University , Suzhou, 215123, China.

出版信息

ACS Appl Mater Interfaces. 2015 Feb 18;7(6):3732-41. doi: 10.1021/am508476d. Epub 2015 Feb 4.

DOI:10.1021/am508476d
PMID:25616022
Abstract

To improve the photocatalytic activity of graphene-based catalysts, silicon phthalocyanine (SiPc) covalently functionalized N-doped ultrasmall reduced graphene oxide (N-usRGO) has been synthesized through 1,3-dipolar cycloaddition of azomethine ylides. The obtained product (N-usRGO/SiPc) was characterized by transmission electron microscopy, atomic force microscopy, Fourier transform infrared spectroscopy, Raman spectra, X-ray photoelectron spectroscopy, fluorescence, and UV-vis spectroscopy. The results demonstrate that SiPc has been successfully grafted on the surface of N-usRGO. The N-usRGO/SiPc nanocomposite exhibits high light-harvesting efficiency covering a range of wavelengths from the ultraviolet to visible light. The efficient fluorescence quenching and the enhanced photocurrent response confirm that the photoinduced electron transfers from the SiPc moiety to the N-usRGO sheet. Moreover, we chose Pt nanoparticles as cocatalyst to load on N-usRGO/SiPc sheets to obtain the optimal H2 production effect. The platinized N-usRGO/SiPc (N-usRGO/SiPc/Pt) demonstrates good hydrogen evolution performance under both UV-vis and visible light (λ>400 nm) irradiation. The apparent quantum yields are 1.3% and 0.56% at 365 and 420 nm, respectively. These results reveal that N-usRGO/SiPc/Pt nanocomposite, consolidating the advantages of SiPc, N-usRGO, and Pt NPs, can be a potential candidate for hydrogen evolution from water under UV-vis or visible light irradiation.

摘要

为了提高基于石墨烯的催化剂的光催化活性,通过甲亚胺叶立德的1,3-偶极环加成反应合成了硅酞菁(SiPc)共价功能化的氮掺杂超小还原氧化石墨烯(N-usRGO)。通过透射电子显微镜、原子力显微镜、傅里叶变换红外光谱、拉曼光谱、X射线光电子能谱、荧光光谱和紫外-可见光谱对所得产物(N-usRGO/SiPc)进行了表征。结果表明,SiPc已成功接枝到N-usRGO的表面。N-usRGO/SiPc纳米复合材料在从紫外光到可见光的一系列波长范围内表现出高光捕获效率。有效的荧光猝灭和增强的光电流响应证实了光生电子从SiPc部分转移到N-usRGO片层。此外,我们选择铂纳米颗粒作为助催化剂负载在N-usRGO/SiPc片层上,以获得最佳的产氢效果。铂化的N-usRGO/SiPc(N-usRGO/SiPc/Pt)在紫外-可见光(λ>400 nm)照射下均表现出良好的析氢性能。在365和420 nm处的表观量子产率分别为1.3%和0.56%。这些结果表明,N-usRGO/SiPc/Pt纳米复合材料结合了SiPc、N-usRGO和Pt NPs的优点,可能是紫外-可见光或可见光照射下从水中析氢的潜在候选材料。

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