Globally increasing energy demands and environmental concerns related to the use of fossil fuels have stimulated extensive research to identify new energy systems and economies that are sustainable, clean, low cost, and environmentally benign. Hydrogen generation from solar-driven water splitting is a promising strategy to store solar energy in chemical bonds. The subsequent combustion of hydrogen in fuel cells produces electric energy, and the only exhaust is water. These two reactions compose an ideal process to provide clean and sustainable energy. In such a process, a hydrogen evolution reaction (HER), an oxygen evolution reaction (OER) during water splitting, and an oxygen reduction reaction (ORR) as a fuel cell cathodic reaction are key steps that affect the efficiency of the overall energy conversion. Catalysts play key roles in this process by improving the kinetics of these reactions. Porphyrin-based and corrole-based systems are versatile and can efficiently catalyze the ORR, OER, and HER. Becau...

Energy-Related Small Molecule Activation Reactions: Oxygen Reduction and Hydrogen and Oxygen Evolution Reactions Catalyzed by Porphyrin- and Corrole-Based Systems

Composite Photocatalysts Nan Zhang,†,‡ Min-Quan Yang,†,‡ Siqi Liu,†,‡ Yugang Sun,* and Yi-Jun Xu*,†,‡ †State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou 350002, P.R. China ‡College of Chemistry, New Campus, Fuzhou University, Fuzhou 350108, P.R. China Center for Nanoscale Materials, Argonne National Laboratory, 9700 South Cass Avenue, Argonne, Illinois 60439, United States

Waltzing with the Versatile Platform of Graphene to Synthesize Composite Photocatalysts.

Hydrogen production from solar water splitting has been considered as an ultimate solution to the energy and environmental issues. Over the past few years, graphene has made great contribution to improving the light-driven hydrogen generation performance. This article provides a comprehensive overview of the recent research progress on graphene-based materials for hydrogen evolution from light-driven water splitting. It begins with a brief introduction of the current status and basic principles of hydrogen generation from solar water splitting, and tailoring properties of graphene for application in this area. Then, the roles of graphene in hydrogen generation reaction, including an electron acceptor and transporter, a cocatalyst, a photocatalyst, and a photosensitizer, are elaborated respectively. After that, the comparison between graphene and other carbon materials in solar water splitting is made. Last, this review is concluded with remarks on some challenges and perspectives in this emerging field.

Graphene-Based Materials for Hydrogen Generation from Light-Driven Water Splitting†

Adsorptive removal of methylene blue by rhamnolipid-functionalized graphene oxide from wastewater.

Photocatalytic water splitting by solar light has received tremendous attention for the production of clean and renewable hydrogen energy from water. Some challenges still remain in improving the solar-to-hydrogen energy conversion efficiency, such as utilizing longer-wavelength photons and enhancing the photocatalytic activity and stability of H2 production over semiconducting materials. Dye sensitization, as a successful strategy for extending the spectral responsive region (even to near-IR light) of wide bandgap semiconductors for H2 production, was developed more than 30 years ago, but it still lacks the corresponding specialized review. This review emphasizes especially the fundamental aspects and the research advances in heterogeneous dye-sensitized semiconductor suspension systems for visible (and even near-IR) light responsive photocatalytic H2 production, and the commonly used dyes, semiconductors, co-catalysts and electron donors are systematically discussed. Also, a short perspective on the challenges and new directions in this field is proposed, which would be of great interest in the field of solar fuel conversion.

Recent advances in dye-sensitized semiconductor systems for photocatalytic hydrogen production

In this paper, a 5,10,15,20-tetrakis(4-(hydroxyl)phenyl) porphyrin (TPPH) noncovalently functionalized reduced graphene oxide (RGO) nanohybrid has been facilely synthesized by immobilizing TPPH on RGO nanosheets. This nanohybrid was characterized by atomic force microscopy (AFM), transmission electron microscopy (TEM), and UV–vis spectra, which demonstrated that the TPPH molecule was attached on the surface of the graphene nanosheet. The results of fluorescence quenching and photocurrent enhancement of TPPH–RGO exhibit that the fast electrons transfer from photoexcited TPPH molecules to RGO sheets. Compared with bare TPPH or RGO functional Pt nanoparticles, the TPPH-sensitized RGO loaded with Pt nanoparticles shows remarkable enhanced photocatalytic activity under UV–vis light irradiation. The superior electron-accepting and electron-transporting properties of graphene greatly accelerate the electron transfer from excited TPPH to Pt catalysts, which promote the photocatalytic activity for hydrogen evoluti...

Surfactant Assistance in Improvement of Photocatalytic Hydrogen Production with the Porphyrin Noncovalently Functionalized Graphene Nanocomposite

Herein, we report an efficient photocatalytic hydrogen evolution system based on Ru-tris(dicarboxybipyridine)–reduced graphene oxide (Ru(dcbpy)3–RGO) hybrid. AFM images and UV-vis spectra validate Ru(dcbpy)3 functionalized RGO via noncovalent interactions. Fluorescence and Raman spectra suggest that Ru(dcbpy)3 acts as an electron donor and RGO serves as an electron acceptor in the hybridized species. Moreover, the photocurrent experiment further confirms that the photoelectrons transfer from Ru(dcbpy)3 to RGO nanosheets and then flow to deposited Pt nanoparticles effectively. Compared with the corresponding single-component Ru(dcbpy)3 and RGO nanosheets, the Ru(dcbpy)3–RGO hybrid displays distinctly enhanced photocatalytic activities under UV-vis or visible light irradiation. Therein, RGO acts as a solid-state electron mediator, which facilitates charge separation and suppresses recombination of photoexcited electron–hole pairs in RGO–Ru(dcbpy)3. Furthermore, the effect of reaction parameters such as pH, the composition of the hybrid and the stability of catalytic performance are also investigated. This study might initiate new possibilities for the development of novel graphene-based photocatalysts with enhanced activity via facile noncovalent modification of graphene with organic photosensitizers.

Enhanced photocatalytic hydrogen evolution performance based on Ru-trisdicarboxybipyridine-reduced graphene oxide hybrid

A novel nanohybrid composed of bipyridine ruthenium complex ((2,2′-bipyridyl)-4-pyridyl-chloro-ruthenium(II), Ru(bpy)2(py)Cl), covalently functionalized graphene (Ru(bpy)2(py)Cl/G), has been synthesized successfully via coordination of Ru(bpy)2Cl2 with pyridine covalently functionalized graphene (py/G), which was synthesized through 1,3-dipolar cycloaddition of azomethine ylides. Ru(bpy)2(py)Cl/G was characterized by atomic force microscopy (AFM), scanning electron microscopy (SEM), transmission electron microscopy (TEM), Raman spectra, Fourier transform infrared (FTIR), and ultraviolet–visible absorption (UV–vis). The fluorescence quenching efficiency of the nanohybrid excited at 290 and 535 nm was calculated to be 83% and 71%, respectively. The photocurrent density of the nanohybrid also significantly improved. The results revealed that fast photoinduced electron transfer from Ru(bpy)2(py)Cl moiety to graphene sheet occurred. Ru(bpy)2(py)Cl/G modified with platinum nanoparticles demonstrates remarkable ...

Improved Superiority by Covalently Binding Dye to Graphene for Hydrogen Evolution from Water under Visible-Light Irradiation

A stable and efficient photocatalytic hydrogen evolution system based on covalently linked silicon-phthalocyanine-graphene with surfactant

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Surfactant Assistance in Improvement of Photocatalytic Hydrogen Production with the Porphyrin Noncovalently Functionalized Graphene Nanocomposite

Enhanced photocatalytic hydrogen evolution performance based on Ru-trisdicarboxybipyridine-reduced graphene oxide hybrid

Improved Superiority by Covalently Binding Dye to Graphene for Hydrogen Evolution from Water under Visible-Light Irradiation

A stable and efficient photocatalytic hydrogen evolution system based on covalently linked silicon-phthalocyanine-graphene with surfactant