A unique CoS-graphene sheet-on-sheet nanocomposite has been successfully prepared by anchoring CoS nanosheets on the surface of graphene nanosheets (GNS) with the assistance of the structure-directing agent of ethylenediamine. The shape and size of the introduced CoS nanosheets can be further adjusted by varying the amount of GNS. The unprecedented sheet-like CoS structure is believed to be matched well with GNS basically due to their similar two-dimensional structure with maximum contact areas between two components. The strong interaction between CoS and the underlying highly conductive graphene can facilitate fast electron and ion transport and improve structure stability of the composite. The composite with 26.2% GNS displays excellent electrochemical performance when evaluated as an anode for rechargeable lithium-ion battery. A larger-than-theoretical reversible capacity of 898 mAh/g can be delivered after 80 cycles at 0.1 C along with excellent highrate cycling performance. The CoS-graphene sheet-on-sheet composite is also used for the first time as a photocatalyst with promising properties for the degradation of methylene blue.

Solar energy is the most abundant renewable energy available to the earth and can meet the energy needs of humankind, but efficient conversion of solar energy to electricity is an urgent issue of scientific research. As the third-generation photovoltaic technology, dye-sensitized solar cells (DSSCs) have gained great attention since the landmark efficiency of ∼7% reported by O'Regan and Grätzel. The most attractive features of DSSCs include low cost, simple manufacturing processes, medium-purity materials, and theoretically high power conversion efficiencies. As one of the key materials in DSSCs, the counter electrode (CE) plays a crucial role in completing the electric circuit by catalyzing the reduction of the oxidized state to the reduced state for a redox couple (e.g., I/I) in the electrolyte at the CE-electrolyte interface. To lower the cost caused by the typically used Pt CE, which restricts the large-scale application because of its low reserves and high price, great effort has been made to develop new CE materials alternative to Pt. A lot of Pt-free electrocatalysts, such as carbon materials, inorganic compounds, conductive polymers, and their composites with good electrocatalytic activity, have been applied as CEs in DSSCs in the past years. Metal selenides have been widely used as electrocatalysts for the oxygen reduction reaction and light-harvesting materials for solar cells. Our group first expanded their applications to the DSSC field by using in situ-grown CoSe nanosheet and NiSe nanoparticle films as CEs. This finding has inspired extensive studies on developing new metal selenides in order to seek more efficient CE materials for low-cost DSSCs, and a lot of meaningful results have been achieved in the past years. In this Account, we summarize recent advances in binary and mutinary metal selenides applied as CEs in DSSCs. The synthetic methods for metal selenides with various morphologies and stoichiometric ratios and deposition methods for CE films are described. We emphasize that the in situ growth method exhibits advantages over other methods for fabricating stable and efficient CEs. We focus on the effect of morphology on the electocatalytic and photovoltaic performance. Application of transparent metal selenide CEs in bifacial DSSCs and the superiority of in situ-grown metal selenide nanosheet fiber CEs used for fiber DSSCs are presented. In addition, we show that metal selenides with a hollow sphere structure can function not only as an efficient electrocatalyst but also as a light-scattering layer. Finally, we present our views on the current challenges and future development of metal selenide CE materials.

Novel ZnIn2S4–g-C3N4 sheet-on-sheet nanocomposites with excellent photocatalytic activities have been synthesized by a facile hydrothermal method.

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In this study, a visible light responsive Cu3SnS4/reduced graphene oxide (RGO) photocatalyst has been synthesized by a facile one-step solvothermal method. The as-synthesized samples were characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM), high-resolution transmission electron microscopy (HRTEM), energy-dispersive X-ray spectroscopy (EDS), X-ray photoelectron spectroscopy (XPS), Raman spectroscopy, N2 adsorption-desorption, UV-vis diffuse reflectance spectra (DRS), and photoluminescence (PL) emission spectroscopy. The photocatalytic activity of the Cu3SnS4/RGO composite under visible-light irradiation (λ > 420 nm) was evaluated by measuring the degradation of rhodamine B (RhB) and phenol. The results revealed that the Cu3SnS4 nanoplates dispersed uniformly on the RGO surface. The Cu3SnS4/RGO composite exhibited much higher photocatalytic activity than pure Cu3SnS4. The enhancement in photocatalytic activity is likely to be due to the synergistic effect of an improved adsorptivity of pollutants, an enhanced visible light absorption and an effective charge separation. In addition, the Cu3SnS4/RGO photocatalyst was stable during the reaction and could be used repeatedly.

Novel visible-light-driven Cd0.2Zn0.8S/g-C3N4 inorganic-organic composite photocatalysts were synthesized by a facile hydrothermal method. The prepared Cd0.2Zn0.8S/g-C3N4 composites were characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), Fourier transform infrared spectroscopy (FT-IR), transmission electron microscopy (TEM), high-resolution transmission electron microscopy (HRTEM), ultraviolet-visible diffuse reflection spectroscopy (DRS), photoluminescence (PL) spectroscopy and photoelectrochemical (PEC) experiments. Under visible-light irradiation, Cd0.2Zn0.8S/g-C3N4 photocatalysts displayed a higher photocatalytic activity than pure g-C3N4 and Cd0.2Zn0.8S for hydrogen evolution and degradation of pollutants, and the optimal g-C3N4 content was 20 wt%. The optimal composite showed a hydrogen evolution rate of 208.0 μmol h(-1). The enhancement of the photocatalytic activity should be attributed to the well-matched band structure and intimate contact interfaces between Cd0.2Zn0.8S and g-C3N4, which lead to the effective transfer and separation of the photogenerated charge carriers. Furthermore, the Cd0.2Zn0.8S/g-C3N4 photocatalysts showed excellent stability during photocatalytic hydrogen evolution and degradation of pollutants.

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