Keyou Yan

A Strongly Coupled Graphene and FeNi Double Hydroxide Hybrid as an Excellent Electrocatalyst for the Oxygen Evolution Reaction

Cost-effective electrocatalysts for the oxygen evolution reaction (OER) are critical to energy conversion and storage processes. A novel strategy is used to synthesize a non-noble-metal-based electrocatalyst of the OER by finely combining layered FeNi double hydroxide that is catalytically active and electric conducting graphene sheets, taking advantage of the electrostatic attraction between the two positively charged nanosheets. The synergy between the catalytic activity of the double hydroxide and the enhanced electron transport arising from the graphene resulted in superior electrocatalytic properties of the FeNi-GO hybrids for the OER with overpotentials as low as 0.21 V, which was further reduced to 0.195 V after the reduction treatment. Moreover, the turnover frequency at the overpotential of 0.3 V has reached 1 s(-1), which is much higher than those previously reported for non-noble-metal-based electrocatalysts.

All-solid-state hybrid solar cells based on a new organometal halide perovskite sensitizer and one-dimensional TiO2 nanowire arrays

A novel organometal halide perovskite (CH3NH3PbI2Br) is synthesized and used as a visible light absorber to sensitize one-dimensional (1D) TiO2 nanowire arrays (NWAs) for all-solid-state hybrid solar cells. It achieved a power conversion efficiency (PCE) of 4.87% and an open circuit voltage (Voc) of 0.82 V, both higher than those of its analogue CH3NH3PbI3.

Secondary branching and nitrogen doping of ZnO nanotetrapods: Building a highly active network for photoelectrochemical water splitting

A photoanode based on ZnO nanotetrapods, which feature good vectorial electron transport and network forming ability, has been developed for efficient photoelectrochemical water splitting. Two strategies have been validated in significantly enhancing light harvesting. The first was demonstrated through a newly developed branch-growth method to achieve secondary and even higher generation branching of the nanotetrapods. Nitrogen-doping represents the second strategy. The pristine ZnO nanotetrapod anode yielded a photocurrent density higher than those of the corresponding nanowire devices reported so far. This photocurrent density was significantly increased for the new photoanode architecture based on the secondary branched ZnO nanotetrapods. After N-doping, the photocurrent density enjoyed an even more dramatic enhancement to 0.99 mA/cm(2) at +0.31 V vs Ag/AgCl. The photocurrent enhancement is attributed to the greatly increased roughness factor for boosting light harvesting associated with the ZnO nanotetrapod branching, and the increased visible light absorption due to the N-doping induced band gap narrowing of ZnO.

Synthesis of Size-Tunable Anatase TiO2 Nanospindles and Their Assembly into Anatase@Titanium Oxynitride/Titanium Nitride−Graphene Nanocomposites for Rechargeable Lithium Ion Batteries with High Cycling Performance

This paper embarks upon three levels of undertaking ranging from nanomaterials synthesis to assembly and functionalization. First, we have prepared size-tunable anatase TiO(2) nanospindles via a hydrothermal process by using tubular titanates as self-sacrificing precursors. Second, we have densely dispersed the TiO(2) nanospindles onto functional graphene oxides (GO) via a spontaneous self-assembly process. After annealing of the TiO(2)/GO hybrid nanocomposite in an NH(3) gas flow, the TiO(2) surface was effectively nitridated and the GO was reduced to graphene sheets (GS) in order to further fortify the electronic functionality of the nanocomposite. Third, the anatase@oxynitride/titanium nitride-GS (TiO(2)@TiO(x)N(y)/TiN-GS) hybrid nanocomposite was studied as an anode material for lithium-ion batteries (LIBs), showing excellent rate capability and cycling performance compared to the pure TiO(2) nanospindles. Our systematic studies have revealed that the TiO(2)@TiO(x)N(y)/TiN-GS nanocomposites with graphene nanosheets covered with the TiO(2)@TiO(x)N(y)/TiN nanospindles on both sides provide a promising solution to the problems of poor electron transport and severe aggregation of TiO(2) nanoparticles by enhancing both electron transport through the conductive matrix and Li-ion accessibility to the active material from the liquid electrolyte. More generally, the size-tunable TiO(2) nanospindles with their unique (101) outer surface planes provide an archetype for the in depth investigation of their surface-specific and size-dependent physicochemical properties.

Hybrid Halide Perovskite Solar Cell Precursors: Colloidal Chemistry and Coordination Engineering behind Device Processing for High Efficiency

The precursor of solution-processed perovskite thin films is one of the most central components for high-efficiency perovskite solar cells. We first present the crucial colloidal chemistry visualization of the perovskite precursor solution based on analytical spectra and reveal that perovskite precursor solutions for solar cells are generally colloidal dispersions in a mother solution, with a colloidal size up to the mesoscale, rather than real solutions. The colloid is made of a soft coordination complex in the form of a lead polyhalide framework between organic and inorganic components and can be structurally tuned by the coordination degree, thereby primarily determining the basic film coverage and morphology of deposited thin films. By utilizing coordination engineering, particularly through employing additional methylammonium halide over the stoichiometric ratio for tuning the coordination degree and mode in the initial colloidal solution, along with a thermal leaching for the selective release of excess methylammonium halides, we achieved full and even coverage, the preferential orientation, and high purity of planar perovskite thin films. We have also identified that excess organic component can reduce the colloidal size of and tune the morphology of the coordination framework in relation to final perovskite grains and partial chlorine substitution can accelerate the crystalline nucleation process of perovskite. This work demonstrates the important fundamental chemistry of perovskite precursors and provides genuine guidelines for accurately controlling the high quality of hybrid perovskite thin films without any impurity, thereby delivering efficient planar perovskite solar cells with a power conversion efficiency as high as 17% without distinct hysteresis owing to the high quality of perovskite thin films.

Inkjet Printing and Instant Chemical Transformation of a CH3NH3PbI3/Nanocarbon Electrode and Interface for Planar Perovskite Solar Cells

A planar perovskite solar cell that incorporates a nanocarbon hole-extraction layer is demonstrated for the first time by an inkjet printing technique with a precisely controlled pattern and interface. By designing the carbon plus CH3NH3I ink to transform PbI2 in situ to CH3NH3PbI3, an interpenetrating seamless interface between the CH3NH3PbI3 active layer and the carbon hole-extraction electrode was instantly constructed, with a markedly reduced charge recombination compared to that with the carbon ink alone. As a result, a considerably higher power conversion efficiency up to 11.60% was delivered by the corresponding solar cell. This method provides a major step towards the fabrication of low-cost, large-scale, metal-electrode-free but still highly efficient perovskite solar cells.

Cost-efficient clamping solar cells using candle soot for hole extraction from ambipolar perovskites

Ambient-unstable hole transporters and expensive and complicated noble metal electrode deposition are incompatible with the large scale and low-cost production of perovskite solar cells and thus would hamper their commercialization. Herein we report a new modality of perovskite solar cells that do away with the use of conventional hole transporters by directly clamping a selective hole extraction electrode made of candle soot and a deliberately engineered perovskite photoanode. The key soot/perovskite interface, which promotes hole extraction and electron blocking by forming a Schottky junction, was established seamlessly by pre-wetting and reaction embedding the carbon particles. Femtosecond time-resolved photoluminescence revealed a high hole extraction rate at 1.92 ns−1. We have now achieved 11.02% efficiency, making an important step towards roll-to-roll production of perovskite solar cells.

A double layered photoanode made of highly crystalline TiO2 nanooctahedra and agglutinated mesoporous TiO2 microspheres for high efficiency dye sensitized solar cells

We report the development of a novel double layered photoanode for dye sensitized solar cells made of highly crystalline TiO2 octahedral nanocrystals and agglutinated mesoporous TiO2 microspheres. The underlayer of nanooctahedra serves as a transparent photoanode for copious and strong dye adsorption on the smooth (101) surfaces and for facilitated electron transport. Although the nanooctahedra are extremely small, our synthetic route has ensured a well-faceted crystalline shape with sharp edges and smooth surfaces, resulting in a 7.61% power conversion efficiency, much higher than that of P25 (5.76%). Separately, the overlayer of hierarchical TiO2 mesoporous microspheres plays the multiple roles of efficient light scattering, dye absorption and electrolyte permeation. Especially noteworthy is the agglutination of the microspheres through our 3D necking process, which has yielded an electron diffusion coefficient five times that of the P25 network and four times that of the nanooctahedra network. This is a significant breakthrough in DSSCs, which ensures that the photogenerated electrons in the overlayer can be effectively transported through such highway-like paths and ultimately collected at the FTO electrode. Therefore, in this double layered photoanode we have taken into consideration a number of disparate factors aimed at enhancing the overall DSSC performance. Drawing on the judicious combination of materials synthesis and engineering of nano-architectures and interfaces, solar cells based on this double layered structure have achieved 8.72% power conversion efficiency even with simple device fabrication procedures, showing promise as a new photoanode design for high efficiency dye sensitized solar cells.

Morphology-conserved transformation: synthesis of hierarchical mesoporous nanostructures of Mn2O3 and the nanostructural effects on Li-ion insertion/deinsertion properties

By means of morphology-conserved transformation, we have synthesized hierarchically structured Mn2O3 nanomaterials with different morphologies and pore structures. The key step of this method consists of the formation of a precursor containing the target materials interlaced with the judiciously chosen polyol-based organic molecules, which are subsequently knocked out to generate the final nanomaterials. In the present work, two kinds of precursor morphologies, oval-shaped and straw-sheaf-shaped, have been selectively prepared by hydrothermal treatment of different functional polyol molecules (oval-shape with fructose and straw-sheaf-shape with β-cyclodextrin) and potassium permanganate. Thermal decomposition of the precursors resulted in the formation of mesoporous Mn2O3 maintaining the original morphologies, as revealed by extensive characterization. These novel hierarchical nanostructures with different pore sizes/structures prompted us to examine their potential as anode materials for lithium ion batteries (LIBs). The electrochemical results with reference to LIBs show that both of our mesoporous Mn2O3 nanomaterials deliver high reversible capacities and excellent cycling stabilities at a current density of 200 mA g−1 compared to the commercial Mn2O3 nanoparticles. Moreover, the straw-sheaf-shaped Mn2O3 exhibits a higher specific capacity and a better cycling performance than the oval-shaped one, due to the relatively higher surface area and the peculiar nanostrip structure resulting in the reduced length for lithium ion diffusion. Morphology-conserved transformation yields two kinds of hierarchical mesoporous Mn2O3 nanomaterials with high capacities and cycling stabilities for lithium ion batteries.

High‐Performance Graphene‐Based Hole Conductor‐Free Perovskite Solar Cells: Schottky Junction Enhanced Hole Extraction and Electron Blocking

Multilayered graphene and single-layered graphene are assembled onto perovskite films in the form of Schottky junctions and ohmic contacts, respectively, for the production of a graphene-based hole transporting material-free perovskite solar cell. Multilayered graphene extracts charge selectively and efficiently, delivering a higher efficiency of 11.5% than single-layered graphene (6.7%).