Shihe Yang

Design Hierarchical Electrodes with Highly Conductive NiCo2S4 Nanotube Arrays Grown on Carbon Fiber Paper for High-Performance Pseudocapacitors

We report on the development of highly conductive NiCo2S4 single crystalline nanotube arrays grown on a flexible carbon fiber paper (CFP), which can serve not only as a good pseudocapacitive material but also as a three-dimensional (3D) conductive scaffold for loading additional electroactive materials. The resulting pseudocapacitive electrode is found to be superior to that based on the sibling NiCo2O4 nanorod arrays, which are currently used in supercapacitor research due to the much higher electrical conductivity of NiCo2S4. A series of electroactive metal oxide materials, including CoxNi1-x(OH)2, MnO2, and FeOOH, were deposited on the NiCo2S4 nanotube arrays by facile electrodeposition and their pseudocapacitive properties were explored. Remarkably, the as-formed CoxNi1-x(OH)2/NiCo2S4 nanotube array electrodes showed the highest discharge areal capacitance (2.86 F cm(-2) at 4 mA cm(-2)), good rate capability (still 2.41 F cm(-2) at 20 mA cm(-2)), and excellent cycling stability (∼ 4% loss after the repetitive 2000 cycles at a charge-discharge current density of 10 mA cm(-2)).

Highly monodisperse polymer-capped ZnO nanoparticles: Preparation and optical properties

We report the preparation of highly monodisperse ZnO nanoparticles using poly(vinyl pyrrolidone) (PVP) as the capping molecules. The surface-modified ZnO nanoparticles were found to be remarkably stable. The optical absorption shows distinct excitonic features. Markedly enhanced near-band-edge ultraviolet photoluminescence and significantly reduced defect-related green emission were also observed. We attribute this observation to the nearly perfect surface passivation of the ZnO nanoparticles by the PVP molecules. The third-order nonlinear optical response of these PVP-capped ZnO nanoparticles in a dilute solution was found to be significantly larger (by at least two orders of magnitude) than that of the bulk ZnO.

High-Rate, Ultralong Cycle-Life Lithium/Sulfur Batteries Enabled by Nitrogen-Doped Graphene

Nitrogen-doped graphene (NG) is a promising conductive matrix material for fabricating high-performance Li/S batteries. Here we report a simple, low-cost, and scalable method to prepare an additive-free nanocomposite cathode in which sulfur nanoparticles are wrapped inside the NG sheets (S@NG). We show that the Li/S@NG can deliver high specific discharge capacities at high rates, that is, ∼ 1167 mAh g(-1) at 0.2 C, ∼ 1058 mAh g(-1) at 0.5 C, ∼ 971 mAh g(-1) at 1 C, ∼ 802 mAh g(-1) at 2 C, and ∼ 606 mAh g(-1) at 5 C. The cells also demonstrate an ultralong cycle life exceeding 2000 cycles and an extremely low capacity-decay rate (0.028% per cycle), which is among the best performance demonstrated so far for Li/S cells. Furthermore, the S@NG cathode can be cycled with an excellent Coulombic efficiency of above 97% after 2000 cycles. With a high active S content (60%) in the total electrode weight, the S@NG cathode could provide a specific energy that is competitive to the state-of-the-art Li-ion cells even after 2000 cycles. The X-ray spectroscopic analysis and ab initio calculation results indicate that the excellent performance can be attributed to the well-restored C-C lattice and the unique lithium polysulfide binding capability of the N functional groups in the NG sheets. The results indicate that the S@NG nanocomposite based Li/S cells have a great potential to replace the current Li-ion batteries.

Facile Ultrasonic Synthesis of CoO Quantum Dot/Graphene Nanosheet Composites with High Lithium Storage Capacity

In this paper, we report a facile ultrasonic method to synthesize well-dispersed CoO quantum dots (3-8 nm) on graphene nanosheets at room temperature by employing Co(4)(CO)(12) as cobalt precursor. The prepared CoO/graphene composites displayed high performance as an anode material for lithium-ion battery, such as high reversible lithium storage capacity (1592 mAh g(-1) after 50 cycles), high Coulombic efficiency (over 95%), excellent cycling stability, and high rate capability (1008 mAh g(-1) with a total retention of 77.6% after 50 cycles at a current density of 1000 mA g(-1), dramatically increased from the initial 50 mA g(-1)). The extraordinary performance arises from the structure advantages of the composites: the nanosized CoO quantum dots with high dispersity on conductive graphene substrates supply not only large quantity of accessible active sites for lithium-ion insertion but also good conductivity and short diffusion length for lithium ions, which are beneficial for high capacity and rate capability. Meanwhile, the isolated CoO quantum dots anchored tightly on the graphene nanosheets can effectively circumvent the volume expansion/contraction associated with lithium insertion/extraction during discharge/charge processes, which is good for high capacity as well as cycling stability. Moreover, regarding the anomalous behavior of capacity increase with cycles (activation effect) observed, we proposed a tentative hypothesis stressing the competition between the conductivity increase and the amorphorization of the composite electrodes during cycling in determining the trends of the capacity, in the hope to gain a fuller understanding of the inner working of the novel nanostructured electrode-based lithium-ion batteries.

Facile synthesis of water-soluble, highly fluorescent graphene quantum dots as a robust biological label for stem cells

We present a facile electrochemical method for synthesizing uniform sized graphene quantum dots (GQDs) with a strong yellow emission at 14% quantum yield. This approach has enabled a large-scale production of aqueous GQD solution without the need for polymeric or surfactant stabilizers. The structure and emission mechanism of the GQDs have been studied by combining extensive characterization techniques, rigorous control experiments and theoretical calculations. We further demonstrate the distinctive advantages of such GQDs for direct and efficient stem cell labeling, opening up great opportunities for their bio-medical applications.

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.

Efficiency Enhancement of Perovskite Solar Cells through Fast Electron Extraction: The Role of Graphene Quantum Dots

We report on a significant power conversion efficiency improvement of perovskite solar cells from 8.81% to 10.15% due to insertion of an ultrathin graphene quantum dots (GQDs) layer between perovskite and TiO2. A strong quenching of perovskite photoluminescence was observed at ∼760 nm upon the addition of the GQDs, which is pronouncedly correlated with the increase of the IPCE and the APCE of the respective cells. From the transient absorption measurements, the improved cell efficiency can be attributed to the much faster electron extraction with the presence of GQDs (90-106 ps) than without their presence (260-307 ps). This work highlights that GQDs can act as a superfast electron tunnel for optoelectronic devices.

UPS of Buckminsterfullerene and other large clusters of carbon

Abstract Ultraviolet photoelectron spectra (UPS) are reported for mass-selected negative carbon clusters extracted from a pulsed supersonic beam. In the size range from 48 to 84 atoms, three clusters were found to be closed-shell species with appreciable HOMO-LUMO gaps: C 50 (0.3–0.6 eV), C 60 (1.5–2.0 eV), and C 70 (0.7–1.2 eV). UPS data for all other clusters revealed no appreciable HOMO-LUMO gap, indicating they are either open-shell species, or closed-shell species with small HOMO-LUMO gaps. Buckminsterfullerene (C 60 ) was found to have the lowest electron affinity (2.6–2.8 eV) of any cluster. Agreement between these UPS data and electronic structure calculations strongly support the spheroidal shell model for C 60 .

UPS of 2–30-atom carbon clusters: Chains and rings

Abstract Ultraviolet photoelectron spectra (UPS) of negative carbon clusters are reported in the size range from 2 through 29 atoms. The clusters were prepared in a supersonic beam by laser vaporization, and a F 2 excimer laser (7.9 eV) was used for photodetachment. The resultant UPS data indicate that carbon clusters in the 2–9-atom size range take the form of linear chains: the even-numbered chains having open shell electronic structures with high electron affinity, the odd chains having closed shell singlet ground states (for the neutral) and substantially lower electron affinity. Clusters in the 10–29-atom range give UPS patterns consistent with a monocyclic ring structure.

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.