Xiaodan Huang

Functional Nanoporous Graphene Foams with Controlled Pore Sizes

A simple hydrophobic-affinity-derived assembly approach to pack graphene sheets into a nanoporous foam structure has been developed. Nanoporous graphene foams with the highest pore volume and large surface area are obtained. The pore diameter of the graphene foams can be finely adjusted from the mesopore to the macropore range by employing spherical templates with different sizes.

Porous Graphene Nanoarchitectures: An Efficient Catalyst for Low Charge-Overpotential, Long Life, and High Capacity Lithium–Oxygen Batteries

The electrochemical performance of lithium-oxygen (Li-O2) batteries awaits dramatic improvement in the design of porous cathode electrodes with sufficient spaces to accommodate the discharge products and discovery of effective cathode catalysts to promote both oxygen reduction reactions and oxygen evolution reactions. Herein, we report the synthesis of porous graphene with different pore size architectures as cathode catalysts for Li-O2 batteries. Porous graphene materials exhibited significantly higher discharge capacities than that of nonporous graphene. Furthermore, porous graphene with pore diameter around 250 nm showed the highest discharge capacity among the porous graphene with the small pores (about 60 nm) and large pores (about 400 nm). Moreover, we discovered that addition of ruthenium (Ru) nanocrystals to porous graphene promotes the oxygen evolution reaction. The Ru nanocrystal-decorated porous graphene exhibited an excellent catalytic activity as cathodes in Li-O2 batteries with a high reversible capacity of 17,700 mA h g(-1), a low charge/discharge overpotential (about 0.355 V), and a long cycle life up to 200 cycles (under the curtaining capacity of 1000 mAh g(-1)). The novel porous graphene architecture inspires the development of high-performance Li-O2 batteries.

Graphene-Co3O4 nanocomposite as electrocatalyst with high performance for oxygen evolution reaction

Graphene-Co3O4 composite with a unique sandwich-architecture was successfully synthesized and applied as an efficient electrocatalyst for oxygen evolution reaction. Field emission scanning electron microscopy (FESEM) and transmission electron microscopy (TEM) analyses confirmed that Co3O4 nanocrystals were homogeneously distributed on both sides of graphene nanosheets. The obtained composite shows enhanced catalytic activities in both alkaline and neutral electrolytes. The onset potential towards the oxygen evolution reaction is 0.406 V (vs. Ag/AgCl) in 1 M KOH solution, and 0.858 V (vs. Ag/AgCl) in neutral phosphate buffer solution (PBS), respectively. The current density of 10 mA/cm2 has been achieved at the overpotential of 313 mV in 1 M KOH and 498 mV in PBS. The graphene-Co3O4 composite also exhibited an excellent stability in both alkaline and neutral electrolytes. In particular, no obvious current density decay was observed after 10 hours testing in alkaline solution and the morphology of the material was well maintained, which could be ascribed to the synergistic effect of combining Co3O4 and graphene.

Hierarchical 3D mesoporous silicon@graphene nanoarchitectures for lithium ion batteries with superior performance

Silicon has been recognized as the most promising anode material for high capacity lithium ion batteries. However, large volume variations during charge and discharge result in pulverization of Si electrodes and fast capacity loss on cycling. This drawback of Si electrodes can be overcome by combination with well-organized graphene foam. In this work, hierarchical three-dimensional carbon-coated mesoporous Si nanospheres@graphene foam (C@Si@GF) nanoarchitectures were successfully synthesized by a thermal bubble ejection assisted chemical-vapor-deposition and magnesiothermic reduction method. The morphology and structure of the as-prepared nanocomposites were characterized by field emission scanning electron microscopy, transmission electron microscopy and Raman spectroscopy. When employed as anode materials in lithium ion batteries, C@Si@GF nanocomposites exhibited superior electrochemical performance including a high specific capacity of 1,200 mAh/g at the current density of 1 A/g, excellent high rate capabilities and an outstanding cyclability. Post-mortem analyses identified that the morphology of 3D C@Si@GF electrodes after 200 cycles was well maintained. The synergistic effects arising from the combination of mesoporous Si nanospheres and graphene foam nanoarchitectures may address the intractable pulverization problem of Si electrode.

Surfactant-Free Assembly of Mesoporous Carbon Hollow Spheres with Large Tunable Pore Sizes

Mesoporous carbon hollow spheres (MCHS) have wide applications, including catalysis, absorption, and energy storage/conversion. Herein, we report a one-pot, surfactant-free synthesis of MCHS using three molecules: resorcinol, formaldehyde, and tetrapropyl orthosilicate. The co-condensation process between the in situ generated silica primary particles and the polymer oligomers is regulated, leading to monodispersed MCHS with adjustable pore sizes from micropores to 13.9 nm. The resultant MCHS shows excellent performance for electrochemical double-layer capacitors with high capacitance (310 F g(-1) at 1 A g(-1)), excellent rate capability (157 F g(-1) at 50 A g(-1)), and outstanding cycling stability (98.6% capacity retention after 10 000 cycles at 10 A g(-1)). Our one-pot synthesis strategy is versatile and can be extended to fabricate metal oxide@mesoporous carbon yolk-shell structures in the absence of surfactant, paving the way toward designed synthesis of nanostructured mesoporous carbon composites for various applications.

A Facile One‐Step Solvothermal Synthesis of SnO2/Graphene Nanocomposite and Its Application as an Anode Material for Lithium‐Ion Batteries

Spare capacity: A SnO/graphene nanocomposite is fabricated by a novel solvothermal method (see picture). The nanocomposite exhibits a reversible lithium storage capacity of 838 mAhg in the first cycle and improved cyclability as an anode material for lithium-ion batteries.

Honeycomb-like porous gel polymer electrolyte membrane for lithium ion batteries with enhanced safety

Lithium ion batteries have shown great potential in applications as power sources for electric vehicles and large-scale energy storage. However, the direct uses of flammable organic liquid electrolyte with commercial separator induce serious safety problems including the risk of fire and explosion. Herein, we report the development of poly(vinylidene difluoride-co-hexafluoropropylene) polymer membranes with multi-sized honeycomb-like porous architectures. The as-prepared polymer electrolyte membranes contain porosity as high as 78%, which leads to the high electrolyte uptake of 86.2 wt%. The PVDF-HFP gel polymer electrolyte membranes exhibited a high ionic conductivity of 1.03 mS cm−1 at room temperature, which is much higher than that of commercial polymer membranes. Moreover, the as-obtained gel polymer membranes are also thermally stable up to 350°C and non-combustible in fire (fire-proof). When applied in lithium ion batteries with LiFePO4 as cathode materials, the gel polymer electrolyte demonstrated excellent electrochemical performances. This investigation indicates that PVDF-HFP gel polymer membranes could be potentially applicable for high power lithium ion batteries with the features of high safety, low cost and good performance.

Mesoporous graphene paper immobilised sulfur as a flexible electrode for lithium–sulfur batteries

Free-standing flexible mesoporous graphene–sulfur nanocomposite electrodes have been prepared by a sulfur vapor treatment approach. Amorphous sulfur homogeneously was distributed in the mesoporous architectures of porous graphene paper, in which sulfur was immobilized. The as-prepared mesoporous graphene–sulfur papers can be directly applied as electrodes in lithium–sulfur batteries without using a binder, conductive additives or an extra current collector. The conductive flexible porous graphene networks can effectively facilitate electron transfer and electrolyte diffusion. The free-standing sulfur–graphene nanocomposite electrodes achieved a high discharge capacity of 1393 mA h g−1 with an enhanced cycling stability and good rate performance.

Micelle-template synthesis of nitrogen-doped mesoporous graphene as an efficient metal-free electrocatalyst for hydrogen production.

Synthesis of mesoporous graphene materials by soft-template methods remains a great challenge, owing to the poor self-assembly capability of precursors and the severe agglomeration of graphene nanosheets. Herein, a micelle-template strategy to prepare porous graphene materials with controllable mesopores, high specific surface areas and large pore volumes is reported. By fine-tuning the synthesis parameters, the pore sizes of mesoporous graphene can be rationally controlled. Nitrogen heteroatom doping is found to remarkably render electrocatalytic properties towards hydrogen evolution reactions as a highly efficient metal-free catalyst. The synthesis strategy and the demonstration of highly efficient catalytic effect provide benchmarks for preparing well-defined mesoporous graphene materials for energy production applications.

Hierarchical macroporous/mesoporous NiCo2O4 nanosheets as cathode catalysts for rechargeable Li–O2 batteries

The key factor to improve the electrochemical performance of Li–O2 batteries is to find bi-functional cathode catalysts to promote the oxygen reduction and evolution reactions. Despite tremendous effects, developing cathode catalysts with high activity remains a great challenge. Herein, we report the synthesis of hierarchical macroporous/mesoporous NiCo2O4 nanosheets as an effective cathode catalyst for Li–O2 batteries. The hierarchical porous catalyst was synthesized by a hydrothermal method, followed by low temperature calcination. SEM and TEM observations clearly present that the as-prepared NiCo2O4 nanosheets showed a hierarchical porous structure with mesopores distributed through the surface of NiCo2O4 nanosheets and macropores formed between the crumpled nanosheets. When investigating as the cathode catalyst in Li–O2 batteries, the as-prepared NiCo2O4 nanosheets exhibited higher reversible capacity, lower charge/discharge overpotential, and better cycling stability than those of pristine carbon black. The enhanced electrochemical performance of NiCo2O4 nanosheets should be attributed not only to the high catalytic activity of NiCo2O4 towards oxygen reduction reaction and oxygen evolution reaction, but also to the novel hierarchical porous structure of NiCo2O4.