Yuan Hou

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.

Polyaniline-modified cetyltrimethylammonium bromide-graphene oxide-sulfur nanocomposites with enhanced performance for lithium-sulfur batteries

Conductive polymer coatings can boost the power storage capacity of lithium-sulfur batteries. We report here on the design and preparation-by combining a facile and green chemical deposition method with an oxidative polymerization approach-of polyaniline (PANI)-modified cetyltrimethylammonium bromide (CTAB)-graphene oxide (GO)-sulfur (S) nanocomposites with significantly enhanced performance in lithium-sulfur batteries. Such conductive polymer modified CTAB-GO-S nanocomposites as sulfur cathode materials can deliver high specific discharge capacities and long-term cycling performance, i.e., ∼970 mAh·g−1 at 0.2 C and ∼715 mAh·g−1 after 300 cycles, ∼820 mAh·g−1 at 0.5 C and ∼670 mAh·g−1 after 500 cycles, ∼770 mAh·g−1 at 1 C and ∼570 mAh·g−1 after 500 cycles. The capacity decay was as low as 0.036% per cycle at 0.5 C, and 0.051% per cycle at 1 C. Under the same condition, batteries using PANI-modified CTAB-GO-S as cathodes exhibited higher specific capacity and higher average coulombic efficiency compared with CTAB-decorated GO-S and GO-S nanocomposites. The improved performance can be attributed to the lower charge transfer resistance and the alleviated dissolution of polysulfides in the PANImodified CTAB-GO-S cathodes.

Synthesis of V2O5 hierarchical structures for long cycle-life lithium-ion storage

A facile solvothermal method was used to synthesize V2O5 nanosheet hierarchical structures. Using different solvent systems, we obtained the hierarchical structures with different nanosheet thicknesses of <10 nm, 50–100 nm and 100–200 nm, respectively. A systematic investigation of their electrochemical properties showed that both the reversible lithium storage capacity and the cycling stability increased with the reduced thickness of nanosheets. In order to prevent the serious structural damage of the V2O5 electrodes during cycling, we employed a voltage-regulation charge/discharge scheme which led to a long cycle-life with an average capacity decay of 0.04% (2.0 to 3.0 V) and 0.10% per cycle (2.8 to 4.0 V) over 500 cycles.

A high energy density Li2S@C nanocomposite cathode with a nitrogen-doped carbon nanotube top current collector

Lithium sulfide (Li2S), with a high theoretical capacity of 1166 mA h g−1, is considered as one of the most promising cathode materials for the next-generation lithium-ion batteries. In this work, a novel cell configuration with a top current collector was designed for Li2S based batteries. The nitrogen-doped carbon nanotube (N-CNT) film was applied on top of the cathode, which serves not only as a top current collector but also as a barrier layer to effectively impede the polysulfide diffusion and enhance the utilization of active materials. A sheet-like Li2S@C nanocomposite was synthesized from low-cost and environmentally friendly raw materials of lithium sulfate (Li2SO4) and activated graphite. The as-prepared Li2S@C composites were directly used as cathode materials without adding any binder or carbon additive, which enabled a high Li2S loading up to 68% in the total cathode weight. The cells exhibited superior electrochemical performance. The specific energy at 0.5C was 804 W h kg−1 based on the total electrode weight including the N-CNT top current collector, which is among the highest values demonstrated so far for sulfur and Li2S cathodes.

Liquid‐Phase Electrochemical Scanning Electron Microscopy for In Situ Investigation of Lithium Dendrite Growth and Dissolution

An in situ electrochemical scanning electronic microscopy method is developed to systematically study the lithium plating/stripping processes in liquid electrolytes. The results demonstrate that the lithium dendrite growth speed and mechanism is greatly affected by the additives in the ether-based electrolyte.

All-Solid-State High-Energy Asymmetric Supercapacitors Enabled by Three-Dimensional Mixed-Valent MnOx Nanospike and Graphene Electrodes

Three-dimensional (3D) nanostructures enable high-energy storage devices. Here we report a 3D manganese oxide nanospike (NSP) array electrode fabricated by anodization and subsequent electrodeposition. All-solid-state asymmetric supercapacitors were assembled with the 3D Al@Ni@MnOx NSP as the positive electrode, chemically converted graphene (CCG) as the negative electrode, and Na2SO4/poly(vinyl alcohol) (PVA) as the polymer gel electrolyte. Taking advantage of the different potential windows of Al@Ni@MnOx NSP and CCG electrodes, the asymmetric supercapacitor showed an ideal capacitive behavior with a cell voltage up to 1.8 V, capable of lighting up a red LED indicator (nominal voltage of 1.8 V). The device could deliver an energy density of 23.02 W h kg(-1) at a current density of 1 A g(-1). It could also preserve 96.3% of its initial capacitance at a current density of 2 A g(-1) after 10000 charging/discharging cycles. The remarkable performance is attributed to the unique 3D NSP array structure that could play an important role in increasing the effective electrode surface area, facilitating electrolyte permeation, and shortening the electron pathway in the active materials.