ABSTRACT
Silicon is an attractive anode material for lithium-ion batteries. However, silicon anodes have the issue of volume change, which causes pulverization and subsequently rapid capacity fade. Herein, we report organic binder and conducting diluent-free silicon-carbon 3D electrodes as anodes for lithium-ion batteries, where we replace the conventional copper (Cu) foil current collector with highly conductive carbon fibers (CFs) of 5-10 µm in diameter. We demonstrate here the petroleum pitch (P-pitch) which adequately coat between the CFs and Si-nanoparticles (NPs) between 700 and 1000 °C under argon atmosphere and forms uniform continuous layer of 6-14 nm thick coating along the exterior surfaces of Si-NPs and 3D CFs. The electrodes fabricate at 1000 °C deliver capacities in excess of 2000 mA h g-1 at C/10 and about 1000 mA h g-1 at 5 C rate for 250 cycles in half-cell configuration. Synergistic effect of carbon coating and 3D CF electrode architecture at 1000 °C improve the efficiency of the Si-C composite during long cycling. Full cells using Si-carbon composite electrode and Li1.2Ni0.15Mn0.55Co0.1O2-based cathode show high open-circuit voltage of >4 V and energy density of >500 W h kg-1. Replacement of organic binder and copper current collector by high-temperature binder P-pitch and CFs further enhances energy density per unit area of the electrode. It is believed that the study will open a new realm of possibility for the development of Li-ion cell having almost double the energy density of currently available Li-ion batteries that is suitable for electric vehicles.
ABSTRACT
Charge transfer at the TiO2/quantum dots (QDs) interface, charge collection at the TiO2/QDs/current collector (FTO or SnO2:F) interface, and back electron transfer at the TiO2/QDs/S2- interface are processes controlled by the electron transport layer or TiO2. These key processes control the power conversion efficiencies (PCEs) of quantum dot solar cells (QDSCs). Here, four TiO2 morphologies, porous nanoparticles (PNPs), nanowires (NWs), nanosheets (NSHs) and nanoparticles (NPs), were sensitized with CdS and the photovoltaic performances were compared. The marked differences in the cell parameters on going from one morphology to the other have been explained by correlating the shape, structure and the above-described interfacial properties of a given TiO2 morphology to the said parameters. The average magnitudes of PCEs follow the order: NWs (5.96%) > NPs (4.95%) > PNPs (4.85%) > NSHs (2.5%), with the champion cell based on NWs exhibiting a PCE of 6.29%. For NWs, an optimal balance between the fast photo-excited electron injection to NWs at the NW/CdS interface, the high resistance offered at the TiO2 NW/CdS/S2- interfaces to electron recombination with the oxidized electrolyte or with the holes in CdS, the low electron transport resistance in NWs, and low dark currents, yields the highest efficiency due to directional unhindered transport of electrons afforded by the NWs. For NSHs, electron trapping in the two dimensional sheets, and a high electron recombination rate prevent the effective transfer of electrons to FTO, thus reducing short circuit current density significantly, resulting in a poor performance. This study provides a deep understanding of charge transfer, transport and collection processes necessary for the design of efficient QDSCs.
