The cathode materials work as the host framework for both Li + diffusion and electron transport in Liion batteries. The Li + diffusion property is always the research focus, while the electron transport property is less studied. Herein, we propose a unique strategy to elevate the rate performance through promoting the surface electric conductivity. Specifically, a disordered rock-salt phase was coherently constructed at the surface of LiCoO 2 , promoting the surface electric conductivity by over one magnitude. It increased the effective voltage (V eff ) imposed in the bulk, thus driving more Li + extraction/insertion and making LiCoO 2 exhibit superior rate capability (154 mAh g À 1 at 10 C), and excellent cycling performance (93 % after 1000 cycles at 10 C). The universality of this strategy was confirmed by another surface design and a simulation. Our findings provide a new angle for developing high-rate cathode materials by tuning the surface electron transport property.
Solar-driven N2 fixation using a photocatalyst in water presents a promising alternative to the traditional Haber-Bosch process in terms of both energy efficiency and environmental concern. At present, the product of solar N2 fixation is either NH4+ or NO3-. Few reports described the simultaneous formation of ammonia (NH4+) and nitrate (NO3-) by a photocatalytic reaction and the related mechanism. In this work, we report a strategy to photocatalytically fix nitrogen through simultaneous reduction and oxidation to produce NH4+ and NO3- by W18O49 nanowires in pure water. The underlying mechanism of wavelength-dependent N2 fixation in the presence of surface defects is proposed, with an emphasis on oxygen vacancies that not only facilitate the activation and dissociation of N2 but also improve light absorption and the separation of the photoexcited carriers. Both NH4+ and NO3- can be produced in pure water under a simulated solar light and even till the wavelength reaching 730 nm. The maximum quantum efficiency reaches 9% at 365 nm. Theoretical calculation reveals that disproportionation reaction of the N2 molecule is more energetically favorable than either reduction or oxidation alone. It is worth noting that the molar fraction of NH4+ in the total product (NH4+ plus NO3-) shows an inverted volcano shape from 365 nm to 730 nm. The increased fraction of NO3- from 365 nm to around 427 nm results from the competition between the oxygen evolution reaction (OER) at W sites without oxygen vacancies and the N2 oxidation reaction (NOR) at oxygen vacancy sites, which is driven by the intrinsically delocalized photoexcited holes. From 427 nm to 730 nm, NOR is energetically restricted due to its higher equilibrium potential than that of OER, accompanied by the localized photoexcited holes on oxygen vacancies. Full disproportionation of N2 is achieved within a range of wavelength from ~427 nm to ~515 nm. This work presents a rational strategy to efficiently utilize the photoexcited carriers and optimize the photocatalyst for practical nitrogen fixation.
Conductive nanocarbons generally are used as the electronic conductive additives to contact with active materials to generate conductive network for electrodes of commercial Li-ion batteries (LIBs). A typical of LiFePO 4 (LFP), which has been widely used as cathode material for LIBs with low electronic conductivity, needs higher quantity of conductive nanocarbons to enhance the performance for cathode electrodes. In this work, we systematically studied three types of conductive nanocarbons and related performances in the LFP electrodes, and classify them as hard/soft-contact conductive carbon (named as H/SCC), respectively, according to their crystallite size, surface graphite-defect, specific surface area and porous structure, in which SCC can generate much larger contact area with active nano-particles of cathode materials than that of HCC. It is found that LFP nanocrystals wrapped in SCC networks perform significantly enhanced both capacity and rate performance than that in HCC. Combined experiments with multiphysics simulation, the mechanism is that LFP nanoparticles embedded in SCC with large contact area enable to generate higher depolarized effects with a relatively uniform current density vector (i s) and lithium flux vector (N Li) than that in HCC. This discovery will guide us to how to design LIBs by selective using conductive carbon for high-performance LIBs.
We report composite electrodes with Li2FeSiO4 nanocrystals wrapped in three different types of conductive carbon, Acetylene Black, carbon nanotubes and Ketjen Black, to demonstrate depolarization effects on the electrochemical performance of Li-ion batteries.
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