Nitrate is ar aw ingredient for the production of fertilizer,g unpowder,a nd explosives.D eveloping an alternative approach to activate the NNbond of naturally abundant nitrogen to form nitrate under ambient conditions will be of importance.Herein, pothole-rich WO 3 was used to catalyse the activation of N Nc ovalent triple bonds for the direct nitrate synthesis at room temperature.T he pothole-rich structure endues the WO 3 nanosheet more dangling bonds and more easily excited high momentum electrons,w hicho vercome the two major bottlenecks in NNb ond activation, that is,p oor binding of N 2 to catalytic materials and the high energy involved in this reaction. The average rate of nitrate production is as high as 1.92 mg g À1 h À1 under ambient conditions,without any sacrificial agent or precious-metal co-catalysts.M ore generally,t he concepts will initiate an ew pathwayf or triggering inert catalytic reactions.
By scrutinizing the energy storage process in Li-ion batteries, tuning Li-ion migration behavior by atomic level tailoring will unlock great potential for pursuing higher electrochemical performance. Vacancy, which can effectively modulate the electrical ordering on the nanoscale, even in tiny concentrations, will provide tempting opportunities for manipulating Li-ion migratory behavior. Herein, taking CuGeO as a model, oxygen vacancies obtained by reducing the thickness dimension down to the atomic scale are introduced in this work. As the Li-ion storage progresses, the imbalanced charge distribution emerging around the oxygen vacancies could induce a local built-in electric field, which will accelerate the ions' migration rate by Coulomb forces and thus have benefits for high-rate performance. Furthermore, the thus-obtained CuGeO ultrathin nanosheets (CGOUNs)/graphene van der Waals heterojunctions are used as anodes in Li-ion batteries, which deliver a reversible specific capacity of 1295 mAh g at 100 mA g, with improved rate capability and cycling performance compared to their bulk counterpart. Our findings build a clear connection between the atomic/defect/electronic structure and intrinsic properties for designing high-efficiency electrode materials.
Exploring efficient and economical electrocatalysts for hydrogen evolution reaction is of great significance for water splitting on an industrial scale. Tungsten oxide, WO, has been long expected to be a promising non-precious-metal electrocatalyst for hydrogen production. However, the poor intrinsic activity of this material hampers its development. Herein, we design a highly efficient hydrogen evolution electrocatalyst via introducing oxygen vacancies into WO nanosheets. Our first-principles calculations demonstrate that the gap states introduced by O vacancies make WO act as a degenerate semiconductor with high conductivity and desirable hydrogen adsorption free energy. Experimentally, we prepared WO nanosheets rich in oxygen vacancies via a liquid exfoliation, which indeed exhibits the typical character of a degenerate semiconductor. When evaluated by hydrogen evolution, the nanosheets display superior performance with a small overpotential of 38 mV at 10 mA cm and a low Tafel slope of 38 mV dec. This work opens an effective route to develop conductive tungsten oxide as a potential alternative to the state-of-the-art platinum for hydrogen evolution.
Developing bifunctional catalysts for both hydrogen and oxygen evolution reactions is apromising approach to the practical implementation of electrocatalytic water splitting. However,m ost of the reported bifunctional catalysts are only applicable to alkaline electrolyzer,although afew are effective in acidic or neutral media that appeals more to industrial applications.H ere,alithium-intercalated iridium diselenide (Li-IrSe 2 )i sd eveloped that outperformed other reported catalysts towardo verall water splitting in both acidic and neutral environments.L ii ntercalation activated the inert pristine IrSe 2 via bringing high porosities and abundant Se vacancies for efficient hydrogen and oxygen evolution reactions.When Li-IrSe 2 was assembled into two-electrode electrolyzers for overall water splitting,t he cell voltages at 10 mA cm À2 were 1.44 and 1.50 Vu nder pH 0a nd 7, respectively,b eing record-low values in both conditions.
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