While sodium-ion batteries (SIBs)
hold great promise for large-scale electric energy storage and low
speed electric vehicles, the poor capacity retention of the cathode
is one of the bottlenecks in the development of SIBs. Following a
strategy of using lithium doping in the transition-metal layer to
stabilize the desodiated structure, we have designed and successfully
synthesized a novel layered oxide cathode P2–Na0.66Li0.18Fe0.12Mn0.7O2,
which demonstrated a high capacity of 190 mAh g–1 and a remarkably high capacity retention of ∼87% after 80
cycles within a wide voltage range of 1.5–4.5 V. The outstanding
stability is attributed to the reversible migration of lithium during
cycling and the elimination of the detrimental P2–O2 phase transition,
revealed by ex situ and in situ X-ray diffraction and solid-state
nuclear magnetic resonance spectroscopy.
We prepare group VI transitional metal dichalcogenides (TMDs, or MX) from the 1T phase with quantum-sized and monolayer features via a quasi-full electrochemical process. The resulting two-dimensional (2D) MX (M = W, Mo; X = S, Se) quantum dots (QDs) are ca. 3.0-5.4 nm in size with a high 1T phase fraction of ca. 92%-97%. We attribute this to the high Li content intercalated in the 1T-MX lattice (mole ratio of Li:M is over 2:1), which is achieved by an increased lithiation driving force and a reduced electrochemical lithiation rate (0.001 A/g). The high Li content not only promotes the 2H → 1T phase transition but also generates significant inner stress that facilitates lattice breaking for MX crystals. Because of their high proportion of metallic 1T phase and sufficient active sites induced by the small lateral size, the 2D 1T-MoS QDs show excellent hydrogen evolution reactivity (with a typical η of 92 mV, Tafel slope of 44 mV/dec, and J of 4.16 × 10 A/cm). This electrochemical route toward 2D QDs might help boost the development of 2D materials in energy-related areas.
Direct formic acid fuel cells (DFAFCs) allow highly efficient low temperature conversion of chemical energy into electricity and are expected to play a vital role in our future sustainable society. However, the massive precious metal usage in current membrane electrode assembly (MEA) technology greatly inhibits their actual applications. Here we demonstrate a new type of anode constructed by confining highly active nanoengineered catalysts into an ultra-thin catalyst layer with thickness around 100 nm. Specifically, an atomic layer of platinum is first deposited onto nanoporous gold (NPG) leaf to achieve high utilization of Pt and easy accessibility of both reactants and electrons to active sites. These NPG-Pt core/shell nanostructures are further decorated by a sub-monolayer of Bi to create highly active reaction sites for formic acid electro-oxidation. Thus obtained layer-structured NPG-Pt-Bi thin films allow a dramatic decrease in Pt usage down to 3 μg·cm -2 , while maintaining very high electrode activity and power performance at sufficiently low overall precious metal loading. Moreover, these electrode materials show superior durability during half-year test in actual DFAFCs, with remarkable resistance to common impurities in formic acid, which together imply their great potential in applications in actual devices.
Developing
highly efficient non-precious-metal catalysts for electrochemical
reduction reaction is vital for artificial nitrogen fixation under
ambient conditions. Herein, we report a bioinspired Fe3C@C composite as an efficient electrocatalyst for nitrogen reduction.
The composite based on a leaf skeleton successfully replicates the
natural vein structure with multichannels. The Fe3C@C core–shell
structure as the real active center contributes to selective electrocatalytic
synthesis of ammonia from nitrogen with Faraday efficiency of 9.15%
and production rate of 8.53 μg/(h mgcat) or 12.80
μg/(h cm2) at a low potential of −0.2 V versus
reversible hydrogen electrode (vs RHE), which is better than that
of recently reported carbon- and iron-based materials, even comparable
with that of noble-metal-based catalyst. Experiments with density
functional theory calculations reveal that graphene-encapsulated Fe3C nanoparticles can improve charge transfer due to core-shell
interaction, beneficial for inducing active sites for N2 adsorption and activation and thereby facilitate ammonia synthesis.
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