Formic acid (or formate) is suggested to be one of the most economically viable products from electrochemical carbon dioxide reduction. However, its commercial viability hinges on the development of highly active and selective electrocatalysts. Here we report that structural defects have a profound positive impact on the electrocatalytic performance of bismuth. Bismuth oxide double-walled nanotubes with fragmented surface are prepared as a template, and are cathodically converted to defective bismuth nanotubes. This converted electrocatalyst enables carbon dioxide reduction to formate with excellent activity, selectivity and stability. Most significantly, its current density reaches ~288 mA cm
−2
at −0.61 V versus reversible hydrogen electrode within a flow cell reactor under ambient conditions. Using density functional theory calculations, the excellent activity and selectivity are rationalized as the outcome of abundant defective bismuth sites that stabilize the *OCHO intermediate. Furthermore, this electrocatalyst is coupled with silicon photocathodes and achieves high-performance photoelectrochemical carbon dioxide reduction.
Atomically dispersed M-N-C (M refers to transition metals) materials represent the most promising catalyst alternatives to the precious metal Pt for the electrochemical reduction of oxygen (ORR), yet the genuine active sites in M-N-C remain elusive. Here, we develop a two-step approach to fabricate Cu-N-C single-atom catalysts with a uniform and well-defined Cu 2+ -N 4 structure that exhibits comparable activity and superior durability in comparison to Pt/C. By combining operando X-ray absorption spectroscopy with theoretical calculations, we unambiguously identify the dynamic evolution of Cu-N 4 to Cu-N 3 and further to HO-Cu-N 2 under ORR working conditions, which concurrently occurs with reduction of Cu 2+ to Cu + and is driven by the applied potential. The increase in the Cu + /Cu 2+ ratio with the reduced potential indicates that the low-coordinated Cu + -N 3 is the real active site, which is further supported by DFT calculations showing the lower free energy in each elemental step of the ORR on Cu + -N 3 than on Cu 2+ -N 4 . These findings provide a new understanding of the dynamic electrochemistry on M-N-C catalysts and may guide the design of more efficient low-cost catalysts.
The discovery of ferromagnetic two-dimensional van der Waals materials has opened up opportunities to explore intriguing physics and to develop innovative spintronic devices. However, controllable synthesis of these 2D ferromagnets and enhancing their stability under ambient conditions remain challenging. Here, we report chemical vapor deposition growth of air-stable 2D metallic 1T-CrTe2 ultrathin crystals with controlled thickness. Their long-range ferromagnetic ordering is confirmed by a robust anomalous Hall effect, which has seldom been observed in other layered 2D materials grown by chemical vapor deposition. With reducing the thickness of 1T-CrTe2 from tens of nanometers to several nanometers, the easy axis changes from in-plane to out-of-plane. Monotonic increase of Curie temperature with the thickness decreasing from ~130.0 to ~7.6 nm is observed. Theoretical calculations indicate that the weakening of the Coulomb screening in the two-dimensional limit plays a crucial role in the change of magnetic properties.
Electrocatalytic CO 2 reduction (CO 2 RR) to valuable fuels is a promising approach to mitigate energy and environmental problems, but controlling the reaction pathways and products remains challenging. Here a novel Cu 2 O nanoparticle film was synthesized by square-wave (SW) electrochemical redox cycling of high-purity Cu foils. The cathode afforded up to 98% Faradaic efficiency for electroreduction of CO 2 to nearly pure formate under ≥45 atm CO 2 in bicarbonate catholytes. When this cathode was paired with a newly developed NiFe hydroxide carbonate anode in KOH/borate anolyte, the resulting two-electrode high-pressure electrolysis cell achieved high energy conversion efficiencies of up to 55.8% stably for long-term formate production. While the high-pressure conditions drastically increased the solubility of CO 2 to enhance CO 2 reduction and suppress hydrogen evolution, the (111)-oriented Cu 2 O film was found to be important to afford nearly 100% CO 2 reduction to formate. The results have implications for CO 2 reduction to a single liquid product with high energy conversion efficiency.
We
report the syntheses of highly dispersed CoNi bimetallic catalysts
on the surface of α-MoC based on the strong metal support interaction
(SMSI) effect. The interaction between the nearly atomically dispersed
Co and Ni atoms was observed for the first time by the real-space
chemical mapping at the atomic level. Combined with the ability of
α-MoC to split water at low temperatures, the as-synthesized
CoNi/α-MoC catalysts exhibited robust and synergistic performance
for the hydrogen production from hydrolysis of ammonia borane. The
metal-normalized activity of the bimetallic 1.5Co1.5Ni/α-MoC
catalyst reached 321.1 molH2·mol–1
CoNi·min–1 at 298 K, which surpasses
all the noble metal-free catalysts ever reported and is four times
higher than that of the commercial Pt/C catalyst.
A Li-rich Layered@Spinel@Carbon heterostructured cathode material for LIBs, which comprises Li-rich layered core, a spinel interlayer and a carbon nano-coating.
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