Kjeldgaard Robles (woollip05)

Photocatalytic CO2 conversion into reproducible chemical fuels (e.g., CO, CH3OH, or CH4) provides a promising scheme to solve the increasing environmental problems and energy demands simultaneously. click here However, the efficiency is severely restricted by the high overpotential of the CO2 reduction reaction (CO2RR) and rapid recombination of photoexcited carriers. Here, we propose that a novel type-II photocatalytic mechanism based on two-dimensional (2D) ferroelectric multilayers would be ideal for addressing these issues. Using density-functional theory and nonadiabatic molecular dynamics calculations, we find that the ferroelectric CuInP2S6 bilayers exhibit a staggered band structure induced by the vertical intrinsic electric fields. Different from the traditional type-II band alignment, the unique structure of the CuInP2S6 bilayer not only effectively suppresses the recombination of photogenerated electron-hole (e-h) pairs but also produces a sufficient photovoltage to drive the CO2RR. The predicted recombination time of photogenerated e-h pairs, 1.03 ns, is much longer than the transferring times of photoinduced electrons and holes, 5.45 and 0.27 ps, respectively. Moreover, the overpotential of the CO2RR will decrease by substituting an S atom with a Cu atom, making the redox reaction proceed spontaneously under solar radiation. The solar-to-fuel efficiency with an upper limit of 8.40% is achieved in the CuInP2S6 bilayer and can be further improved to 32.57% for the CuInP2S6 five-layer. Our results indicate that this novel type-II photocatalytic mechanism would be a promising way to achieve highly efficient photocatalytic CO2 conversion based on the 2D ferroelectric multilayers.Solid-state lithium batteries (SSLBs) based on garnet-type solid-state electrolytes (SSEs) have attracted much attention due to their high energy density and chemical stability. However, poor room-temperature ionic conductivity and low density of SSEs induced by conventional preparation routes limit their potential future applications. In this work, an oriented attachment strategy is employed to enhance the Li-ion conductivity and density of garnet-type SSE Li6.5La3Zr1.5Ta0.5O12 by introducing La2O3 nanoparticles. The oriented attachment of the ZrO2(Ta2O5) matrix mediates the epitaxial growth of the La-Zr(Ta)-O intermediate phase due to the addition of La2O3 nanoparticles. Continuous Li-ion transport pathways along grain boundaries are produced by the combination of residual La2O3 and gas Li2O. A densification interface is obtained when 10 wt % La2O3 is doped. The maximum value of Li-ion conductivity reaches 8.20 × 10-4 S·cm-1, with a relative density of 97.3%. SSLBs with a LiFePO4 cathode showing a stable cycling performance with a discharge capacity of 123.1 mA·h·g-1 and a Coulombic efficiency of 99.2% after 300 cycles (0.5C) at room temperature. This work is comparable to the state-of-the-art methodology, which provides a feasible approach to creating SSEs with high performances for SSLBs.Reversible solid oxide cells (RSOCs) present a conceivable potential for addressing energy storage and conversion issues through realizing efficient cycles between fuels and electricity based on the reversible operation of the fuel cell (FC) mode and electrolysis cell (EC) mode. Reliable electrode materials with high electrochemical catalytic activity and sufficient durability are imperatively desired to stretch the talents of RSOCs. Herein, oxygen vacancy engineering is successfully implemented on the Fe-based layered perovskite by introducing Zr4+, which is demonstrated to greatly improve the pristine intrinsic performance, and a novel efficient and durable oxygen electrode material is synthesized. The substitution of Zr at the Fe site of PrBaFe2O5+δ (PBF) enables enlarging the lattice free volume and generating more oxygen vacancies. Simultaneously, the target material delivers more rapid oxygen surface exchange coefficients and bulk diffusion coeffi