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            Abstract An ultra-thin overcoating of zirconium oxide (ZrO2) film on CuO-ZnO-Al2O3(CZA) catalysts by atomic layer deposition (ALD) was proved to enhance the catalytic performance of CZA/HZSM-5 (H form of Zeolite Socony Mobil-5) bifunctional catalysts for hydrogenation of CO2to dimethyl ether (DME). Under optimal reaction conditions (i.e. 240 °C and 2.8 MPa), the yield of product DME increased from 17.22% for the bare CZA/HZSM-5 catalysts, to 18.40% for the CZA catalyst after 5 cycles of ZrO2ALD with HZSM-5 catalyst. All the catalysts modified by ZrO2ALD displayed significantly improved catalytic stability of hydrogenation of CO2to DME reaction, compared to that of CZA/HZSM-5 bifunctional catalysts. The loss of DME yield in 100 h of reaction was greatly mitigated from 6.20% (loss of absolute value) to 3.01% for the CZA catalyst with 20 cycles of ZrO2ALD overcoating. Characterizations including hydrogen temperature programmed reduction, x-ray powder diffraction, and x-ray photoelectron spectroscopy revealed that there was strong interaction between Cu active centers and ZrO2.more » « less
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            Abstract Interphase layers that form at contact points between the solid electrolyte (SE) and cathode active material in solid‐state lithium‐ion batteries (SS‐LIBs) increase cell impedance, but the mechanisms for this interphase formation are poorly understood. Here, we demonstrate a simple workflow to study cathode–electrolyte interphase (CEI) formation using 4D‐scanning transmission electron microscopy (4D‐STEM) that does not require SS‐LIB assembly. We show benefits of MoCl5:EtOH as a chemical delithiating agent, and prepare chemically delithiated cathode LiNi0.6Co0.2Mn0.2O2(NMC) powder in contact with Li10GeP2S12(LGPS) SE powder as a SS‐LIB CEI surrogate. We map the composition and structure of the CEI layers using 4D‐STEM, energy dispersive X‐ray spectroscopy (EDS), and electron pair distribution function analysis (ePDF). EDS indicates O migration from NMC into LGPS. ePDF analysis indicates sulfate and phosphate formation localized on the surface of LGPS, as well as Li2O formation within the LGPS phase, and self‐decomposition of NMC. These results are consistent with an electrochemical self‐discharge mechanism for interphase formation arising from coupled redox reactions of sulfur oxidation in LGPS and transition metal reduction in NMC. This suggests that coatings which stop anion transport but allow Li+and e−transport may prevent interphase formation and reduce impedance in SS‐LIBs.more » « less
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            Abstract While the discovery of two-dimensional (2D) magnets opens the door for fundamental physics and next-generation spintronics, it is technically challenging to achieve the room-temperature ferromagnetic (FM) order in a way compatible with potential device applications. Here, we report the growth and properties of single- and few-layer CrTe 2 , a van der Waals (vdW) material, on bilayer graphene by molecular beam epitaxy (MBE). Intrinsic ferromagnetism with a Curie temperature ( T C ) up to 300 K, an atomic magnetic moment of ~0.21 $${\mu }_{{\rm{B}}}$$ μ B /Cr and perpendicular magnetic anisotropy (PMA) constant ( K u ) of 4.89 × 10 5 erg/cm 3 at room temperature in these few-monolayer films have been unambiguously evidenced by superconducting quantum interference device and X-ray magnetic circular dichroism. This intrinsic ferromagnetism has also been identified by the splitting of majority and minority band dispersions with ~0.2 eV at Г point using angle-resolved photoemission spectroscopy. The FM order is preserved with the film thickness down to a monolayer ( T C ~ 200 K), benefiting from the strong PMA and weak interlayer coupling. The successful MBE growth of 2D FM CrTe 2 films with room-temperature ferromagnetism opens a new avenue for developing large-scale 2D magnet-based spintronics devices.more » « less
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