Copper (Cu) is a catalyst broadly used in industry for hydrogenation of carbon dioxide, which has broad implications for environmental sustainability. An accurate understanding of the degeneration behavior of Cu catalysts under operando conditions is critical for uncovering the failure mechanism of catalysts and designing novel ones with optimized performance. Despite the widespread use of these materials, their failure mechanisms are not well understood because conventional characterization techniques lack the necessary time and spatial resolution to capture these complex behaviors. In order to overcome these challenges, we carried out transmission electron microscopy (TEM) with a specialized in situ gas environmental holder, which allows us to unravel the dynamic behavior of the Cu nanowires (NWs) in operando. The failure process of these nanoscale Cu catalysts under CO2 atmosphere were tracked and further rationalized based on our numerical modeling using phase-field methods.
Entropy-engineered materials are garnering considerable attention owing to their excellent mechanical and transport properties, such as their high thermoelectric performance. However, understanding the effect of entropy on thermoelectrics remains a challenge. In this study, we used the PbGeSnCd x Te3+x family as a model system to systematically investigate the impact of entropy engineering on its crystal structure, microstructure evolution, and transport behavior. We observed that PbGeSnTe3 crystallizes in a rhombohedral structure at room temperature with complex domain structures and transforms into a high-temperature cubic structure at ∼373 K. By alloying CdTe with PbGeSnTe3, the increased configurational entropy lowers the phase-transition temperature and stabilizes PbGeSnCd x Te3+x in the cubic structure at room temperature, and the domain structures vanish accordingly. The high-entropy effect results in increased atomic disorder and consequently a low lattice thermal conductivity of 0.76 W m–1 K–1 in the material owing to enhanced phonon scattering. Notably, the increased crystal symmetry is conducive to band convergence, which results in a high-power factor of 22.4 μW cm–1 K–1. As a collective consequence of these factors, a maximum ZT of 1.63 at 875 K and an average ZT of 1.02 in the temperature range of 300–875 K were obtained for PbGeSnCd0.08Te3.08. This study highlights that the high-entropy effect can induce a complex microstructure and band structure evolution in materials, which offers a new route for the search for high-performance thermoelectrics in entropy-engineered materials.
Nanoscale tailoring of catalytic materials and Libattery alternatives has elevated the importance of in situ gas-phase electron microscopy. Such advanced techniques are often performed using an environmental cell inserted into a conventional S/TEM setup, as this method facilitates concurrent electrochemical and temperature stimulations in a convenient and costeffective manner. However, these cells are made by encapsulating gas between two insulating membranes, which introduces additional electron scattering. We have evaluated strengths and limitations of the gas-phase E-cell S/TEM technique, both experimentally and through simulations, across a variety of practical parameters. We reveal the degradation of image quality in an E-cell setup from various components and explore opportunities to improve imaging quality through intelligent choice of experimental parameters. Our results underscore the benefits of using an E-cell STEM technique, due to its versatility and excellent ability to suppress the exotic contributions from the membrane device.
Oil spills have huge and immediate economically, socially, and environmentally adverse impacts. Current methods to remediate oil spills do not provide a sustainable solution, in terms of cost, ease of deployment, and further impact on the environment. Here we report an oil spill remediation solution in form of an oleophilic, hydrophobic, and magnetic (OHM) sponge that is economical, efficient, and ecofriendly; thereby promising a potentially industry-adaptable approach. The OHM sponge can not only selectively remove the oil from oil/water interface but also recover the oil by a simple squeezing process. Furthermore, the OHM sponge can be reused for many cycles. The OHM sponge works effectively in diverse and extreme aquatic conditions (pH, salinity) and can absorb a variety of oils and oil-based compounds. The selective absorption/desorption, recovery, high absorption capacity, and reusability under one platform open new prospects for potentially sustainable water and environmental remediation applications.
Superconducting thin films of niobium have been extensively employed in transmon qubit architectures. Although these architectures have demonstrated improvements in recent years, further improvements in performance through materials engineering will aid in large-scale deployment. Here, we use information retrieved from secondary ion mass spectrometry and electron microscopy to conduct a detailed assessment of the surface oxide that forms in ambient conditions for transmon test qubit devices patterned from a niobium film. We observe that this oxide exhibits a varying stoichiometry with NbO and NbO2 found closer to the niobium film/oxide interface and Nb2O5 found closer to the surface. In terms of structural analysis, we find that the Nb2O5 region is semicrystalline in nature and exhibits randomly oriented grains on the order of 1–3 nm corresponding to monoclinic N–Nb2O5 that are dispersed throughout an amorphous matrix. Using fluctuation electron microscopy, we are able to map the relative crystallinity in the Nb2O5 region with nanometer spatial resolution. Through this correlative method, we observe that the highly disordered regions are more likely to contain oxygen vacancies and exhibit weaker bonds between the niobium and oxygen atoms. Based on these findings, we expect that oxygen vacancies likely serve as a decoherence mechanism in quantum systems.
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