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Bimetallic nanoparticles often show properties superior to their single-component counterparts. However, the large parameter space, including size, structure, composition, and spatial arrangement, impedes the discovery of the best nanoparticles for a given application. High-throughput methods that can control the composition and spatial arrangement of the nanoparticles are desirable for accelerated materials discovery. Herein, we report a methodology for synthesizing bimetallic alloy nanoparticle arrays with precise control over their composition and spatial arrangement. A dual-channel nanopipet is used, and nanofluidic control in the nanopipet further enables precise tuning of the electrodeposition rate of each element, which determines the final composition of the nanoparticle. The composition control is validated by finite element simulation as well as electrochemical and elemental analyses. The scope of the particles demonstrated includes Cu–Ag, Cu–Pt, Au–Pt, Cu–Pb, and Co–Ni. We further demonstrate surface patterning using Cu–Ag alloys with precise control of the location and composition of each pixel. Additionally, combining the nanoparticle alloy synthesis method with scanning electrochemical cell microscopy (SECCM) allows for fast screening of electrocatalysts. The method is generally applicable for synthesizing metal nanoparticles that can be electrodeposited, which is important toward developing automated synthesis and screening systems for accelerated material discovery in electrocatalysis. 

Reclamation of coal fly ash, a legacy waste material, provides an alternative pathway for the recovery of rare earth elements (REEs) while reducing the environmental stresses that stem from traditional mining. The reactive transport processes underlying the recovery of REEs from ash wastes, however, are yet to be fully elucidated owing to the physicochemical complexity of the micro/nanoscale fly ash particles, including the crystallinity of the particulate matrix. In this work, we use transmission electron microscopy to characterize the material properties of ash particles and reveal the impact of crystallinity on the reactive transport processes governing access to and recovery of the encapsulated REEs. Our results show, for the first time, two distinct crystalline structures of REE-bearing aluminosilicate particles: dense amorphous matrices that facilitate the exchange of chemical species through their lattice interstices and porous polycrystalline matrices characterized by connected intraparticle pores and chemical inertness to leaching solutions. Notably, the presence of matrix crystallinity, or the lack thereof, governs the extent of reagents consumed parasitically by secondary reactions with the aluminosilicate matrix. Our work reveals how the variability of crystalline structures of the ash matrices hosting REEs defines the pathways for the recovery of REEs, providing key insights required for the development of targeted recovery processes. 

The ability to scale two-dimensional (2D) material thickness down to a single monolayer presents a promising opportunity to realize high-speed energy-efficient memristors. Here, we report an ultra-fast memristor fabricated using atomically thin sheets of 2D hexagonal Boron Nitride, exhibiting the shortest observed switching speed (120 ps) among 2D memristors and low switching energy (2pJ). Furthermore, we study the switching dynamics of these memristors using ultra-short (120ps-3ns) voltage pulses, a frequency range that is highly relevant in the context of modern complementary metal oxide semiconductor (CMOS) circuits. We employ statistical analysis of transient characteristics to gain insights into the memristor switching mechanism. Cycling endurance data confirms the ultra-fast switching capability of these memristors, making them attractive for next generation computing, storage, and Radio-Frequency (RF) circuit applications.

 

Monolayer materials can be vertically stacked into artificial solids, known as the van der Waals heterostructures (vd-WHs) [1], to realize a new class of ultrathin optoelectronic, electronic, and quantum devices, which have significant potential to revolutionize the field of nanoelectronics and impact a wide range of application areas including transparent displays, sensor arrays, and logic and memory circuits. However, today’s assembly of vdWH devices is still primarily through manual manipulation, which lacks the precision and repeatability needed for the scalable manufacturing of wafer-scale vdWH device arrays outside a research setting. Aiming to enable the automated, scalable, and repeatable manufacturing of vdWH device arrays, this paper presents the design, prototyping, and preliminary tests of a novel semi-automated soft-robotic stamp transfer system for thin-film materials. The system uses a dry elastomer stamp with its adhesion controlled by temperature and peeling speed for material transfer. A combination of electromagnetic and pneumatic actuation is used for the soft-robotic stamp to realize a gentle and uniform pressing of the stamp over the material. An optical microscope, force sensors, and temperature sensors are integrated to enable instrumentation of the transfer process. Preliminary experiments were conducted using our system to conduct for exfoliated graphite transfer. Test results demonstrate the reliable and repeatable transfer of 2D crystal flakes, which show promise to enable the deterministic and scalable assembly of vdWH-based device arrays at wafer scale. 

2D memristors have demonstrated attractive resistive switching characteristics recently but also suffer from the reliability issue, which limits practical applications. Previous efforts on 2D memristors have primarily focused on exploring new material systems, while damage from the metallization step remains a practical concern for the reliability of 2D memristors. Here, the impact of metallization conditions and the thickness of MoS₂films on the reliability and other device metrics of MoS₂‐based memristors is carefully studied. The statistical electrical measurements show that the reliability can be improved to 92% for yield and improved by ≈16× for average DC cycling endurance in the devices by reducing the top electrode (TE) deposition rate and increasing the thickness of MoS₂films. Intriguing convergence of switching voltages and resistance ratio is revealed by the statistical analysis of experimental switching cycles. An “effective switching layer” model compatible with both monolayer and few‐layer MoS₂, is proposed to understand the reliability improvement related to the optimization of fabrication configuration and the convergence of switching metrics. The Monte Carlo simulations help illustrate the underlying physics of endurance failure associated with cluster formation and provide additional insight into endurance improvement with device fabrication optimization.

 

The nature of the atomic configuration and the bonding within epitaxial Pt‐graphene films is investigated. Graphene‐templated monolayer/few‐multilayers of Pt, synthesized as contiguous 2D films by room temperature electrochemical methods, is shown to exhibit a stable {100} structure in the 1–2 layer range. The fundamental question being investigated is whether surface Pt atoms rendered in these 2D architectures are as stable as those of their bulk Pt counterparts. Unsurprisingly, a single layer Pt on the graphene (Pt_1ML/GR) shows much larger Pt dissociation energy (−7.51 eV) than does an isolated Pt atom on graphene. However, the dissociation energy from Pt_1ML/GR is similar to that of bulk Pt(100), −7.77 eV, while in bi‐layer Pt on the graphene (Pt_2ML/GR), this energy changes to −8.63 eV, surpassing its bulk counterpart. At Pt_2ML/GR, the dissociation energy also slightly surpasses that of bulk Pt(111). Bulk‐like stability of atomically thin Pt–graphene results from a combination of interplanar PtC covalent bonding and inter/intraplanar metallic bonding. This unprecedented stability is also accompanied by a metal‐like presence of electronic states at the Fermi level. Such atomically thin metal‐graphene architectures can be a new stable platform for synthesizing 2D metallic films with various applications in catalysis, sensing, and electronics.

 

Direct synthesis of graphene with well‐defined nanoscale pores over large areas can transform the fabrication of nanoporous atomically thin membranes (NATMs) and greatly enhance their potential for practical applications. However, scalable bottom‐up synthesis of continuous sheets of nanoporous graphene that maintain integrity over large areas has not been demonstrated. Here, it is shown that a simple reduction in temperature during chemical vapor deposition (CVD) on Cu induces in‐situ formation of nanoscale defects (≤2–3 nm) in the graphene lattice, enabling direct and scalable synthesis of nanoporous monolayer graphene. By solution‐casting of hierarchically porous polyether sulfone supports on the as‐grown nanoporous CVD graphene, large‐area (>5 cm²) NATMs for dialysis applications are demonstrated. The synthesized NATMs show size‐selective diffusive transport and effective separation of small molecules and salts from a model protein, with ≈2–100× increase in permeance along with selectivity better than or comparable to state‐of‐the‐art commercially available polymeric dialysis membranes. The membranes constitute the largest fully functional NATMs fabricated via bottom‐up nanopore formation, and can be easily scaled up to larger sizes permitted by CVD synthesis. The results highlight synergistic benefits in blending traditional membrane casting with bottom‐up pore creation during graphene CVD for advancing NATMs toward practical applications.