Engineering topics
Li, Peng
Publications and source records attributed to Li, Peng.
General synthesis of single-atom catalysts with high metal loading using graphene quantum dots
Transition-metal single-atom catalysts present extraordinary activity per metal atomic site, but suffer from low metal-atom densities (typically less than 5 wt% or 1 at.%), which limits their overall catalytic performance. Here we report a general method for the synthesis of single-atom catalysts with high transition-metal-atom loadings of up to 40 wt% or 3.8 at.%, representing several-fold improvements compared to benchmarks in the literature. Graphene quantum dots, later interweaved into a carbon matrix, were used as a support, providing numerous anchoring sites and thus facilitating the generation of high densities of transition-metal atoms with sufficient spacing between the metal atoms to avoid aggregation. A significant increase in activity in electrochemical CO 2 reduction (used as a representative reaction) was demonstrated on a Ni single-atom catalyst with increased Ni loading.
Skip-Connected Self-Recurrent Spiking Neural Networks with Joint Intrinsic Parameter and Synaptic Weight Training
As an important class of spiking neural networks (SNNs), recurrent spiking neural networks (RSNNs) possess great computational power and have been widely used for processing sequential data like audio and text. However, most RSNNs suffer from two problems. 1. Due to the lack of architectural guidance, random recurrent connectivity is often adopted, which does not guarantee good performance. 2. Training of RSNNs is in general challenging, bottlenecking achievable model accuracy. To address these problems, we propose a new type of RSNNs called Skip-Connected Self-Recurrent SNNs (ScSr-SNNs). Recurrence in ScSr-SNNs is introduced in a stereotyped manner by adding self-recurrent connections to spiking neurons. The SNNs with self-recurrent connections can realize recurrent behaviors similar to those of more complex RSNNs while the error gradients can be more straightforwardly calculated due to the mostly feedforward nature of the network. The network dynamics is enriched by skip connections between nonadjacent layers. Moreover, we propose a new backpropagation (BP) method called backpropagated intrinsic plasticity (BIP) to further boost the performance of ScSr-SNNs by training intrinsic model parameters. Unlike standard intrinsic plasticity rules that adjust the neuron's intrinsic parameters according to neuronal activity, the proposed BIP method optimizes intrinsic parameters based on the backpropagated error gradient of a well-defined global loss function in addition to synaptic weight training. Here, based on challenging speech, neuromorphic speech, and neuromorphic image datasets, the proposed ScSr-SNNs can boost performance by up to 2.85% compared with other types of RSNNs trained by state-of-the-art BP methods.
Charge-spin interconversion in epitaxial Pt probed by spin-orbit torques in a magnetic insulator
We measure spin-orbit torques (SOTs) in a model system of all-epitaxial ferrite/Pt bilayers to gain insights into charge-spin interconversion in Pt. With negligible electronic conduction in the insulating ferrite, the crystalline Pt film acts as the sole source of charge-to-spin conversion. A small fieldlike SOT independent of Pt thickness suggests a weak Rashba-Edelstein effect at the ferrite/Pt interface. By contrast, we observe a sizable dampinglike SOT that depends on the Pt thickness, from which we deduce the dominance of an extrinsic spin-Hall effect (skew scattering) and Dyakonov-Perel spin relaxation in the crystalline Pt film. Furthermore, our results point to a large internal spin-Hall ratio of ≈ 0.8 in epitaxial Pt. Furthermore, our experimental work takes an essential step towards understanding the mechanisms of charge-spin interconversion and SOTs in Pt-based heterostructures, which are crucial for power-efficient spintronic devices.
Azatricyclic Inverse Agonists of ROR[gamma]t That Demonstrate Efficacy in Models of Rheumatoid Arthr
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Ultra-high-voltage Ni-rich layered cathodes in practical Li metal batteries enabled by a sulfonamide-based electrolyte
By increasing the charging voltage, a cell specific energy of >400 Wh kg-1 is in principle achievable with LiNi0.8Mn0.1Co0.1O2 in lithium-metal batteries (LMBs). However, stable cycling of high-nickel cathodes at ultra-high voltages is extremely challenging. Here we report that a rationally designed sulfonamide-based electrolyte enables stable cycling of commercial LiNi0.8Co0.1Mn0.1O2 with a cut-off voltage up to 4.7 V in LMBs. In contrast to commercial carbonate electrolytes, the electrolyte not only suppresses side reactions, intergranular cracking, transition-metal dissolution, and impedance growth on the cathode side, but also enables highly reversible Li metal stripping and plating leading to compact morphology and low pulverization. Our LMB delivers a specific capacity >230 mAh g-1 and an average Coulombic efficiency >99.65% over 100 cycles. Even under harsh testing conditions, the 4.7 V LMB can retain >88% capacity for 90 cycles, demonstrating significant advances in practical LMBs.
Topological Hall Effect in a Topological Insulator Interfaced with a Magnetic Insulator
A topological insulator (TI) interfaced with a magnetic insulator (MI) may host an anomalous Hall effect (AHE), a quantum AHE, and a topological Hall effect (THE). Recent studies, however, suggest that coexisting magnetic phases in TI/MI heterostructures may result in an AHE-associated response that resembles a THE but in fact is not. Here, we report a genuine THE in a TI/MI structure that has only one magnetic phase. The structure shows a THE in the temperature range of T = 2–3 K and an AHE at T = 80–300 K. Over T = 3–80 K, the two effects coexist but show opposite temperature dependencies. Control measurements, calculations, and simulations together suggest that the observed THE originates from skyrmions, rather than the coexistence of two AHE responses. The skyrmions are formed due to a Dzyaloshinskii–Moriya interaction (DMI) at the interface; the DMI strength estimated is substantially higher than that in heavy metal-based systems.
Detector Tilt Considerations in Bragg Coherent Diffraction Imaging: A Simulation Study
This paper addresses the three-dimensional signal distortion and image reconstruction issues in X-ray Bragg coherent diffraction imaging (BCDI) in the event of a general non-orthogonal orientation of the area detector with respect to the diffracted beam. Growing interest in novel BCDI adaptations at fourth-generation synchrotron light sources has necessitated improvisations in the experimental configuration and the subsequent data analysis. One such possibly unavoidable improvisation that is envisioned in this paper is a photon-counting area detector whose face is tilted away from the perpendicular to the Bragg-diffracted beam during the acquisition of the coherent diffraction signal. We describe a likely circumstance in which one would require such a detector configuration, along with the experimental precedent at third-generation synchrotrons. Using physically accurate diffraction simulations from synthetic scatterers in the presence of such tilted detectors, we analyze the general nature of the observed signal distortion qualitatively and quantitatively and provide a prescription to correct for it during image reconstruction. Our simulations and reconstructions are based on an adaptation of the known theory of BCDI sampling geometry, as well as the recently developed projection-based methods of wavefield propagation. Such configurational modifications and their numerical remedies are potentially valuable in realizing unconventional coherent diffraction measurement geometries, eventually paving the way for the integration of BCDI into new material characterization experiments at next-generation light sources.
Experimental parameters, combined dynamics, and nonlinearity of a magnonic-opto-electronic oscillator (MOEO)
We report the construction and characterization of a comprehensive magnonic-opto-electronic oscillator (MOEO) system based on 1550-nm photonics and yttrium iron garnet (YIG) magnonics. The system exhibits a rich and synergistic parameter space because of the ability to control individual photonic, electronic, and magnonic components. Taking advantage of the spin wave dispersion of YIG, the frequency self-generation as well as the related nonlinear processes becomes sensitive to the external magnetic field. Besides being known as a band-pass filter and a delay element, the YIG delay line possesses spin wave modes that can be controlled to mix with the optoelectronic modes to generate higher-order harmonic beating modes. With the high sensitivity and external tunability, the MOEO system may find usefulness in sensing applications in magnetism and spintronics beyond optoelectronics and photonics.
A historical overview of the activation and porosity of metal–organic frameworks
Since the first reports of metal–organic frameworks (MOFs), this unique class of crystalline, porous materials has garnered increasing attention in a wide variety of applications such as gas storage and separation, catalysis, enzyme immobilization, drug delivery, water capture, and sensing. A fundamental feature of MOFs is their porosity which provides space on the micro- and meso-scale for confining and exposing their functionalities. Therefore, designing MOFs with high porosity and developing suitable activation methods for preserving and accessing their pore space have been a common theme in MOF research. Reticular chemistry allows for the facile design of MOFs from highly tunable metal nodes and organic linkers in order to realize different pore structures, topologies, and functionalities. With the hope of shedding light on future research endeavors in MOF porosity, it is worthwhile to examine the development of MOFs, with an emphasis on their porosity and how to properly access their pore space. In this review, we will provide an overview of the historic evolution of porosity and activation of MOFs, followed by a synopsis of the strategies to design and preserve permanent porosity in MOFs.
Detecting Phase-Resolved Magnetization Dynamics by Magneto-Optic Effects at 1550 nm Wavelength
We demonstrate the detection of phase-resolved magnetization dynamics with combinatorial magneto-optic Kerr and Faraday effects. The method uses a continuous-wave laser that is amplitude-modulated at the spin dynamic frequencies, and thus allows for coherent tracking of the spin dynamics, akin a “lock-in” type measurement. In particular, our method, using a single 1550-nmwavelength, probes simultaneously the ferromagnetic resonance of Y 3 Fe 5 O 12 (YIG) and Permalloy (Py = Ni 80 Fe 20 ) in a YIG-Pyhetero structure. The fiber-based magneto-optic components also have the advantage of being made into a compact, tabletop or even portable system with yet robust measurement performances. We believe that our method will be found useful in studying hybrid quantum magnonic systems and/or investigating phase-resolved spin dynamics in nanomagnet structures involving both ferromagnetic insulators and metals.
Stabilization of Photocatalytically Active Uranyl Species in a Uranyl–Organic Framework for Heterogeneous Alkane Fluorination Driven by Visible Light
When photoactivated, the uranyl ion is a robust oxidant capable of abstracting hydrogen atoms from nonactivated C–H bonds. Yet, the highly reactive singly reduced [U V O 2 ] + intermediate is unstable with respect to disproportionation to the uranyl dication and insoluble tetravalent uranium phases, which limits the usage of uranyl ions as robust photocatalysts. Herein, we demonstrate that photoactivated uranyl ions can be stabilized by immobilizing and separating them spatially in a uranyl–organic framework heterogeneous catalyst, NU-1301. The visible-light-photoactivated uranyl ions in NU-1301 demonstrated longer-lived U(V) and radicals than those in homogeneous counterparts, as evidenced by X-ray photoelectron spectroscopy and time-dependent electron paramagnetic resonance, leading to higher turnovers and enhanced stability for the fluorination of nonactivated alkanes.
Coordination Chemistry in the Structural and Functional Exploration of Actinide-Based Metal-Organic Frameworks
The coordination chemistry between inorganic and organic species can be optimally exemplified by metal–organic frameworks (MOFs), whose structures and functionalities can be rationally designed from these highly tunable building blocks. The high porosity, stability, and versatile functionalities of MOFs have attracted wide-spread attention from energy-related research and pollution remediation to biomedical applications. A unique and underexplored subset of these materials are MOFs based on actinide nodes; these MOFs have distinguished themselves as a unique platform for investigating the versatile oxidation states, reactivity, and coordination chemistry of actinides. Herein, we will focus on the rational design and synthesis of actinide-based MOFs under the general guidelines of coordination chemistry for their structural and functional explorations. The dimensionality, topology, and structures of actinide-based MOFs can be controlled by selecting pre-designed building blocks of actinide-based nodes and organic linkers with certain desired coordination geometries and functionalities. Furthermore, these unique actinide-based MOFs have shown promise for applications in nuclear waste mitigation, pollution control, and catalysis.
The role of iron in magnetic damping of Mg(Al,Fe) 2 O 4 spinel ferrite thin films
© 2020 Author(s). We have investigated magnesium aluminum ferrite thin films with a range of iron concentrations and identified the optimal iron content to obtain high crystalline quality thin films with the low magnetic damping required for spin current-based applications. Epitaxial MgAl 2-x FexO4 films with 0.8 < x < 2.0 were grown by pulsed laser deposition on single crystal MgAl2O4 substrates and were characterized structurally and magnetically. We find that the x = 1.5 composition minimizes the room-temperature magnetic damping with a typical Gilbert damping parameter of α eff = 1.8 × 10-3. This minimized damping is governed by a competition between the more robust magnetic ordering with increased iron content, x, and the more defective structure due to larger film-substrate lattice mismatch with increased iron content. The temperature-dependent magnetization curves indicate that Tc is suppressed below room temperature for iron content x ≤ 1.2 and eventually suppressed entirely for x = 0.8. X-ray magnetic circular dichroism results indicate that for all x the magnetic moment is dominated by Fe 3 + cations distributed in a 60:40 ratio on the octahedral and tetrahedral sites, with minimal contribution from Fe 2 + cations. Films with x = 1.4-1.6 exhibit very strong ferromagnetic resonance and low Gilbert damping with α eff = (1.8-6) × 10-3, making them ideal candidates for microwave and spintronic applications.