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Ren, Yang

Publications and source records attributed to Ren, Yang.

At least 55 records · Page 3
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Direct Synthesis of Ammonia from Nitrate on Amorphous Graphene with Near 100% Efficiency

Abstract Ammonia is an indispensable commodity in the agricultural and pharmaceutical industries. Direct nitrate‐to‐ammonia electroreduction is a decentralized route yet challenged by competing side reactions. Most catalysts are metal‐based, and metal‐free catalysts with high nitrate‐to‐ammonia conversion activity are rarely reported. Herein, it is shown that amorphous graphene synthesized by laser induction and comprising strained and disordered pentagons, hexagons, and heptagons can electrocatalyze the eight‐electron reduction of NO 3 − to NH 3 with a Faradaic efficiency of ≈100% and an ammonia production rate of 2859 µg cm −2 h −1 at −0.93 V versus reversible hydrogen electrode. X‐ray pair‐distribution function analysis and electron microscopy reveal the unique molecular features of amorphous graphene that facilitate NO 3 − reduction. In situ Fourier transform infrared spectroscopy and theoretical calculations establish the critical role of these features in stabilizing the reaction intermediates via structural relaxation. The enhanced catalytic activity enables the implementation of flow electrolysis for the on‐demand synthesis and release of ammonia with >70% selectivity, resulting in significantly increased yields and survival rates when applied to plant cultivation. The results of this study show significant promise for remediating nitrate‐polluted water and completing the NO x cycle.

Huang, Libei↗
DOE OSTI2023

An anomalous structure disordering in Zr–Cu–Ag supercooled glass-forming liquids

An anomalous ordering-to-disordering transition in a Zr–Cu–Ag supercooled glass-forming liquid has been revealed by in situ high-energy x-ray diffraction. Upon heating, the supercooled liquid exhibits a structural crossover at T c = 716 K, evident by the change in statistical characteristics of the first sharp diffraction peak. When annealed in the vicinity of T c , the supercooled liquid first relaxes from its initial state to a denser and more ordered state. Subsequently, it becomes disordered at the medium-range scale with a slowing down of densification, as demonstrated by the broadening of the first sharp diffraction peak and a decrease in the peak intensities of the higher atomic shells in the reduced pair distribution function. Finally, a scenario for the evolution of less correlated locally favored clusters in the liquid–liquid phase transition is discussed.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Synthesis of Free-Standing Pd-Ni-P Metallic Glass Nanoparticles with Durable Medium-Range Ordered Structure for Enhanced Electrocatalytic Properties

Topologically disordered metallic glass nanoparticles (MGNPs) with highly active and tailorable surface chemistries have immense potential for functional uses. The synthesis of free-standing MGNPs is crucial and intensively pursued because their activity strongly depends on their exposed surfaces. Herein, a novel laser-evaporated inert-gas condensation method is designed and successfully developed for synthesizing free-standing MGNPs without substrates or capping agents, which is implemented via pulse laser-induced atomic vapor deposition under an inert helium atmosphere. In this way, the metallic atoms vaporized from the targets collide with helium atoms and then condense into short-range-order (SRO) clusters, which mutually assemble to form the MGNPs. Using this method, free-standing Pd 40 Ni 40 P 20 MGNPs with a spherical morphology are synthesized, which demonstrates satisfactory electrocatalytic activity and durability in oxygen reduction reactions. Moreover, local structure investigations using synchrotron pair distribution function techniques reveal the transformation of SRO cluster connection motifs of the MGNPs from face-sharing to edge-sharing modes during cyclic voltammetry cycles, which enhances the electrochemical stability by blocking crystallization. Further, this approach provides a general strategy for preparing free-standing MGNPs with high surface activities, which may have widespread functional applications

36 MATERIALS SCIENCE↗
DOE OSTI2023

Tailoring planar slip to achieve pure metal-like ductility in body-centred-cubic multi-principal element alloys

Uniform tensile ductility (UTD) is crucial for the forming/machining capabilities of structural materials. Normally, planar-slip induced narrow deformation bands localize the plastic strains and hence hamper UTD, particularly in body-centred-cubic (bcc) multi-principal element high-entropy alloys (HEAs), which generally exhibit early necking (UTD < 5%). Here we demonstrate a strategy to tailor the planar-slip bands in a Ti-Zr-V-Nb-Al bcc HEA, achieving a 25% UTD together with nearly 50% elongation-to-failure (approaching a ductile elemental metal), while offering gigapascal yield strength. The HEA composition is designed not only to enhance the B2-like local chemical order (LCO), seeding sites to disperse planar slip, but also to generate excess lattice distortion upon deformation-induced LCO destruction, which promotes elastic strains and dislocation debris to cause dynamic hardening. Further, this encourages second-generation planar-slip bands to branch out from first-generation bands, effectively spreading the plastic flow to permeate the sample volume. Moreover, the profuse bands frequently intersect to sustain adequate work-hardening rate (WHR) to large strains. Our strategy showcases the tuning of plastic flow dynamics that turns an otherwise-undesirable deformation mode to our advantage, enabling an unusual synergy of yield strength and UTD for bcc HEAs.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Laser additive manufacturing for infrastructure repair: A case study of a deteriorated steel bridge beam

As our transportation infrastructure ages, its deterioration is becoming a growing concern. Rapid and effective methods for repair can reduce the need for time-and cost-intensive replacement of structures such as roadway bridges. In this work, laser-based additive manufacturing (AM) was developed for the re-pair of damaged beams in steel bridges. A corroded structural beam of low-carbon A36 steel was selected for this case study and 316L stainless steel was used for repair due to its excellent mechanical properties and corrosion resistance. Simulated repair experiments were performed on specimens extracted from the beam, and prepared with various groove shapes (Rectangular, Trapezoidal, and U-shaped). More in-depth parametric and microstructural studies were carried out with a series of U-shaped specimens repaired with the linear laser input energy varied from 19.5 to 30.0 J mm -1 . The tensile properties of the repaired specimens and interface structures were also investigated in detail. It was found that the repaired specimens had a slightly higher tensile strength despite a reduction in tensile elongation compared to the A36 steel base metal. The influence of interfacial microstructure and heterogeneity on the mechanical proper-ties of the repaired specimens was discussed. Furthermore, our work suggests the promising potential to employ AM for structural repair and provides fundamental insights into processing-structure-property relationships in laser AM-repaired materials.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Correlations of multiscale structural evolution and homogeneous flows in metallic glass ribbons

Studying the flow behavior is critical to understand the deformation mechanism of amorphous solids. However, detecting the basic flow events in amorphous solids is challenging. Here, by simultaneous SAXS/WAXS, elementary flow carriers in wound metallic glasses are identified from flow-induced structural heterogeneities with a radius of gyration of 2.5~3.5 nm. Their size increases and morphology changes from sphere-like to rod-like under flow. Moreover, the atomic structure exhibits an unusual change to a more disordered state during winding/annealing at the temperature of ~0.8 T g . This work provides an atomic-to-nanoscale description of the flow carriers of amorphous solids during deformation. Impact Statement The elementary flow carriers in metallic glasses have a radius of gyration of 2.5~3.5 nm. During flow, their size increases and morphology changes from sphere-like to rod-like.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Synchrotron x-Ray Study of Heterostructured Materials: A Review

Heterostructured materials (HSMs) have shown great potential for breaking the strength-ductility tradeoff. HSMs consist of heterogeneous zones that may have different sizes, shapes, compositions, structures, etc. Interactions and competitions among them often lead to unprecedented properties. However, due to the complex structures in a broad range of length scales, it is challenging to unravel deformation physics and strengthening mechanisms underlying extraordinary mechanical properties. Synchrotron x-rays provide powerful techniques and indispensable tools for investigating HSMs at various length scales. Here, we will present in situ high-energy x-ray diffraction and Laue x-ray microdiffraction techniques and their application in studying the HSMs. In this study, the principles of these techniques will be briefly introduced. We will focus on their application in studying stress partitioning and plastic accommodation during tensile deformation, thermo-driven and/or stress-driven phase transformations and various deformation microstructures like geometrically necessary dislocations and local stress/strain distributions, etc., in HSMs. Some important findings will be summarized. Challenging issues remain in studying HSMs and will be discussed.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Emergence of high piezoelectricity from competing local polar order-disorder in relaxor ferroelectrics

Relaxor ferroelectrics are known for outstanding piezoelectric properties, finding a broad range of applications in advanced electromechanical devices. Decoding the origins of the enhanced properties, however, have long been complicated by the heterogeneous local structures. Here, we employ the advanced big-box refinement method by fitting neutron-, X-ray-based total scattering, and X-ray absorption spectrum simultaneously, to extract local atomic polar displacements and construct 3D polar configurations in the classical relaxor ferroelectric Pb(Mg 1/3 Nb 2/3 )O 3 –PbTiO 3 . Our results demonstrate that prevailing order-disorder character accompanied by the continuous rotation of local polar displacements commands the composition-driven global structure evolution. The omnidirectional local polar disordering appears as an indication of macroscopic relaxor characteristics. Combined with phase-field simulations, it demonstrates that the competing local polar order-disorder between different states with balanced local polar length and direction randomness leads to a flattening free-energy profile over a wide polar length, thus giving rise to high piezoelectricity. Our work clarifies that the critical structural feature required for high piezoelectricity is the competition states of local polar rather than relaxor.

42 ENGINEERING↗
DOE OSTI2023

P2-Type Moisture-Stable and High-Voltage-Tolerable Cathodes for High-Energy and Long-Life Sodium-Ion Batteries

P2-Na 0.67 Ni 0.33 Mn 0.67 O 2 represents a promising cathode for Na-ion batteries, but it suffers from severe structural degradation upon storing in a humid atmosphere and cycling at a high cutoff voltage. Here we propose an in situ construction to achieve simultaneous material synthesis and Mg/Sn cosubstitution of Na 0.67 Ni 0.33 Mn 0.67 O 2 via one-pot solid-state sintering. Here, the materials exhibit superior structural reversibility and moisture insensitivity. In-operando XRD reveals an essential correlation between cycling stability and phase reversibility, whereas Mg substitution suppressed the P2–O2 phase transition by forming a new Z phase, and Mg/Sn cosubstitution enhanced the P2–Z transition reversibility benefiting from strong Sn–O bonds. DFT calculations disclosed high chemical tolerance to moisture, as the adsorption energy to H 2 O was lower than that of the pure Na 0.67 Ni 0.33 Mn 0.67 O 2 . A representative Na 0.67 Ni 0.23 Mg 0.1 Mn 0.65 Sn 0.02 O 2 cathode exhibits high reversible capacities of 123 mAh g –1 (10 mA g –1 ), 110 mAh g –1 (200 mA g –1 ), and 100 mAh g –1 (500 mA g –1 ) and a high capacity retention of 80% (500 mA g –1 , 500 cycles).

25 ENERGY STORAGE↗
DOE OSTI2023

Achieving giant electrostrain of above 1% in (Bi,Na)TiO 3 -based lead-free piezoelectrics via introducing oxygen-defect composition

Piezoelectric ceramics have been extensively used in actuators, where the magnitude of electrostrain is key indicator for large-stroke actuation applications. Here, we propose an innovative strategy based on defect chemistry to form a defect-engineered morphotropic phase boundary and achieve a giant strain of 1.12% in lead-free Bi 0.5 Na 0.5 TiO 3 (BNT)–based ceramics. The incorporation of the hypothetical perovskite BaAlO 2.5 with nominal oxygen defect into BNT will form strongly polarized directional defect dipoles, leading to a strong pinning effect after aging. The large asymmetrical strain is mainly attributed to two factors: The defect dipoles along crystallographic [001] direction destroy the long-range ordering of the ferroelectric and activate a reversible phase transition while promoting polarization rotation when the dipoles are aligned along the applied electric field. Our results not only demonstrate the potential application of BNT-based materials in low-frequency, large-stroke actuators but also provide a general methodology to achieve large strain.

36 MATERIALS SCIENCE↗
DOE OSTI2023

High-Performance Layered Ni-Rich Cathode Materials Enabled by Stress-Resistant Nanosheets

Here, layered O3-type transition metal oxides are promising cathode candidates for high-energy-density Li-ion batteries. However, the structural instability at the highly delithiated state and low kinetics at the fully lithiated state are arduous challenges to overcome. Here, a facile approach is developed to make secondary particles of Ni-rich materials with nanosheet primary grains. Because the alignment of the primary grains reduces internal stress buildup within the particle during charge-discharge and provides straightforward paths for Li transport, the as-synthesized Ni-rich materials do not undergo cracking upon cycling with higher overall Li + ion diffusion rates. Specifically, a LiNi 0.75 Co 0.14 Mn 0.11 O 2 cathode with nanosheet grains delivers a high reversible capacity of 206 mAh g -1 and shows ultrahigh cycling stability, e.g., 98% capacity retention over 500 cycles in a full cell with a graphite anode.

25 ENERGY STORAGE↗
DOE OSTI2023

An Innovative Insight into Performance Degradation of NCM111 Cathode Induced by Suspension of Operation

The lifespan of lithium-ion batteries varies enormously from fundamental study to practical applications. This big difference has been typically ascribed to the high degree of uncertainty in unpredictable and complicated operation conditions in real-life applications. Here, in this paper, we report that the pause of the charging–discharging process, which is frequently operated in practice but rarely studied in academics, is an important reason for the performance degradation of the NCM111 cathode. It is found that the pause during cycling could trigger a remarkable drop in capacity, giving rise to ~30% more capacity decay compared with the continuously cycled sample. In situ synchrotron X-ray diffraction analysis reveals that the harmful H1–H2 phase transition, which typically appears in the initial cycle but disappears in subsequent cycles, is reactivated by the pausing process. The anisotropic lattice strains that occur during the H1–H2 transition result in mechanical fractures that terminate with an inert NiO-type rock-salt phase on the surface of particles. The present study indicates that the discontinuous usage of rechargeable batteries is also a key factor for cycle life, which might provide a distinct perspective on the performance decay in practical applications.

25 ENERGY STORAGE↗
DOE OSTI2023

Coordination Polymer Electrocatalysts Enable Efficient CO‐to‐Acetate Conversion

Abstract Upgrading carbon dioxide/monoxide to multi‐carbon C 2+ products using renewable electricity offers one route to more sustainable fuel and chemical production. One of the most appealing products is acetate, the profitable electrosynthesis of which demands a catalyst with higher efficiency. Here, a coordination polymer (CP) catalyst is reported that consists of Cu(I) and benzimidazole units linked via Cu(I)‐imidazole coordination bonds, which enables selective reduction of CO to acetate with a 61% Faradaic efficiency at −0.59 volts versus the reversible hydrogen electrode at a current density of 400 mA cm −2 in flow cells. The catalyst is integrated in a cation exchange membrane‐based membrane electrode assembly that enables stable acetate electrosynthesis for 190 h, while achieving direct collection of concentrated acetate (3.3 molar) from the cathodic liquid stream, an average single‐pass utilization of 50% toward CO‐to‐acetate conversion, and an average acetate full‐cell energy efficiency of 15% at a current density of 250 mA cm −2 .

Luo, Mingchuan↗
DOE OSTI2023

Amino-tethering synthesis strategy toward highly accessible sub-3-nm L1 0 -PtM catalysts for high-power fuel cells

Because of the poor accessibility of embedded active sites, platinum (Pt)-based electrocatalysts suffer from insufficient Pt utilization and mass transport in membrane electrode assemblies (MEAs), limiting their performance in polymer electrolyte membrane fuel cells. Here, we report a simple and universal approach to depositing sub-3-nm L1 0 -PtM nanoparticles over external surfaces of carbon supports through pore-tailored amino (NH 2 )-modification, which enables not only excellent activity for the oxygen reduction reaction, but also enhanced Pt utilization and mass transport in MEAs. Using a low loading of 0.10 mg Pt ∙cm -2 , the MEA of PtCo/KB-NH 2 delivered an excellent mass activity of 0.691 A∙mgPt -1 , a record-high power density of 0.96 W∙cm -2 at 0.67 V, and only a 30-mV drop at 0.80 A∙cm -2 after 30,000 voltage cycles, which meets nearly all targets set by the Department of Energy. Finally, this work provides an efficient strategy for designing advanced Pt-based electrocatalysts and realizing high-power fuel cells.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
DOE OSTI2023

Reversible Iron Oxyfluoride (FeOF)–Graphene Composites as Sustainable Cathodes for High Energy Density Lithium Batteries

Two large barriers are impeding the wide implementation of electric vehicles, namely driving-range and cost, primarily due to the low specific energy and high cost of mono-valence cathodes used in lithium-ion batteries. Iron is the ideal element for cathode materials considering its abundance, low cost and toxicity. However, the poor reversibility of (de)lithiation and low electronic conductivity prevent iron-based high specific energy multi-valence conversion cathodes from practical applications. In this work, a sustainable FeOF nanocomposite is developed with extraordinary performance. The specific capacity and energy reach 621 mAh g –1 and 1124 Wh kg –1 with more than 100 cycles, which triples the specific capacity, and doubles the specific energy of current mono-valence intercalation LiCoO 2 . This is the result of an effective approach, combing the nanostructured FeOF with graphene, realized by making the (de)lithiation reversible by immobilizing FeOF nanoparticles and the discharge products over the graphene surface and providing the interparticle electric conduction. Importantly, it demonstrates that introducing small amount of graphene can create new materials with desired properties, opening a new avenue for altering the (de)lithiation process. Finally, such extraordinary performance represents a significant breakthrough in developing sustainable conversion materials, eventually overcoming the driving range and cost barriers.

25 ENERGY STORAGE↗
DOE OSTI2023

All-temperature zinc batteries with high-entropy aqueous electrolyte

Electrification of transportation and rising demand for grid energy storage continue to build momentum around batteries across the globe. However, the supply chain of Li-ion batteries is exposed to the increasing challenges of resourcing essential and scarce materials. Therefore, incentives to develop more sustainable battery chemistries are growing. Here, in this paper, we show an aqueous ZnCl 2 electrolyte with introduced LiCl as supporting salt. Once the electrolyte is optimized to Li 2 ZnCl 4 ∙9H 2 O, the assembled Zn–air battery can sustain stable cycling over the course of 800 hours at a current density of 0.4 mA cm -2 between -60 °C and +80 °C, with 100% Coulombic efficiency for Zn stripping/plating. Even at -60 °C, >80% of room-temperature power density can be retained. Advanced characterization and theoretical calculations reveal a high-entropy solvation structure that is responsible for the excellent performance. The strong acidity allows ZnCl 2 to accept donated Cl - ions to form ZnCl 4 2- anions, while water molecules remain within the free solvent network at low salt concentration or coordinate with Li ions. Our work suggests an effective strategy for the rational design of electrolytes that could enable next-generation Zn batteries.

25 ENERGY STORAGE↗