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Jin, Song

Publications and source records attributed to Jin, Song.

31 records · Page 2
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Defect-mediated ferromagnetism in correlated two-dimensional transition metal phosphorus trisulfides

Controlling the magnetic spin states of two-dimensional (2D) van der Waals (vdW) materials with strong electronic or magnetic correlation is important for spintronic applications but challenging. Crystal defects that are often present in 2D materials such as transition metal phosphorus trisulfides (MPS 3 ) could influence their physical properties. Here, we report the effect of sulfur vacancies on the magnetic exchange interactions and spin ordering of few-layered vdW magnetic Ni 1-x Co x PS 3 nanosheets. Magnetic and structural characterization in corroboration with theoretical calculations reveal that sulfur vacancies effectively suppress the strong intralayer antiferromagnetic correlation, giving rise to a weak ferromagnetic ground state in Ni 1-x Co x PS 3 nanosheets. Notably, the magnetic field required to tune this ferromagnetic state (<300 Oe) is much lower than the value needed to tune a typical vdW antiferromagnet (> several thousand oersted). These findings provide a previously unexplored route for controlling competing correlated states and magnetic ordering by defect engineering in vdW materials.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Modifying redox properties and local bonding of Co 3 O 4 by CeO 2 enhances oxygen evolution catalysis in acid

Developing efficient and stable earth-abundant electrocatalysts for acidic oxygen evolution reaction is the bottleneck for water splitting using proton exchange membrane electrolyzers. Here, we show that nanocrystalline CeO 2 in a Co 3 O 4 /CeO 2 nanocomposite can modify the redox properties of Co 3 O 4 and enhances its intrinsic oxygen evolution reaction activity, and combine electrochemical and structural characterizations including kinetic isotope effect, pH- and temperature-dependence, in situ Raman and ex situ X-ray absorption spectroscopy analyses to understand the origin. The local bonding environment of Co 3 O 4 can be modified after the introduction of nanocrystalline CeO 2 , which allows the CoIII species to be easily oxidized into catalytically active CoIV species, bypassing the potential-determining surface reconstruction process. Co 3 O 4 /CeO 2 displays a comparable stability to Co 3 O 4 thus breaks the activity/stability tradeoff. This work not only establishes an efficient earth-abundant catalysts for acidic oxygen evolution reaction, but also provides strategies for designing more active catalysts for other reactions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Anion Exchange of Ruddlesden–Popper Lead Halide Perovskites Produces Stable Lateral Heterostructures

Heterostructures of three-dimensional (3D) halide perovskites are unstable because of facile anion interdiffusion at halide interfaces. Two-dimensional (2D) Ruddlesden–Popper halide perovskites (RPPs) show suppressed and anisotropic ion diffu-sion that could enable stable RPP heterostructures, yet the direct and general growth of lateral RPP heterostructures remains challenging. Here we show that halide miscibility in RPPs decreases with perovskite layer thickness (n), enabling the for-mation of sharp halide lateral heterostructures from n = 1 and 2 RP lead iodide microplates via anion exchange with hydro-gen bromide vapor. In contrast, RPPs with n = 3 form more diffuse lateral heterojunctions, more similar to those in 3D perov-skites. The anion exchange behaviors are further modulated by the spacer and A-site cations in the RPP structures. These new insights, and kinetic studies of the exchange reactions, enable the preparation of lateral heterostructures from various n = 2 RPPs that are more stable against anion interdiffusion and degradation for potential device applications.

Roy, Chris R.↗
DOE OSTI2021

Stable Tetrasubstituted Quinone Redox Reservoir for Enhancing Decoupled Hydrogen and Oxygen Evolution

In this report, we discuss Redox reservoirs (RRs) that may be used to decouple the two half-reactions of water electrolysis, enabling the spatial and temporal separation of hydrogen and oxygen evolution. Organic RRs are appealing candidates for this application; however, their instability limits their utility. Here we show that a tetrathioether-substituted quinone, tetramercaptopropanesulfonate quinone (TMQ), exhibits significantly enhanced stability relative to anthraquinone-2,7-disulfonate, the most effective organic RR reported previously. The enhanced stability, confirmed by symmetric flow-battery experiments under relevant conditions, enables the stable electrochemical production of H 2 and O 2 in a continuous-flow electrolysis cell. The reduced RR, tetramercaptopropanesulfonate hydroquinone, is not susceptible to decomposition, whereas the oxidized state, TMQ, undergoes slow decomposition, evident only after sustained operation (>60 h). The analysis of the byproducts provides a basis for a decomposition mechanism, establishing a foundation for the design of new organic RRs with even better performance.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Modular Electrochemical Synthesis Using a Redox Reservoir Paired with Independent Half-Reactions

Electrochemical synthesis of high-value chemicals using renewable electricity could lead to sustainability advantages over conventional chemical manufacturing. The tight coupling between paired anodic and cathodic reactions in conventional electrochemical processes, however, constrains the products and their efficiencies. Here, we demonstrate a strategy to achieve modular electrochemical synthesis (ModES) of different chemicals by decoupling and pairing the oxidative and reductive half-reactions with a heterogeneous redox reservoir (RR). Specifically, sodium nickel hexacyanoferrate (NaNiHCF) can serve as a robust and reversible RR that enables the modular production of several strong oxidants, hydrogen peroxide (H 2 O2) and sodium persulfate (Na 2 S 2 O 8 ) or active chlorine, in separate RR-coupled electrochemical processes. The system’s excellent performance and operational stability is demonstrated by continuous operation over 100 cycles (~36 h) to produce H 2 O 2 and Na 2 S 2 O 8 with a high voltage efficiency. The concept presented here highlights the prospects for using RRs to enable efficient, modular, and on-demand electrochemical synthesis of valuable chemicals.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Supertwisted spirals of layered materials enabled by growth on non-Euclidean surfaces

Using curves to make twists The growth of layered materials on flat substrates usually occurs in stacked layers, although defects or a lattice mismatch can induce strains that distort the shape of subsequent layers. However, these effects are usually small and can be uncontrolled. Zhao et al. now demonstrate the possibility of synthesizing multilayers of two-dimensional materials with certain twists between the layers induced by the presence of screw dislocations in combination with curved substrate surfaces. Different twist angles are achieved by varying the amount of nonplanarity and the character (conical or hyperbolic) of the surface. Science , this issue p. 442

Science & Technology - Other Topics↗
DOE OSTI2020

Quantum interference between the optical Stark effect and resonant harmonic generation in WS 2

An applied field can modulate optical signals by resonance shifting via the Stark effect. The optical Stark effect uses ultrafast light in the transparency region of a material to shift resonances with speeds limited by the pulse duration or system coherence. In this Rapid Communication, we investigate the optical Stark effect in resonant optical harmonic generation using the A exciton transition of WS 2 . Multidimensional pump-harmonic-probe measurements, in which the probe is second- or third-harmonic emission, reveal not only large Stark shifts that are commensurate with the large optical susceptibilities common to WS 2 excitons, but also behaviors more complex than simple optical Stark effect treatments predict. We show how another manifestation of the Stark effect, brought forth by coherent photon exchange between the pump and harmonic generation fundamental fields, can strongly enhance or suppress harmonic generation.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗