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Li, Jing

Publications and source records attributed to Li, Jing.

At least 145 records · Page 8

Eco-friendly, solution-processable and efficient low-energy lighting phosphors: copper halide based hybrid semiconductors Cu 4 X 6 (L) 2 (X = Br, I) composed of covalent, ionic and coordinate bonds

A series of copper halide based inorganic–organic hybrid semiconductors have been synthesized. Structural analysis confirms that all compounds are composed of one-dimensional Cu 4 X 6 2- anionic chains that coordinate to cationic ligands via Cu–N dative bonds. Different coordination affinities of the ligands lead to two types of ligand arrangements with various structural distortions. All compounds are highly resistant to heat and moisture as a result of the combination of coordinate and ionic bonds. Low energy emission with high efficiency is achieved for these compounds and the emission energy (~552–615 nm) and color (yellow-orange) can be tuned by varying the ligand and halogen element. The electronic structure and luminescence mechanism are examined by both experimental and theoretical methods. More importantly, all compounds demonstrate good solubility in polar aprotic solvents, a desired property that is absent in all other CuX hybrid families of extended structures, which is attributed primarily to the ionic nature of this material class. Furthermore, the good solution-processability, and cost effective and easily scalable synthesis coupled with high quantum efficiencies and framework stability make these hybrid materials promising phosphors for general lighting applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

A robust and multifunctional calcium coordination polymer as a selective fluorescent sensor for acetone and iron (+3) and as a tunable proton conductor

A multifunctional calcium coordination polymer (Ca-CP) formulated as [(CH 3 ) 2 NH 2 ][Ca(Me 2 tcpbH)(H 2 O)] (1) has been synthesized and characterized. Compound 1 features a robust and novel three-dimensional (3D) network with cage-like cavities. The high thermal and moisture stability of the title compound makes it a good candidate for possible environment or energy related applications. Fluorescence (FL) studies demonstrate that 1 shows emission with a maximum at 350 nm under 270 nm excitation. The title compound acts as a selective and sensitive fluorescent sensor for the detection of acetone and Fe 3+ ions at low concentrations. The FL intensity quenching percentage and the concentration ratio of Fe 3+ /Fe 2+ showed a linear relation with a Fe 3+ concentration as low as 50 μM in Fe 2+ aqueous solutions, offering an easy way to probe the extent of Fe 2+ oxidation. Moreover, due to the relatively high hydration character of Ca 2+ , the terminal water molecules and undeprotonated carboxylate groups form a strong hydrogen-bonded network within the structure, facilitating its tunable proton conduction under various humidity and temperature conditions. The proton conducting mechanism has been investigated using PXRD, IR, and EA methods.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Spontaneous Valley Polarization of Interacting Carriers in a Monolayer Semiconductor

Here, we report magnetoabsorption spectroscopy of gated WSe 2 monolayers in high magnetic fields up to 60 T. When doped with a 2D Fermi sea of mobile holes, well-resolved sequences of optical transitions are observed in both σ ± circular polarizations, which unambiguously and separately indicate the number of filled Landau levels (LLs) in both K and K ' valleys. This reveals the interaction-enhanced valley Zeeman energy, which is found to be highly tunable with hole density p . We exploit this tunability to align the LLs in K and K ' , and find that the 2D hole gas becomes unstable against small changes in LL filling and can spontaneously valley polarize. These results cannot be understood within a single-particle picture, highlighting the importance of exchange interactions in determining the ground state of 2D carriers in monolayer semiconductors.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Porous Ti-MOF-74 Framework as a Strong-Binding Nitric Oxide Scavenger

Combining synthesis, infrared spectroscopy, and ab initio modeling we show that the titanium-based porous framework Ti-MOF-74 has potential as an environmental nitric oxide (NO) scavenger, exhibiting an extraordinarily strong binding affinity and selectivity over other flue-gas components. The robustness upon exposure to water vapor and high flue-gas stack temperatures suggests that this material can perform well in an industrial environment. In-depth analysis of the Ti-NO bond indicates that the NO forms a strong covalent bond with the Ti. The process of this NO bond formation involves a reaction with the OH- capping groups of the Ti to form NO x groups, after which the excess NO binds to the open Ti metal sites. Ti-MOF-74 thus becomes, to the best of our knowledge, the first known porous framework that binds NO significantly stronger than water, providing novel avenues for environmental and physiological scavenging applications.

36 MATERIALS SCIENCE↗

A fundamental look at electrocatalytic sulfur reduction reaction

The fundamental kinetics of the electrocatalytic sulfur reduction reaction (SRR), a complex 16-electron conversion process in lithium–sulfur batteries, is so far insufficiently explored. In this study, by directly profiling the activation energies in the multistep SRR, we reveal that the initial reduction of sulfur to the soluble polysulfides is relatively easy owing to the low activation energy, whereas the subsequent conversion of the polysulfides into the insoluble Li 2 S 2 /Li 2 S has a much higher activation energy, contributing to the accumulation of polysulfides and exacerbating the polysulfide shuttling effect. We use heteroatom-doped graphene as a model system to explore electrocatalytic SRR. We show that nitrogen and sulfur dual-doped graphene considerably reduces the activation energy to improve SRR kinetics. Density functional calculations confirm that the doping tunes the p-band centre of the active carbons for an optimal adsorption strength of intermediates and electroactivity. This study establishes electrocatalysis as a promising pathway to tackle the fundamental challenges facing lithium–sulfur batteries.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Surface oxygenation of multicomponent nanoparticles toward active and stable oxidation catalysts

Abstract The need for active and stable oxidation catalysts is driven by the demands in production of valuable chemicals, remediation of hydrocarbon pollutants and energy sustainability. Traditional approaches focus on oxygen-activating oxides as support which provides the oxygen activation at the catalyst-support peripheral interface. Here we report a new approach to oxidation catalysts for total oxidation of hydrocarbons (e.g., propane) by surface oxygenation of platinum (Pt)-alloyed multicomponent nanoparticles (e.g., platinum-nickel cobalt (Pt–NiCo)). The in-situ/operando time-resolved studies, including high-energy synchrotron X-ray diffraction and diffuse reflectance infrared Fourier transform spectroscopy, demonstrate the formation of oxygenated Pt–NiOCoO surface layer and disordered ternary alloy core. The results reveal largely-irregular oscillatory kinetics associated with the dynamic lattice expansion/shrinking, ordering/disordering, and formation of surface-oxygenated sites and intermediates. The catalytic synergy is responsible for reduction of the oxidation temperature by ~100 °C and the high stability under 800 °C hydrothermal aging in comparison with Pt, and may represent a paradigm shift in the design of self-supported catalysts.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Thermally Activated Adsorption in Metal–Organic Frameworks with a Temperature‐Tunable Diffusion Barrier Layer

Abstract Modification of the external surfaces of metal–organic frameworks offers a new level of control over their adsorption behavior. It was previously shown that capping of MOFs with ethylenediamine (EDA) can effectively retain small gaseous molecules at room temperature. Reported here is a temperature‐induced variation in the capping‐layer gate‐opening mechanism through a combination of in situ infared experiments and ab initio simulations of the capping layer. An atypical acceleration and increase in the loading of weakly adsorbed molecules upon raising the temperature above room temperature is observed. These findings show the discovery of novel temperature‐dependent kinetics that goes beyond standard kinetics and suggest a new avenue for tailoring selective adsorption by thermally tuning the surface barrier.

Tan, Kui↗

Functional metal–organic frameworks as effective sensors of gases and volatile compounds

Developing efficient sensor materials with superior performance for selective, fast and sensitive detection of gases and volatile organic compounds (VOCs) is essential for human health and environmental protection, through monitoring indoor and outdoor air pollutions, managing industrial processes, controlling food quality and assisting early diagnosis of diseases. Metal–organic frameworks (MOFs) are a unique type of crystalline and porous solid material constructed from metal nodes (metal ions or clusters) and functional organic ligands. They have been investigated extensively for possible use as high performance sensors for the detection of many different gases and VOCs in recent years, due to their large surface area, tunable pore size, functionalizable sites and intriguing properties, such as electrical conductivity, magnetism, ferroelectricity, luminescence and chromism. The high porosity of MOFs allows them to interact strongly with various analytes, including gases and VOCs, thus resulting in easily measurable responses to different physicochemical parameters. Although much of the recent work on MOF-based luminescent sensors have been summarized in several excellent reviews (up to 2018), a comprehensive overview of these materials for sensing gases and VOCs based on chemiresistive, magnetic, ferroelectric, and colorimertic mechanisms is missing. In this review, we highlight the most recent progress in developing MOF sensing and switching materials with an emphasis on sensing mechanisms based on electricity, magnetism, ferroelectricity and chromism. We provide a comprehensive analysis on the MOF–analyte interactions in these processes, which play a key role in the sensing performance of the MOF-based sensors and switches. We discuss in detail possible applications of MOF-based sensing and switching materials in detecting oxygen, water vapor, toxic industrial gases (such as hydrogen sulfide, ammonia, sulfur dioxide, nitrous oxide, carbon oxides and carbon disulfide) and VOCs (such as aromatic and aliphatic hydrocarbons, ketones, alcohols, aldehydes, chlorinated hydrocarbons and N,N'-dimethylformamide). Altogether, this review serves as a timely source of information and provides insight for the future development of advanced MOF materials as next-generation gas and VOC sensors.

36 MATERIALS SCIENCE↗

Surface-Mediated Interconnections of Nanoparticles in Cellulosic Fibrous Materials toward 3D Sensors

Fibrous materials serve as an intriguing class of 3D materials to meet the growing demands for flexible, foldable, biocompatible, biodegradable, dis- posable, inexpensive, and wearable sensors and the rising desires for higher sensitivity, greater miniaturization, lower cost, and better wearability. The use of such materials for the creation of a fibrous sensor substrate that interfaces with a sensing film in 3D with the transducing electronics is however difficult by conventional photolithographic methods. Here, a highly effective pathway featuring surface-mediated interconnection (SMI) of metal nanoclusters (NCs) and nanoparticles (NPs) in fibrous materials at ambient conditions is demon- strated for fabricating fibrous sensor substrates or platforms. Bimodally distrib- uted gold–copper alloy NCs and NPs are used as a model system to demonstrate the semiconductive-to-metallic conductivity transition, quantized capacitive charging, and anisotropic conductivity characteristics. Upon coupling SMI of NCs/NPs as electrically conductive microelectrodes and surface-mediated assembly (SMA) of the NCs/NPs as chemically sensitive interfaces, the resulting fibrous chemiresistors function as sensitive and selective sensors for gaseous and vaporous analytes. Finally, this new SMI–SMA strategy has significant implications for manufacturing high-performance fibrous platforms to meet the growing demands of the advanced multifunctional sensors and biosensors.

36 MATERIALS SCIENCE↗

Solid-state neutron detector

A method for fabricating a neutron detector includes providing an epilayer wafer of Boron-10 enriched hexagonal boron nitride (h-10BN or h-BN or 10BN or BN) having a thickness (t), dicing or cutting the epilayer wafer into one or more BN strips having a width (W) and a length (L), and depositing a first metal contact on a first surface of at least one of the BN strip and a second metal contact on a second surface of the at least one BN strip. The neutron detector includes an electrically insulating submount, a BN epilayer of Boron-10 enriched hexagonal boron nitride (h-10BN or h-BN or 10BN or BN) placed on the insulating submount, a first metal contact deposited on a first surface of the BN epilayer, and a second metal contact deposited on a second surface of the BN epilayer.

36 MATERIALS SCIENCE↗

Designer Metal–Organic Frameworks for Size–Exclusion–Based Hydrocarbon Separations: Progress and Challenges

The separation of hydrocarbons is of primary importance in the petrochemical industry but remains a challenging process. Hydrocarbon separations have traditionally relied predominantly on costly and energy intensive heat-driven procedures such as low temperature distillations. Adsorptive separation based on porous solids represents an alternative technology that is potentially more energy efficient for the separation of some hydrocarbons. Great efforts have been made recently not only on the development of adsorbents with optimal separation performance but also towards the subsequent implementation of adsorption-based separation technology. Emerging as a relatively new class of multifunctional porous materials, metal-organic frameworks hold substantial promise as adsorbents for highly efficient separation of hydrocarbons. This is because of their exceptional and intrinsic porosity tunability which enables size-exclusion based separations that render the highest possible separation selectivity. In this review, we highlight the recent advances in the development of MOFs for separation of selected groups of hydrocarbons, including methane/C2 hydrocarbons, normal alkanes, alkane isomers, alkane/alkene/alkyne, and C8 alkylaromatics, with a particular focus on separations based on size-exclusion mechanism. Insights into tailor-made structures, material design strategies, and structure-property relations will be elucidated. In addition, the existing challenges and possible future directions of this important research field will be discussed.

36 MATERIALS SCIENCE↗

Thermally activated adsorption in metal–organic frameworks with a temperature–tunable diffusion barrier layer

Modification of the external surfaces of metal organic frameworks offers a new level of control over their adsorption behavior. Here, we have previously shown that capping of MOFs with ethylenediamine (EDA) can effectively retain small gaseous molecules at room temperature. Here, we report a temperature–induced variation in the capping–layer gate opening mechanism through a combination of in situ IR experiments and ab initio simulations of the capping layer. We find an atypical acceleration and increase in the loading of weakly adsorbed molecules upon raising the temperature above room temperature. Our findings show the discovery of a novel temperature–dependent kinetics that goes beyond standard kinetics and suggest a new avenue for tailoring selective adsorption by thermally tuning the surface barrier.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Theoretical Development of Controller Transfer applied to Dynamical Systems

Data-driven control strategies suffer from the necessity of training and its associated computational time and cost. This motivates the continuous increase of popularity of transfer learning based methods. In this paper, we have investigated transfer learning in the context of controller for dynamical systems. First, we have derived conditions under which controller can be transferred between two linear dynamical systems. Furthermore, we have introduced a novel algorithm to design the transferable and non-transferable control components for linear systems. Secondly, we have derived conditions under which a stabilizing controller can be transferred between two different nonlinear dynamical systems. Furthermore, we have used the notion of zero dynamics to transform the nonlinear dynamics into global normal form, to derive the transferability conditions on the controller. Finally, we have numerically evaluated the performance of our transfer learning based methods for two sets of example linear and nonlinear dynamical systems.

Chakraborty, Indrasis↗

Improving Solution Accuracy and Convergence for Stochastic Physics Parameterizations with Colored Noise

Stochastic parameterizations are used in numerical weather prediction and climate modeling to help capture the uncertainty in the simulations and improve their statistical properties. Convergence issues can arise when time integration methods originally developed for deterministic differential equations are applied naively to stochastic problems. In previous studies, it has been demonstrated that a correction term, known in stochastic analysis as the Itô correction, can help improve solution accuracy for various deterministic numerical schemes and ensure convergence to the physically relevant solution without substantial computational overhead. The usual formulation of the Itô correction is valid only when the stochasticity is represented by white noise. In this study, a generalized formulation of the Itô correction is derived for noises of any color. The formulation is applied to a test problem described by an advection–diffusion equation forced with a spectrum of fast processes. We present numerical results for cases with both constant and spatially varying advection velocities to show that, for the same time step sizes, the introduction of the generalized Itô correction helps to substantially reduce time integration error and significantly improve the convergence rate of the numerical solutions when the forcing term in the governing equation is rough (fast varying); alternatively, for the same target accuracy, the generalized Itô correction allows for the use of significantly longer time steps and, hence, helps to reduce the computational cost of the numerical simulation.

54 ENVIRONMENTAL SCIENCES↗