Strong Interaction Research Articles

Incorporation of Pd Single-atom Sites in Perovskite with an Excellent Selectivity toward Photocatalytic Semihydrogenation of Alkynes.

Semihydrogenation is a crucial industrial process. Noble metals such as Pd have been extensively studied in semihydrogenation reactions, owing to their unique catalytic activity toward hydrogen activation. However, the overhydrogenation of alkenes to alkanes often happens due to the rather strong adsorption of alkenes on Pd active phases. Herein, we demonstrate that the incorporation of Pd active phases as single-atom sites in perovskite lattices such as SrTiO3 can greatly alternate the electronic structure and coordination environment of Pd active phases to facilitate the desorption of alkenes rather than further hydrogenation. Furthermore, the incorporated Pd sites can be well stabilized without sintering by a strong host-guest interaction with SrTiO3 during the activation of H species in hydrogenation reactions. As a result, the Pd incorporated SrTiO3 (Pd-SrTiO3) exhibits an excellent time-independent selectivity (> 99.9 %) and robust durability for the photocatalytic semihydrogenation of phenylacetylene to styrene. This strategy based on incorporation of active phases in perovskite lattices will have broad implications in the development of high-performance photocatalysts for selective hydrogenation reactions.

A colorimetric platform for sensitive sensing of Hg2+ and S2− based on Se-AuNPs with Hg2+-activated peroxidase-like activity

Herein, the selenium (Se) modified gold nanoparticles (Se-AuNPs) was synthesized using cerium doped carbon dots (Ce-CDs) as a reducing agent and template. As desired, Se-AuNPs displays enhanced peroxidase (POD)-like activity in the presence of Hg2+. The mechanism for the enhanced activity was attributed to the increased affinity between Se-AuNPs-Hg2+ and the substrate, in which Se and Au elements have a strong binding capacity to Hg2+, forming Hg–Se bonds and Au–Hg amalgam to generate more ·OH. This POD-like activity of Se-AuNPs-Hg2+ correlates with the colorimetric reaction by the catalytic reaction between 3,3′,5,5′-tetramethylbenzidine (TMB) and H2O2. The oxidation of TMB was completely inhibited by the introduction of the reductive S2−. Based on the above findings, a strategy for the colorimetric detection of Hg2+ and S2− by Se-AuNPs was established with linear ranges of 0.33–66 μg/L and 0.625–75 μg/L, and low detection limits of 0.17 μg/L and 0.12 μg/L (3.3 δ/k), respectively. When the colorimetric probes for detection of Hg2+ and S2− was applied in environmental water samples, the recoveries were in the range of 90.3–108.0 %. This method will provide a new idea for the colorimetric detection strategy of Hg2+ due to the strong interaction between Hg and Se.

Glutathione-Coated Gold Nanoparticles Enabling Bifunctional Therapy at the Buried Interface for Efficient and UV-Resistant Perovskite Solar Cells.

Very recently, the poor contact between the perovskite and carrier selective layer has been regarded as a critical issue for improving the performance and stability of perovskite solar cells (PSCs). In this study, the buried interface of regularly structured PSCs has been targeted. Glutathione-coated gold nanoparticles (GSH-AuNPs) are used as double-sided passivating agents to improve the quality of the perovskite films. It has been demonstrated that the GSH-AuNPs interact strongly with the SnO2 underlayer and the upper perovskite layer, significantly reducing the defect densities of this interface. Thus, the power conversion efficiency (PCE) of the PSCs can be increased from 20.46% (control, 19.38%, IPCE corrected) to 22.22% (GSH-AuNPs modified, 21.10%, IPCE corrected) with notable enhancement in Voc and FF. Moreover, the strong interaction between the C═O groups of GSH-AuNPs and the undercoordinated Pb2+ species of the perovskite films inhibits the formation of metallic Pb0. As a result, the unencapsulated GSH-AuNPs-modified devices retained 80% of their initial PCEs after 1000 h at ambient conditions, with a relative humidity (RH) of 60 ± 5%. UV-resistant PSCs have also been demonstrated after introducing GSH-AuNPs. Therefore, our findings demonstrate the bidirectional therapy strategy as a feasible approach for achieving efficient and UV-resistant PSCs.

From the standard model to M-theory: The development of string theory

String theory is now the most competitive theory of quantum gravity, and it takes an important role in theoretical physics. In this article, we introduced why we need string theory and how string theory is formed. The importance of string theory is described through general relativity and the Standard Model of particle physics. String theory is originally discovered to describe strong interaction. While a better model for strong interaction was developed, string theory was found to be a candidate for a theory about quantum gravity. The first version of string theory is the bosonic string theory, which was constructed in 26-dimensional space and used to describe bosons. After supersymmetry was introduced, the dimensions were reduced to 10, and the theory is hence called the superstring theory. In the first superstring revolution, 5 different superstring theories were constructed and compactified on the 6-dimensional Calabi-Yau manifold. In the second superstring revolution, the idea of different dualities was introduced in string, as well as D-branes. Hence, it was found that the 5 different superstrings can be unified to get the 11-dimensional M-theory.

Study of charged particle multiplicity with centrality in Au+Au collisions at SNN = 200 GeV

We have carried out methods of study to find the correlation between charged particle multiplicity and collision centrality of Au+Au collisions at SNN = 200 GeV. We have studied the open data from the ALICE experiment and arrived at the conclusion that central collisions produced a greater number of charged particles than peripheral collisions. This is done by reconstructing the three silicon layers inside the inner tracking system of the detector and studying the change in two spatial variables between layers: pseudorapidity with range || < 1 and azimuthal angle with acceptance , which can then be input into the sideband method to find the final multiplicity of each event. The study provides an insight into the transient nature of the Quark Gluon Plasma (QGP) produced in collisions by exploring how collision aftermaths vary with different conditions of the partons, which hopefully adds to the understanding of matter under the strong force at extreme energy density.

Mechanism of the Terahertz Wave-MXene Interaction and Surface/Interface Chemistry of MXene for Terahertz Absorption and Shielding.

ConspectusOver the past two decades, terahertz (THz) technology has undergone rapid development, driven by advancements and the growing demand for THz applications across various scientific and technological domains. As the cornerstone of THz technology, strong THz-matter interactions, especially realized as high THz intrinsic absorption in nanometer-thick materials, play a highly important role in various applications including but not limited to THz absorption/shielding, detection, etc. The rigorous electromagnetic theory has posited a maximum intrinsic absorption of 50% for electromagnetic waves by thin films, and the succinct impedance matching condition has also been formulated to guide the design of highly intrinsically absorbing materials. However, these theories face challenges when applied to the THz spectrum with an ultrabroad bandwidth. Existing thin films typically achieve a maximum intrinsic absorption within a narrow frequency range, significantly limiting the performance of THz absorbers and detectors. To date, both theoretical frameworks and experimental solutions are lacking in overcoming the challenge of achieving broadband maximum intrinsic absorption in the THz regime.In this Account, we describe how two-dimensional (2D) transition-metal carbide and/or nitride (MXene) films with nanometer thickness can realize the maximum intrinsic absorption in the ultrabroad THz band, which successfully addresses the forementioned longstanding issue. Surprisingly, traditional DC impedance matching theory fails to explain this phenomenon, while we instead propose a novel theory of AC impedance matching to provide a satisfactory explanation. By delving into the microscopic transport behavior of free electrons in MXene, we discover that intraflake transport dominates terahertz conductivity under THz wave excitation, while interflake transport primarily dictates DC conductivity. This not only elucidates the significant disparities between DC and AC impedance in MXenes but also underscores the suitability of AC impedance matching for achieving broadband THz absorption limits. Furthermore, we identify a high electron concentration and short relaxation time as crucial factors for achieving broadband maximum absorption in the THz regime. Although approaching the THz intrinsic absorbing limits, it still faces hurdles to the use of MXene in practical applications. First, diverse and uncontrollable terminations exist on the surface of MXene stemming from the synthesis process, which largely influence the electron structure and THz absorbing property of MXene. Second, MXene suffers from poor stability in the presence of oxygen and water. To address the above issues, we have undertaken distinctive works to precisely control the terminations and suppress the oxidation of MXene even at high temperature through surface and interface chemistry, such as low-temperature Lewis basic halide treatment and building a Ti3C2Tx/extracted bentonite (EB) interface. For practical application consideration, we proposed a copolymer-polyacrylic latex (PAL)-based MXene waterborne paint (MWP) with a strong intermolecular polar interaction between MWP and the substrate provided by the cyano group in PAL. This not only has strong THz EMI shielding/absorption efficiency but also can easily adhere to various substrates that are commonly used in the THz band. These studies may have significant implications for future applications of MXene nanofilms in THz optoelectronic devices.

The impact of high rainfall events on the submesoscale salinity field in a coastal sea: Greater Cook Strait, New Zealand

ABSTRACT River inflow into the coastal oceanic environment can result in low salinity submesoscale features (LSMFs). The enhanced water column stability sustained within these coherent structures affects local biological productivity. With-event and seasonal variability of LSMFs were investigated in a coastal sea -- Greater Cook Strait -- that is characterised by strong tidal and wind forcing as well as being forced at the land-sea boundary by several major rivers. A combination of ocean glider and satellite observations revealed the existence of seasonal variability in temperature, chlorophyll and stratification in LSMFs. High rainfall from ex-cyclone enhanced production of LSMFs in seasons when they would otherwise be less frequent. Stronger stratification was observed at the end of spring, in summer and at the beginning of autumn both in ambient shelf conditions and within LSMFs. Subsurface chlorophyll-a maxima were found associated with summer and spring LSMFs, when temperature had a stronger contribution to vertical stratification. In the available samples, LSMFs were advected seawards when river discharges exceeded 600 m 3 s − 1 . When river flows were lower than this threshold, other drivers such as wind or currents were required to advect the observed LSMFs offshore.

Mullite Mineral-Derived Robust Solid Electrolyte Enables Polyiodide Shuttle-Free Zinc-Iodine Batteries.

Zinc dendrite, active iodine dissolution, and polyiodide shuttle caused by the strong interaction between liquid electrolyte and solid electrode are the chief culprits for the capacity attenuation of aqueous zinc-iodine batteries (ZIBs). Herein, mullite is adopted as raw material to prepare Zn-based solid-state electrolyte (Zn-ML) for ZIBs through zinc ion exchange strategy. Owing to the merits of low electronic conductivity, low zinc diffusion energy barrier, and strong polyiodide adsorption capability, Zn-ML electrolyte can effectively isolate the redox reactions of zinc anode and AC@I2 cathode, guide the reversible zinc deposition behavior, and inhibit the active iodine dissolution as well as polyiodide shuttle during cycling process. As expected, wide operating voltage window of 2.7V (vs Zn2+/Zn), high Zn2+ transference number of 0.51, and low activation energy barrier of 29.7kJ mol-1 can be achieved for the solid-state Zn//Zn cells. Meanwhile, high reversible capacity of 127.4 and 107.6 mAh g-1 can be maintained at 0.5 and 1 A g-1 after 3000 and 2100 cycles for the solid-state Zn//AC@I2 batteries, corresponding to high-capacity retention ratio of 85.2% and 80.7%, respectively. This study will inspire the development of mineral-derived solid electrolyte, and facilitate its application in Zn-based secondary batteries.

Educational Environment Management in the Perspective of Climate Change in Indonesia

Education has been managed in such a way that the maximum educational goals can be achieved. In its implementation, education is certainly inseparable from management and its surrounding environment. In management, the presence of the right strategy and a solid team is needed so that the goals can be achieved. Meanwhile, the strategy in management itself only reacts to the human-shaped environment, which is society. Both management and the school environment have strong interactions and influences on the education management process. Educational institutions' management must ensure that their methods are in line with societal demands, as social and cultural institutions have a significant impact on how the institution operates. The educational environment should be managed in such a way that the educational goals can be achieved. With good interaction and support from the community and parties related to the educational environment, it is hoped that schools will advance. In other words, good cooperation from lecturers, parents, education boards, committees, and the community around the school environment is believed to be able to develop potential and improve the quality of education.

Investigation on Heterostructured SeO2–TiO2 Nanofluoroprobe for Highly Selective and Sensitive Detection of a Neonicotinoid Insecticide, Imidacloprid in Soil and Water Matrixes

Heterostructured SeO2–TiO2 nanoparticles were used as a highly sensitive and selective fluoroprobe for the detection and determination of neonicotinoid insecticide imidacloprid. The sonication-assisted co-precipitation technique was used to create nanoparticles, which were then characterized using UV–Vis, SEM–EDS, HRTEM, XRD, and TGA. These analyses revealed that the nanoparticles had globular morphology, a crystallite size of 14 nm, a bandgap of 2.45 eV, and stability at high temperatures. Fluorescence emission at 548 nm wavelength exhibits high sensitivity and selectivity for imidacloprid over other pesticides with complete fluorescent quenching at 2 × 10–4 M concentration of imidacloprid. Stern–Volmer equation and thermodynamic parameters applied to the experimental data over a temperature range of 20–50 °C provide the Ksv value in the range of 1.56 × 105 to 2.69 × 105 M−1 and indicate strong interactions, dynamic, spontaneous, and endothermic quenching process. Furthermore, the excellent salient features and notably the unaffected performance even in the presence of various anions, fertilizer, and binary mixture of pesticides often sprayed on plants, will pave the way for the development of rapid, affordable, selective fluoroprobe for onsite monitoring of imidacloprid. The reliability for determination is also examined for spiked soil samples to develop a hybrid SeO2–TiO2 nanoparticles fluoroprobe as a simple alternative to existing techniques for the detection of imidacloprid.Graphical

Unbounding the Future: Designing NiAl-Based Catalysts for Dry Reforming of Methane.

Dry reforming of methane (DRM), the catalytic conversion of CH4 and CO2 into syngas (H2+CO), is an important process closely correlated to the environment and chemical industry. NiAl-based catalysts have been reported to exhibit excellent activity, low cost, and environmental friendliness. At the same time, the rapid deactivation caused by carbon deposition, Ni sintering, and phase transformation exerts great challenges for its large-scale applications. This review summarizes the recent advances in NiAl-based catalysts for DRM, particularly focusing on the strategies to construct efficient and stable NiAl-based catalysts. Firstly, the thermodynamics and elementary steps of DRM, including the activation of reactants and coke formation and elimination, are summarized. The roles of Al2O3 and its mixed oxides as the support, and the influences of the promoters employed in NiAl-based catalysts over the DRM performance, are then illustrated. Finally, the design of anti-coking and anti-sintering NiAl-based catalysts for DRM is suggested as feasible and promising by tailoring the structure and states of Ni and the modification of Al-based supports including small Ni size, high Ni dispersion, proper basicity, strong metal-support interaction (SMSI), active oxygen species as well as high phase stability.

Heavy-Metal Ions Removal and Iodine Capture by Terpyridine Covalent Organic Frameworks.

Porous materials are excellent candidates for water remediation in environmental issues. However, it is still a key challenge to design efficient adsorbents for rapid water purification from various heavy metal ions-contaminated wastewater in one step. Here, two robust nitrogen-rich covalent organic frameworks (COFs) bearing terpyridine units on the pore walls by a "bottom-up" strategy are reported. Benefitting from the strong chelation interaction between the terpyridine units and various heavy metal ions, these two terpyridine COFs show excellent removal efficiency and capability for Pb2+, Hg2+, Cu2+, Ag+, Cd2+, Ni2+, and Cr3+ from water. These COFs are shown to remove such heavy metal ions with >90% of contents at one time after the aqueous metal ions mixture is passed through the COF filter. The nitrogen-rich features of the COFs also endow them with the capability of capturing iodine vapors, offering the terpyridine COFs the potential for environmental remediation applications.

Wide-Dynamic-Range Control of Quantum-Electrodynamic Electron Transfer Reactions in the Weak Coupling Regime.

Catalyzing reactions effectively by vacuum fluctuations of electromagnetic fields is a significant challenge within the realm of chemistry. As opposed to most studies based on vibrational strong coupling, we introduce an innovative catalytic mechanism driven by weakly coupled polaritonic fields. Through the amalgamation of macroscopic quantum electrodynamics (QED) principles with Marcus electron transfer (ET) theory, we predict that ET reaction rates can be precisely modulated across a wide dynamic range by controlling the size and structure of nanocavities. Compared to QED-driven radiative ET rates in free space, plasmonic cavities induce substantial rate enhancements spanning the range from 103- to 10-fold. By contrast, Fabry-Perot cavities engender rate suppression spanning the range from 10-2- to 10-1-fold. This work overcomes the necessity of using strong light-matter interactions in QED chemistry, opening up a new era of manipulating QED-based chemical reactions in a wide dynamic range.

Albumin as a functional carrier solubilizing and facilitating fusidic acid transmembrane delivery into Gram-negative bacteria

Reversing the bacterial resistance is of great significance and importance. Fusidic acid (FA) is commonly effective against Gram-positive bacterial infections, but most Gram-negative bacteria have intrinsic resistance to FA, primarily due to the strong cell membrane-FA interactions, which highly inhibit the intracellular transport of FA. Herein, we use albumin (bovine serum albumin, BSA) as a bifunctional carrier to solubilize FA and facilitate its transmembrane delivery into Gram-negative bacterial cells. The water solubility of FA is significantly enhanced from 11.87 to 442.20 μg/mL by 5 mg/mL BSA after forming FA-BSA complex. Furthermore, FA-BSA (200 μg/mL) causes 99.96 % viability loss to the model pathogen E. coli upon incubation for 3 h, while free FA or BSA alone shows little activity. Elongation of E. coli cells after treated by FA-BSA is demonstrated by SEM, and the transmembrane transport of FA-BSA is demonstrated by CLSM. Interestingly, increasing the BSA amount substantially reduce the antibacterial activity of FA-BSA, implying an albumin-based transmembrane delivery mechanism may exist. This is the first report regarding successfully reversing the intrinsic resistance of Gram-negative bacteria to FA in the form of FA-BSA. The ready availability of albumin and the simple preparation allows FA-BSA to have great potentials for clinical use.

Using In-situ Transmission Electron Microscopy to Study Strong Metal-Support Interactions in Heterogeneous Catalysis.

Precisely controlling the microstructure of supported metal catalysts and regulating metal-support interactions at the atomic level are essential for achieving highly efficient heterogeneous catalysts. Strong metal-support interaction (SMSI) not only stabilizes metal nanoparticles and improves their resistance to sintering but also modulates the electrical interaction between metal species and the support, optimizing the catalytic activity and selectivity. Therefore, understating the formation mechanism of SMSI and its dynamic evolution during the chemical reaction at the atomic scale is crucial for guiding the structural design and performance optimization of supported metal catalysts. Recent advancements in in-situ transmission electron microscopy (TEM) have shed new light on these complex phenomena, providing deeper insights into the SMSI dynamics. Here, the research progress of in-situ TEM investigation on SMSI in heterogeneous catalysis is systematically reviewed, focusing on the formation dynamics, structural evolution during the catalytic reactions, and regulation methods of SMSI. The significant advantages of in-situ TEM technologies for SMSI research are also highlighted. Moreover, the challenges and probable development paths of in-situ TEM studies on the SMSI are also provided.

Natural flavonoids as promising lactate dehydrogenase A inhibitors: Comprehensive in vitro and in silico analysis.

The inhibitory potential of 17 flavonoids on lactate dehydrogenase A (LDHA), a key enzyme in the downstream process of aerobic glycolysis in cancer cells, is investigated. Fisetin exhibited excellent inhibitory activity (IC50 = 0.066 µM). Quercetin 3-β-D-glucoside, quercetin 3-galactoside, luteolin, neoeriocitrin, and luteolin 7-O-β-D-glucoside showed good inhibitory activity (IC50 = 1.397-15.730 µM). Biochanin A, baicalein, quercetin, scutellarein-7-glucuronide, diosmetin, baicalein 7-O-β-D-glucuronide, and apigenin 7-apioglucoside demonstrated moderate inhibitory activity (IC50 = 33.007-86.643 µM). Eriodictyol, quercetin 7-O-β-D-glucoside, apigenin 7-O-β-D-glucoside, and epicatechin were inactive. The Lineweaver-Burk plot showed that fisetin competitively inhibits NADH binding (Ki = 0.024 µM). Ki values for other compounds were calculated using the Cheng-Prusoff equation (Ki = 0.2799-2.1661 µM). The study revealed that the inhibitory effect of flavonoids varies with the number and position of OH groups and bound sugars. Molecular docking analyses indicated that flavonoids exhibited strong interactions with the NADH binding site of LDHA through hydrophobic interactions and hydrogen bonds. Molecular dynamic simulations tested the stability of the fisetin-LDHA complex over 100 ns and showed fisetin's high binding affinity to LDHA, maintaining strong hydrogen bonds. The binding energy of fisetin with LDHA was -33.928 kcal/mol, indicating its effectiveness as an LDHA inhibitor. Consequently, flavonoids identified as strong inhibitors could be potential cancer treatment sources through LDHA inhibition.

Discovery of Novel Acethydrazide-Containing Flavonol Derivatives as Potential Antifungal Agents.

In this study, a series of novel hydrazide-containing flavonol derivatives was designed, synthesized, and evaluated for antifungal activity. In the in vitro antifungal assay, most of the target compounds exhibited potent antifungal activity against seven tested phytopathogenic fungi. In particular, compound C32 showed the best antifungal activity against Rhizoctonia solani (EC50 = 0.170 μg/mL), outperforming carbendazim (EC50 = 0.360 μg/mL) and boscalid (EC50 = 1.36 μg/mL). Compound C24 exhibited excellent antifungal activity against Valsa mali, Botrytis cinerea, and Alternaria alternata with EC50 values of 0.590, 0.870, and 1.71 μg/mL, respectively. The in vivo experiments revealed that compounds C32 and C24 were potential novel agricultural antifungals. 3D quantitative structure-activity relationship (3D-QSAR) models were used to analyze the structure-activity relationships of these compounds. The analysis results indicated that introducing appropriate electronegative groups at position 4 of a benzene ring could effectively improve the anti-R. solani activity. In the antifungal mechanism study, scanning electron microscopy and transmission electron microscopy analyses revealed that C32 disrupted the normal growth of hyphae by affecting the structural integrity of the cell membrane and cellular respiration. Furthermore, compound C32 exhibited potent succinate dehydrogenase (SDH) inhibitory activity (IC50 = 8.42 μM), surpassing that of the SDH fungicide boscalid (IC50 = 15.6 μM). The molecular dynamics simulations and docking experiments suggested that compound C32 can occupy the active site and form strong interactions with the key residues of SDH. Our findings have great potential for aiding future research on plant disease control in agriculture.

Novel shish-kebab structured nanofibrous decorating chitosan unidirectional scaffolds to mimic extracellular matrix for tissue engineering

Electrospun nanofibrous scaffolds are renowned for their ability to mimic the microstructure of the extracellular matrix (ECM). However, they often fail to replicate the geometry of target tissues, and the biocompatibility of these scaffolds those made from synthetic polymers is always limited due to the lack of cell binding sites. To address these issues, we proposed an innovative approach that combined unidirectional freeze-drying and electrospinning. During this process, electrospun polycaprolactone (PCL) nanofibers were chopped into nanofibrils, which range in size up to several hundred micrometers, and were incorporated into the chitosan scaffolds via unidirectional freeze-drying. In these scaffolds, the chitosan phase was responsible for maintaining the structural integrity at the macroscale, while the embedded nanofibers enhanced the surface topography at the microscale. The resulting scaffolds exhibited a high porosity of 90% and an impressive water uptake capacity of 2500%. Furthermore, 3T3 fibroblast cells showed strong interactions with the scaffolds, characterized by high rates of cell proliferation and viability. The cells also displayed significant orientation along the direction of the pores, suggesting that the scaffolds effectively guided cellular growth.

Oxygen Vacancy Engineering in ZnO/ZrO2 Composite Catalysts for Highly Enhanced Hydrogen Production by Methanol Steam Reforming

The ZnO/ZrO2 binary catalyst system has been an emerging and promising catalyst for efficient production of H2 through methanol steam reforming (MSR). Herein, ZrO2 supports with different crystalline phases were prepared by the oxygen vacancy engineering strategy of Li doping, and then ZnO/ZrO2 catalysts were prepared by the isovolumic impregnation method. The different quantities of doped Li have been found to have a significant impact on dominant crystal phase of ZrO2 supports, which dictates the interaction between ZnO and ZrO2 and the number of oxygen vacancies. In comparison with ZnO/ZrO2-20Li and ZnO/ZrO2-40Li catalysts with predominate tetragonal and monoclinic crystal phase, ZnO/ZrO2-3Li with a mixed crystalline phase exhibits higher catalytic activity for methanol conversion (XCH3OH) and CO selectivity (SCO). Complete methanol conversion of the best performing ZnO/ZrO2-3Li catalyst was observed at a very low CO selectivity of 3.1% at 375 ℃. The XRD, UV, and XPS characterization results indicate that the strong interaction between ZrO2 and ZnO leads to the appearance of large amount of oxygen vacancies at the ZnO/ZrO2 interface, which greatly improves the performance of the catalyst. ZnO/ZrO2 catalyst showed remarkable stability without obvious deactivation after 32hours of continuous testing. This work highlights the effectiveness of oxygen vacancy engineering of the ZnO/ZrO2 catalysts for applications in methanol steam reforming and other heterogeneous catalytic systems.

Are NaTFSI and NaFSI Salt-Based Water-in-Salt Electrolytes Structurally Similar or Different?

Water-in-salt electrolytes (WiSEs) are a promising class of electrolytes due to their wide electrochemical stability window and nonflammability. In this study, we explore the structural organization of sodium bis(trifluoromethylsulfonyl)imide (NaTFSI) and sodium bis(fluorosulfonyl)imide (NaFSI) salt-based aqueous electrolytes, covering dilute to highly concentrated regions, by employing an all-atom molecular dynamics simulation. For the NaTFSI-based electrolyte, we observe that Na+ ions are mostly surrounded by water molecules at all the salt concentrations due to the very strong interaction between them. While TFSI anions weakly coordinate with Na+ ions and other TFSI anions, they also mostly prefer to be surrounded by water molecules. These interactions were found to have moderate dependence on the concentration of the NaTFSI salt. For the NaFSI-based electrolyte, while the Na+-water interaction is stronger at lower salt concentrations, the number of nearest neighbor FSI anions is found to be more than that of water at higher concentrations (≥20 m). This is because the increase in the salt concentration leads to expulsion of water molecules from the solvation shell of Na+ ions and enhances the interaction between Na+ ions and oxygen atoms of FSI. At the highest salt concentration (solubility limit), the bulk-like water structure is completely disrupted and dominated by an anionic network in the FSI-based electrolyte. In contrast, water-water hydrogen bonding network is still present even in the highly concentrated TFSI-based electrolyte. The simulated X-ray scattering pattern displays a low-q peak, revealing the presence of an intermediate range ordering due to alternating anion-rich and water/Na+-rich regions in both the electrolytes. However, the characteristic length scale corresponding to the low-q peak decreases with increasing the salt content in both the electrolytes.