Strong Interaction Research Articles

Synergistic Role of Indium Doping and g-C3N4 Reinforcement in Boosting the Visible Light-Triggered Rhodamine B and Diclofenac Sodium Salt Degradation over Rare Earth Molybdate

Designing and fabricating cost-efficient and eco-friendly photocatalysts for removing organic pollutants from wastewater streams is a crucial research objective for effectively managing industrial effluents to tackle environmental sustainability issues. In this study, we prepared bare cerium molybdate (Ce2(MoO4)3, M1) and indium-doped cerium molybdate (In- Ce2(MoO4)3, M2) photocatalysts via a hydrothermal method. We then synthesized a nanocomposite of In- Ce2(MoO4)3 (M3) with the promising material graphitic carbon nitride (g-C3N4) using an ultrasonication approach. The synthesized photocatalysts were effectively applied to degrade the Rhodamine B dye and diclofenac sodium salt (a drug) from synthetic industrial wastewater through a photocatalysis approach. The impact of indium (In3+) doping on the bare (Ce2(MoO4)3 and the strong interaction between the (In-Ce2(MoO4)3 and g-C3N4 nanosheets were analyzed through physical and electrochemical techniques, including SEM, EDS, XRD, FTIR, UV-Vis spectroscopy, and EIS analysis. The comprehensive photocatalytic degradation of dye and the drug via first-order kinetic parameters under visible light irradiation for all the prepared catalyst samples was evaluated. The nanocomposite In-Ce2(MoO4)3/g-C3N4 exhibited excellent photocatalytic activity, degrading the maximum amount of RhB dye and drug (RhB:96%, drug:87%) in 90 minutes with a higher rate constant (k) compared to In-Ce2(MoO4)3 (RhB:69%, drug:56%) and Ce2(MoO4)3 (RhB:56%, drug:38%). Furthermore, the In-Ce2(MoO4)3/g-C3N4 samples produced a 7-fold and 3-fold increase in transient photogenerated current response compared to pristine Ce2(MoO4)3 and In-Ce2(MoO4)3 samples, respectively. These findings pave the way for synthesizing an economical, versatile, and efficient In-Ce2(MoO4)3/g-C3N4 photocatalyst to eliminate pollutants from industrial wastewater streams and boost environmental sustainability.

A systematic study on Au-PDA@Fe3O4 core-shell catalysts for enhanced catalytic reduction of 4-nitrophenol

The development of nanogold catalysts with high activity and high stability is of great significance for their industrial applications. In this paper, Au-PDA@Fe3O4 catalysts were prepared through the gold sol adsorption method. First, micron-sized magnetic Fe3O4 spheres were synthesized via a solvothermal method, serving as the core to endow the catalyst with excellent recyclability. Subsequently, a layer of polydopamine (PDA) shell was polymerized on the magnetic core surface. By controlling the timing of introducing the gold sol containing Au nanoparticles (NPs), the spatial position of Au NPs within the PDA layer was regulated, leading to a series of magnetic core-shell nano gold catalysts with varying spatial positions of Au. Using the 4-nitrophenol (4-NP) hydrogenation as the probe, the influence of Au spatial position, Au size, and other conditions on the catalytic performance was investigated. Results showed that, in the prepared Au-PDA@Fe3O4-16 catalyst, the Au NPs are encapsulated within the PDA shell and positioned close to the outer layer. This not only provides remarkable stability to the Au NPs but also maintains their proximity to the surface of the PDA shell, allowing easier access of the substrate 4-NP to the Au NPs and conferring good reactivity upon the catalyst. The strong electron metal-support interaction between PDA and Au enables PDA to effectively stabilize Au NPs. The prepared Au-PDA@Fe3O4-16 catalyst exhibits excellent stability, maintaining a high conversion rate of 91% even after 14 cycles of use. Our findings not only deepen the understanding of the catalytic mechanisms involved but also pave the path towards the creation of highly efficient and robust gold-based catalysts, facilitating their widespread utilization in industrial applications.

Overexpression of miRNA29a gene inhibits proliferation and promotes apoptosis of jejunal epithelial cells in yak.

MicroRNAs (miRNAs) were identified to be involved in various biological functions by regulating the degradation or suppressing the translation of their downstream target genes. Recent studies have identified miR-29a play a key role in functions of mammal cell differentiation, proliferation, apoptosis, and signal transduction. However, the underlying functions for miR-29a in jejunal epithelial cells biological function still to be investigated. In order to explore the yak jejunal epithelial cells proliferation and barrier dysfunction with over expression of miR-29a gene, three 0-day-old Pamir male yaks were randomly selected and slaughtered in present study, and the jejunal epithelial cells were isolated and cultured to determine yak jejunal epithelial cells proliferation and protein composition on differential expression of miR-29a gene in Pamir plateau. Here, we demonstrated that the overexpression of miR-29a gene could inhibit the proliferation of Pamir yaks jejunum epithelial cells, and contribute to the apoptosis of Pamir yaks jejunal epithelial cells with some extent. A total of 133 differentially expressed proteins were identified in different expression of miR-29a groups by label-free Mass Spectrometry (MS), which could be concluded to two predominant themes: cell proliferation and inflammatory response. Interestingly, GPR41, as a bridge protein, was contacted two predominant themes to involved in Pamir Yaks jejunal mechanical barrier PPI network, and the target proteins displayed strong mutual interactions in the complex PPI network. Overall, our study suggested that the over-expression miR-29a inhibited the jejunal epithelial cells proliferation and the expressions of specific proteins, which damaged jejunal barrier function to slow down the intestine structure and function advanced mature development during young livestock period for influence the enhanced performance of production efficiency.

Highly efficient Ru/CeO2 catalyst using colloidal chemical method for propane oxidation

Although supported-Ru catalysts have been widely studied for the light alkane oxidation root in their lower cost compared to Pt and Pd, developing Ru-based catalysts with high efficiency for low-temperature light alkane elimination remains a significant challenge. Herein, Ru/CeO2 catalysts were prepared utilizing the colloidal synthesis (Ru/CeO2-CS) and compared with the catalyst prepared with the traditional impregnation method (Ru/CeO2-IM) in the textural properties and catalytic propane oxidation. It was discovered that Ru/CeO2-CS sample contained a higher concentration of active Ru − O − Ce interface and oxygen vacancies attributed to the strong Ru-CeO2 interaction, which further enhanced the redox capacity. Besides, the lower valence state of Ru species and higher contents of Lewis acid sites on Ru/CeO2-CS sample boosted the adsorption, dissociation, and activation of propane, thus promoting the deep oxidation of propane to CO2 and H2O. The reaction mechanism of propane oxidation was revealed by in-situ DRIFTS, and both the catalysts showed bands related to acrylate species, suggesting that propane underwent an acrylate oxidation pathway on Ru/CeO2-CS and Ru/CeO2-IM samples. The distinct textural properties of these catalysts resulted in Ru/CeO2-CS synthesized by colloidal methods showing a T90 of 170 °C, and Ea of 50.9 ± 1.8 kJ·mol−1, markedly lower than Ru/CeO2-IM prepared with the traditional impregnation method. Apart from the activity, the Ru/CeO2-CS sample obtained superior water resistance, thermal stability, and durability. This comprehensive work provides promising insights into low-temperature propane oxidation.

An experimental study of a rectangular floating breakwater with flexible curtains as wave-dissipating components

In this study, the flexible curtains are attached to the bottom of a rectangular floating breakwater as wave-dissipating components. Through a comprehensive experimental investigation, the wave attenuation, motion responses, and mooring forces of the proposed floating breakwater are examined, with a particular focus on the effects of wave height and the hanging length and porosity of the flexible curtain. Meanwhile, comparative analyses are conducted with the stand-alone rectangular floating breakwater and with attaching one rigid slotted barrier. Our experimental results indicate that one underhanging flexible curtain can augment wave attenuation across all tested wave conditions, which is comparable to the rigid slotted barrier. Furthermore, attaching two flexible curtains contributes to a more significant enhancement for harbor or coastal protection, especially against long waves. This can be attributed to the buffer function of flexible curtains, and the increased added mass induced by the water body confined between them, which increases the natural period of floating breakwaters. Furthermore, the attachment of the flexible curtains significantly suppresses the motion responses of the breakwater, which can alleviate the undesirable strong mooring forces. In general, increasing the length or decreasing the porosity of flexible curtains leads to similar trends in the performance of floating breakwaters. The flexible curtains have been proven to be effective wave-dissipating components for rectangular floating breakwaters.

Exploring the Therapeutic Potential of Ginkgo biloba Polyphenols in Targeting Biomarkers of Colorectal Cancer: An In-silico Evaluation.

Colorectal cancer (CRC) is a major contributor to cancer-related deaths worldwide, driving the need for effective anticancer therapies with fewer side effects. The exploration of Ginkgo biloba, a natural source, offers a hopeful avenue for novel treatments targeting key colorectal biomarkers involved in CRC treatment. The aim of this study was to explore the binding affinity of natural molecules derived from G. biloba to essential biomarkers associated with CRC, including Kirsten rat sarcoma virus, neuroblastoma RAS mutations, serine/threonine-protein kinase B-Raf, phosphatidylinositol 3'-kinase, and deleted colorectal cancer, using molecular docking. The focus of this research was to evaluate how effectively these molecules bind to specified targets in order to identify potential inhibitors for the treatment of CRC. A total of 152 polyphenolic compounds from G. biloba were selected and subjected to molecular docking simulations to evaluate their interactions with CRC-related biomarkers. The docking results were analysed to identify ligands exhibiting strong affinities towards the targeted genes, suggesting potential inhibitory effects. Docking simulations unveiled the strong binding affinities between selected polyphenolic compounds derived from G. biloba and genes associated with CRC. The complex glycoside structures that are found in flavonols are of significant importance. These compounds, including derivatives with distinctive arrangements, exhibited promising docking scores, signifying substantial interactions with the targeted biomarkers. The study demonstrates the potential of G. biloba-derived molecules as effective anticancer agents for colorectal cancer. The identified ligands exhibit strong interactions with crucial CRC-related biomarkers, suggesting potential inhibition ability. Further in vitro and in vivo investigations are needed to validate and build upon these promising findings, advancing the development of novel and efficient CRC therapies.

Strong Metal-Support Interaction between Pt and TiO2 over High-temperature CO2 Hydrogenation.

The catalytic activities and stability of oxide-supported metal catalysts are significantly affected by metal-support interactions (MSI) between oxidic supports and supported metals. The surface properties of the support, such as its phase and defects, are crucial in MSI, including both the strong metal-support interaction (SMSI) and electronic metal-support interaction (EMSI). In this study, modulation of SMSI was achieved on rutile-supported Pt nanoparticles (NP) over high-temperature CO2 hydrogenation. The encapsulation of Pt NP surfaces with TiO2-x overlayers is precisely controlled by the defects. It is found that oxygen vacancy defects significantly enhance the catalytic stability of Pt/rutile under high-temperature reverse water-gas shift (RWGS) reaction by inhibiting the occurrence of SMSI. Pt/rutile with oxygen vacancies achieves a 301 molCO×gM-1×h-1 space time yield and considerably catalytic stability (decreased by 8%) at 800 °C over 100 h time-on-stream. Density functional theory (DFT) calculations suggest that the adsorption capacity of Pt NP on the rutile overlayer can be reduced by increasing electron density. Experimental results combined with DFT calculations show that electron transfer from Pt NP to rutile is reduced by the oxygen vacancy defects on Pt/R, preserving the metallic nature of Pt species during CO2 hydrogenation, thereby preventing the formation of SMSI.

Designing Impact Resistance and Robustness into Slippery Lubricant Infused Porous Surfaces.

Slippery lubricant infused porous surfaces (SLIPS) have the potential to address daunting challenges such as undesirable surface fouling/biofouling, icing, etc. However, the depletion of lubricants hampers their practical utility. As a solution, here a rational strategy is introduced that operates synergistically in three parts. First, ultra-high capillary pressure is exploited from the reticular structure of metal-organic frameworks (MOFs) with sub-nanometer pores. Second, the need for geometric compatibility is demonstrated; the lubricant chain diameter must be smaller than the MOF pore to enable lubricant chain intercalation. Lastly, the MOF pore chemistry is tailored to achieve a strong intermolecular interaction for any given MOF/lubricant combination. The strategy is investigated through experiments and quantum/molecular simulations, which show that the approach helps lock the intercalated lubricant chains inside the MOF pores and forms a non-conventional supramolecular structure. The resulting SLIPS (including those with fluorine-free chemistry) not only show typical low wetting hysteresis, friction, and ice adhesion but are uniquely resistant to more stringent tests such as continuous dripping and sliding of water droplets (up to 50hrs), repeated impacts of high-speed water jets (liquid impact Weber number >4×104) and prevent bacterial biofilm formation even in dynamic flow conditions. The findings may widen the practical applications of SLIPS.

N-type and P-type series integrated hydrogel thermoelectric cells for low-grade heat harvesting

Low-grade heat is abundant and ubiquitous, but it is generally discarded due to the lack of cost-effective recovery technologies. Ion thermoelectric cells are an affordable and straightforward approach of converting low-grade heat into usable electricity for sustainable power. Despite their potential, ion thermoelectric cells face challenges such as limited Seebeck coefficient and required series integration. Here, we demonstrate that the N-type and P-type conversion of ion thermoelectric cells can be achieved through the phase transition of temperature-sensitive hydrogel containing the triiodide/iodide redox couple. Through the strong interaction between the hydrophobic region of the hydrogel and triiodide, the hydrophobic side selectively captures triiodide and the hydrophilic side repels triiodide, raising the concentration difference of triiodide and thereby increasing the Seebeck coefficient. Specifically, the Seebeck coefficient of the N-type ion thermoelectric cells is 7.7 mV K−1, and the Seebeck coefficient of P-type ion thermoelectric cells is −6.3 mV K−1 (ΔT = 15 K). By connecting 10 pairs of the N-type and P-type ion thermoelectric cells, we achieve a voltage of 1.8 V and an output power of 85 μW, surpassing the reported triiodide/iodide-based ion thermoelectric cells. Our work proposes a phase transition strategy for the N-P conversion of ion thermoelectric cells, and highlights the prospect of series integrated hydrogel ion thermoelectric cells for low-grade heat harvesting.

A Stable Layered Microporous MOF Assembled with Y-O Chains for Separation of MTO Products.

Benefiting from highly tunable pore environments, some metal-organic frameworks (MOFs) have recently shown promising prospects in the separation of methanol-to-olefin (MTO) products (mainly C3H6 and C2H4). However, the "trade-off" between gas storage capacity and selectivity always results in inefficient separation. In addition, poor stability of MOFs also limits practical separation applications. Herein, we have successfully assembled a layered Y-MOF (FJI-W9) with bent diisophthalate ligands (H4L), Y-O chains, and 2-fluorobenzoic acids. As expected, FJI-W9 not only exhibits good chemical stability but also shows significant potential for C3H6/C2H4 separation. For FJI-W9, the C3H6 uptake at 298 K and 10 kPa is 63 cm3/g, and the IAST selectivity of FJI-W9 for C3H6/C2H4 (V/V = 50/50) is calculated to be 20.5. To the best of our knowledge, both C3H6 uptake and selectivity of FJI-W9 surpass most porous materials. GCMC simulation indicates that the special supramolecular binding sites in FJI-W9 have much stronger interactions with C3H6 than C2H4 molecules. More importantly, practical breakthrough experiments demonstrate that FJI-W9 can effectively separate C3H6/C2H4 (50/50) mixtures, thus obtaining high-purity C2H4 and C3H6, respectively.

Rational Design of Ultrahigh-Loading Ir Single Atoms on Reconstructed Mn─NiOOH for Enhanced Catalytic Performance in Urea-Water Electrolysis.

Investigating advanced electrocatalysts is crucial for improving the efficacy of water splitting to generate environmentally friendly fuel. The discovery of highly effective electrocatalysts, capable of driving oxygen evolution reaction (OER) and urea oxidation reaction (UOR) in urea-alkaline environments, is pivotal for advancing large-scale hydrogen production. This study aims to introduce a new method that involves creating nanosheets of high-loading iridium single atoms embedded in a manganese-containing nickel oxyhydroxide matrix (Ir@Mn─NiOOH). These nanostructures are derived from self-supported hydrate pre-catalyst nanosheets grown on nickel foam and then activated through electrochemical etching pretreatment. The Ir@Mn─NiOOH nanoarchitecture displays outstanding electrocatalytic activity, having a low overpotential of just 258mV and a potential of 1.319V (at 10mAcm-2) for OER and UOR, respectively. Such extraordinary catalytic characteristics of Ir@Mn─NiOOH is mainly owing to the strong synthetic electronic interaction between Ir single atoms and Mn─NiOOH, which can change its electronic characteristics and boost electrochemical catalytic sites. This research presents a new way to produce exceptionally efficient catalysts by adding a synergistic effect to complex multi-electron processes.

Recent Advances in Engineering Fe-N-C Catalysts for Oxygen Electrocatalysis in Zn-Air Batteries.

Fe-N-C single-atom catalysts (SACs) have emerged as one of the most promising candidates for oxygen electrocatalysis due to their maximized atom utilization efficiency, high intrinsic activity, and strong metal-support interaction. Significant progress has been made in engineering Fe-N-C SACs for oxygen electrocatalysis in Zn-air batteries (ZABs). This review provides a comprehensive overview of the recent advancements in Fe-N-C SACs, with a special focus on effective engineering strategies, their performance in oxygen electrocatalysis, and their potential applications in ZABs. The review also discusses the key challenges and future directions in the development of Fe-N-C SACs for efficient and durable oxygen electrocatalysis in ZABs. This review aims to offer valuable insights into the current state of research in this field and to guide future efforts in the development of advanced oxygen electrocatalysts for ZABs.

Strong Antiferromagnetic Interactions in the Binuclear Cobalt(II) Complex with a Bridged Nitroxide Diradical

A binuclear cobalt–radical complex formed by the reaction of Co(hfac)2·2H2O (hfac = hexafluoroacetylacetonate) with the 2,2-bis(1-oxyl-3-oxide-4,4,5,5-tetramethylimidazolinyl) biradical (BR) has been synthesized. The complex {(hfac)CoII(BN)CoII(hfac)} crystallizes in the triclinic space group P1¯ : C34H28Co2F24N4O12, a = 11.1513(5) Å, b = 12.8362(7) Å, c = 18.2903(8) Å, α = 103.061(1)°, β = 100.898(2)°, γ = 102.250(1)°, Z = 2. The compound consists of two non-equivalent pseudo-octahedral CoII ions, each bearing two hfac ancillary ligands bridged by the tetradentate bis-nitroxide (BN). The temperature dependence of the magnetic susceptibility indicates a strong antiferromagnetic exchange between each of the Co2+ ions and the nitroxyl biradical, as well as between the spins within the bridging ligand, forming a spin-frustrated system. Micro-squid investigations, performed on a single crystal of {(hfac)CoII(BN)CoII(hfac)}, reveal a peculiarity of the M(H) graph at temperatures below 0.4 K displaying a step that is a result of ground and first excited levels mixing by the applied magnetic field due to a small energy gap between them, as inferred from ab initio calculation. The latter was also carried out for two models of mononuclear Co2+ complexes in order to obtain a set of initial parameters for fitting the experimental magnetic curves using the Phi program. Moreover, direct CAS(12,10)/def2-TZVP calculations of the magnetic dependences χT(T) and M(H) were performed, which satisfactorily reproduced the experimental ones.

Time-resolved counterpropagating edge transport in the topological insulating phase

We have investigated the time-resolved low-energy charge dynamics in counterpropagating edge channels formed in the quantum Hall regime of an electron-hole bilayer system in band-inverted InAs/InGaSb composite quantum wells. In the studied magnetic field range, the system remains in the topological phase where an equal number of counterpropagating electronlike and holelike edge channels exist in the bulk energy gap, analogous to the helical edge channels in a quantum spin Hall insulator. When the Fermi level was set in the conduction band, the injected charge pulses propagated unidirectionally as chiral edge magnetoplasmon (EMP) wave packets. In contrast, in the nonchiral regime with the Fermi level set in the band gap, the injected charge pulses propagated identically in both directions with significantly reduced velocity. In addition, as the channel length increased, we observed a sharp crossover from EMP transport to diffusive transport, manifested as pronounced waveform broadening and dissipation. Simulations using a distributed capacitance model including interchannel tunneling well reproduced the observed behavior in both chiral and nonchiral regimes, revealing that interchannel charge transfer between counterpropagating channels plays a crucial role. The slow EMP transport in the nonchiral regime and its crossover to diffusive transport are consequences of the strong interchannel interaction and interchannel tunneling, respectively. Our results will thus provide insights into charge dynamics and scattering mechanism in analogous one-dimensional systems, including a quantum spin Hall insulator with helical edge modes and its expected Tomonaga-Luttinger liquid behavior. Published by the American Physical Society 2024

Plasma protein profile associated with a family history of early-onset coronary heart disease

Abstract Introduction Although family history of coronary heart disease (CHD) is an established risk factor for subsequent CHD, its relation to the circulating proteome is unknown. Proteins linked to coronary atherosclerosis in subjects with a family history could uncover new pathophysiological mechanisms of heritable CHD. Purpose Firstly, we aimed to study the protein profile associated with a family history of early-onset CHD. Secondly, we aimed to identify proteins among which family history was an effect modifier for the association between each protein and coronary atherosclerosis. Methods Plasma levels of proteins were assessed with Olink panels CVD-II and -III in the population-based Swedish CArdioPulmonary bioImage Study (SCAPIS) cohort. The coronary segment involvement score (SIS) was assessed from computed tomography angiography. Subjects without known CHD were cross-referenced with national registers to identify records of myocardial infarction or coronary revascularization in any parent before 55 or 65 years of age in males and females, respectively. The associations between a family history of CHD and each protein were studied with linear regression adjusted for age, sex and study site, using a False Discovery Rate (FDR) of 5%. Associations were subsequently adjusted for cardiovascular risk factors. Similarly, associations between each protein and SIS were modelled linearly with an FDR of 5%. For significant proteins, the statistical interactions between each protein and family history for the association between proteins and SIS were studied. Results Of 4,251 subjects, 9.5% had a family history CHD. 43 proteins were significantly associated with family history, and when adjusted for risk factors 29 protein associations remained significant (p<0,05) [Figure 1]. The strongest associations were observed for cathepsin D, paraoxonase 3, interleukin-1 receptor antagonist protein and renin. 79 proteins were associated with SIS at FDR<5%, and family history was a significant effect modifier 18 for proteins [Figure 2]. The strongest modifying effects were observed for transferrin receptor protein 1 (β 0.64, 95% CI 0.25–1.04 for those with family history vs β -0.04, 95% CI -0.14–0.06 in those without, p for interaction=0.001), LDL-receptor (β 0.68, 95% CI 0.36–1.00 vs β 0.18, 95% CI 0.08–0.26) and tissue-type plasminogen activator (β 0.45, 95% CI 0.19–0.70 vs β 0.13, 95% CI 0.05–0.21). Conclusion We found that 43 proteins, with biological features of inflammation and vascular function, were associated with a family history of early-onset CHD. Most were also linked to the coronary atherosclerosis burden. Notably, 18 biomarkers, among them transferrin receptor protein 1, LDL-receptor and tissue-type plasminogen activator, exhibited strong statistical interactions with family history in the association with SIS, indicating that they are of particular importance for the genetic susceptibility and the pathophysiology of heritable CHD.

Cause and Characteristics of Changes in Mesoscale Convective Systems within a Convection-Permitting Regional Climate Model

Abstract Changes in the frequency and intensity of mesoscale convective systems (MCS) are assessed using convection-permitting regional climate model simulations. We present a novel classification method that relates MCSs to the magnitude of their large-scale forcing environments to better understand the changing nature of MCSs across different forcing environments in a possible future climate scenario. Overall, the annual frequency, intensity, and amount of precipitation associated with MCSs are projected to increase for broad portions of the eastern conterminous United States (CONUS). Furthermore, changes in the characteristics of MCSs show larger, longer-lived, and faster MCSs particularly over the Midwest and Southeast. Seasonal examination of this response reveals a robust intensification of March–May (MAM) MCSs. The higher frequency of MAM MCSs are found to occur in weakly forced synoptic environments. Increased rainfall amounts are explained by an intensification of MCSs due to changing thermodynamics and enhanced lower-tropospheric moisture transport into the central CONUS by the North Atlantic Subtropical High. Differences in mid-latitude storm tracks are favorable towards the enhanced development of MCSs associated with strong baroclinic forcing within the Midwest and Northern Plains, but are only realized in the presence of strong changes in lower-tropospheric moisture transport. Overall, these results suggest a shift in the behavior of MAM MCSs that more closely corresponds to the behavior of June–August (JJA) MCSs in the historical climate. The increased occurrence of MCSs in weakly forced environments, particularly in MAM, deserves further investigation.

Facile Fabrication of LaFeO 3 Supported Pd Nanoparticles as Highly Effective Heterogeneous Catalyst for Suzuki–Miyaura Coupling Reaction

Supported Pd catalysts have been widely studied due to their enormous potential as candidates for heterogeneous Suzuki–Miyaura coupling reactions. However, the sintering and low activity of active sites still remain challenges. A vesicle‐shaped LaFeO3‐supported Pd catalyst (I‐Pd/LaFeO3) was successfully fabricated using the impregnation method and tested for the Suzuki–Miyaura coupling reaction. Compared to P‐Pd/LaFeO3 prepared with photo‐deposition and Pd/Al2O3 prepared with impregnation, the I‐Pd/LaFeO3 catalyst exhibits significantly higher catalytic activity, stability, and reusability. The chemical composition and electron states of different Pd‐based catalysts were well studied based on various characterizations and the results indicated that the excellent performance of I‐Pd/LaFeO3 can be attributed to its unique nanostructure and the strong interactions between LaFeO3 and palladium nanoparticles. The impregnation method and the choice of the LaFeO3 support show a great influence on the electronic properties of Pd species, their reducibility, and, consequently, their reaction behavior. This unique LaFeO3 supported Pd catalyst provided an environmentally friendly heterogeneous method for the Suzuki–Miyaura coupling reaction.

Lattice Strain Regulated by Hetero/homo Atom Interface Merging on NiMo Nanocluster for High-performance Hydrogen Production.

Lattice strain engineering represents a cutting-edge approach capable of delivering enhanced performance across various applications. The lattice strain can affect the performance of electrochemical catalysts by changing the binding energy between the surface-active sites and intermediates. In this work, lattice strain is regulated through a homo/heterogeneous atomic interface merging. The strong lattice strain and electronic interactions between Ni and Mo facilitated the reaction kinetic of HER. The prepared NiMo/SSM exhibiting excellent HER catalytic performance with 70 mV overpotential at the current density of 10 mA cm-2 and long-term stability. The method of controlling lattice strain through hetero/homo atom interface merging provides a new strategy for designing high-performance alkaline HER electrocatalysts.

Chain-like Pentanuclear Complexes: Syntheses, Crystal Structures and Long-range Electronic Interactions of Cyanido-Bridged M2Ru3 (M = Fe, Ru).

In this work, we report the design and synthesis of two chain-like pentanuclear cyanido-bridged complexes trans-[Ru(bpy)2(μ-CN)2][cis-Ru(bpy)2(μ-NC)M(dppe)Cp*]2[PF6]4(M = Fe, 14+; M = Ru, 24+) and the electronic communication properties of their oxidized products 1m+ (m = 6, 7, 8) and 2n+ (n = 5, 6, 7, 8). The single-crystal X-ray diffraction analysisof 1m+ (m = 4, 6, 7) and 24+ show that 14+ and 24+ possess a Z-type array structure, 17+ is a U-type one, and 16+ exhibits both the types. The investigations indicate that both 1 and 2 show an extraordinarily strong electronic interaction between the two side Ru across the central NC-Ru-CN, leading to the formation of a fully delocalized cyanidometal Ru-Ru-Ru bridge for both three-electron oxidized states 17+ and 27+. Moreover, it should be noted that in 1 there exists no electronic interaction between the two terminal Fe ions. Upon substitution of Fe by Ru, however, 2 exhibits an electronic interaction between the two terminal metal ions across the trinuclear cyanidometal CN-Ru-NC-Ru-CN-Ru-NC bridge which is up to 20 Å.

Coupling CoIr Nanoalloys with MXene by Lewis Acidic Molten Salt Etching for Wide-pH-Environment Hydrogen Evolution Reaction.

Metal/MXene-based materials show broad prospects in energy conversation through the strong metal-support interaction (SMSI). However, the difficulty and harshness of synthesis heavily limit their further application. Herein, using Lewis acidic molten salt to etch MAX as a precursor of MXene, a more convenient and safer strategy is designed to in situ construct the MXene-supported CoIr nanoalloy (CoIr/MXene) catalyst through Ti─O─M bond. The special layered structure and oxygen-containing functional group of MXene regulate the SMSI upon CoIr nanoalloys. Moreover, the contact angle and in situ Raman test results exhibit good interface hydrophilicity of MXene, enhancing the water adsorption on interfaces, and accelerating the mass transfer process. As a result, CoIr/MXene shows high hydrogen evolution reaction (HER) performance, which only needs overpotentials of 34 and 50mV to drive a current density of 10mA cm-2 in alkaline and acidic media, respectively, with excellent stability. Especially, in alkaline media, CoIr/MXene possesses 6 times higher HER mass activity (4.297 A mgIr -1) than commercial Pt/C catalysts (0.686 A mgPt -1) at the potential of 50mV, indicating larger active site density and intrinsic activity for CoIr/MXene. This work expands the application of the molten salt assist etching strategy and provides new insight for the development of metal/MXene-based catalysts.