Exploring the spatial distribution of land use/coverage (LUCC) and ecosystem carbon reserves in the future of climate change can provide a scientific basis for optimizing the distribution of land resources and formulating social economic sustainable development policies. In this study, we integrated the plaques generating land use simulation (PLUS) model and ecosystem services and weighing comprehensive evaluation (InVEST) model. Based on the CMIP6-based sharing socio-economic path and representative concentration path (SSP-RCP), we evaluated the Loess Plateau for time and space dynamic changes in LUCC and ecosystem carbon reserves, analyzed the impact of driving factors on different regions, and explored the correlation between carbon reserves in various regions.
View Article and Find Full Text PDFStrong interaction between circularly polarized light and chiral plasmonic nanostructures can enable controllable asymmetric photophysical processes, such as selective chiral switching of a plasmonic nanorod-dimer. Here, we uncover the underlying physics that governs this chiral switching by theoretically investigating the interplay between asymmetric photothermal and optomechanical effects. We find that the photothermally induced local temperature rises could play a key role in activating the dynamic chiral configurations of a plasmonic dimer due to the temperature-sensitive molecular linkages located at the gap region.
View Article and Find Full Text PDFA series of FeMn bimetallic ferrocene-based metal-organic frameworks (FeMn-Fc-MOFs) with various molar ratios of Fe and Mn (1:9, 2:8, 4:6, 6:4) were successfully synthesized using a simple hydrothermal synthesis method and employed as an efficient activator on persulfate (PS) activation for water decontamination. Characterizations demonstrated that Fe and Mn were smoothly introduced into ferrocene-based MOFs and various molar ratios of Fe:Mn had some influence on crystallinity and surface structure of FeMn-Fc-MOFs. Within 120 min, FeMn-Fc-MOFs demonstrated the best catalytic activity among the different molar ratios, and acid orange 7(AO7) degradation rate was up to 92.
View Article and Find Full Text PDFUnderstanding how the morphology of a layered double hydroxide (LDH)-based catalyst alters its catalytic activity provides an available strategy for the rational design and fabrication of high-efficiency catalysts at a micro-scale. Herein, three nickel-iron layered double hydroxide (NiFe-LDH) catalysts including 2D-plate-like hexagon (P-NiFe-LDH), 2D/3D-flower-like solid sphere (FS-NiFe-LDH), and 2D/3D-flower-like hollow sphere (FH-NiFe-LDH) with regulable oxygen vacancies (OVs) were fabricated via a morphological regulation method of Ostwald ripening. The experimental results demonstrated that the three types of NiFe-LDH exhibited different abilities to activate persulfate (PS) for the abatement of acid orange 7 (AO7) with a sequence of FH-NiFe-LDH > FS-NiFe-LDH > P-NiFe-LDH.
View Article and Find Full Text PDFA series of LaNiO perovskite nanoparticles with different morphologies, such as spheres, rods and cubes, were prepared through co-precipitation and hydrothermal methods, and used as the catalysts for peroxydisulfate (PDS) activation. The physical and chemical characterization of LaNiO perovskites was performed, including X-ray diffraction (XRD), scanning electron microscopy (SEM), nitrogen isotherm absorption (BET), electrochemical impedance spectroscopy (EIS), and X-ray photoelectron spectroscopy (XPS). The LaNiO with different shapes showed different activities in Acid Orange 7 (AO7) degradation.
View Article and Find Full Text PDFFerrocene-based metal-organic framework with different transition metals (M-Fc-MOFs, M = Fe, Mn, Co) was synthesized by a simple hydrothermal method and used as a heterogeneous catalyst for persulfate activation. The samples were characterized by X-ray diffraction, transmission electron microscopy, X-ray electron spectroscopy, cyclic voltammetry, and electrochemical impedance spectroscopy. Meanwhile, the influences of factors such as catalyst dosage, persulfate concentration, and pH on the degradation of acid orange 7 (AO7) were studied in detail.
View Article and Find Full Text PDFMolecular chirality recognition plays a pivotal role in chiral generation and transfer in living systems and makes important contribution to the development of diverse applications spanning from chiral separation to soft nanorobots. To detect chirality recognition, most of the molecular sensors described to date are based on the design and preparation of the host-guest complexation with chromophore or fluorophore at the reporter unit. Nevertheless, the involved tedious procedures and complicated chemical syntheses hamper their practical applications.
View Article and Find Full Text PDFMolecular chirality transfer and amplification is at the heart of the fundamental understanding of chiral origin and fabrication of artificial chiral materials. We investigate here the nonlinear amplification effect in the chiral transfer from small molecules to assembled plasmonic nanoparticles. Our results show clearly a recognizable nonlinear behavior of the electronic and plasmonic circular dichroism activities, demonstrating the validity of the "majority-rules" principle operating in both the three-dimensional interface-confined molecularly chiral environment and the assembled plasmonic nanoparticles.
View Article and Find Full Text PDFExceptional points (EPs), branch points of complex energy surfaces at which eigenvalues and eigenvectors coalesce, are ubiquitous in non-Hermitian systems. Many novel properties and applications have been proposed around the EPs. One of the important applications is to enhance the detection sensitivity.
View Article and Find Full Text PDFThe ability to detect chiral molecules renders plasmonic nanosensors as promising tools for the study of chirality phenomena in living systems. Using gold nanorod based plasmonic nanosensors, we investigated here typically chiral zwitterionic electrostatic (Zw-Es) and hydrogen-bonding (Hb) interactions occurring via amine and carboxylic groups at nanoscale interfaces in aqueous solutions. Our results reveal that the plasmonic circular dichroism responses of the nanosensors can have both conformational sensitivity and chiral selectivity to the interfacial molecular interactions.
View Article and Find Full Text PDFWe report here the chiroptical amplification effect occurring in the hybrid systems consisting of chiral molecules and Si nanostructures. Under resonant excitation of circularly polarized light, the hybrid systems show strong CD induction signals at the optical frequency, which arise from both the electric and magnetic responses of the Si nanostructures. More interestingly, the induced CD signals from Si-based dielectric nanoantennas are always larger than that from Au-based plasmonic counterparts.
View Article and Find Full Text PDFRecently, there has been great interest in studying ultrasensitive detection and characterization of biomolecules using plasmonic particles, because they are of considerable importance in biomedical science and pharmaceutics. So far, all the theories on plasmon-induced circular dichroism (CD) have been based on the dipole approximation; the electric quadrupolar contribution is generally considered to be relatively small and neglected. Here we demonstrate that the electric quadrupolar contribution not only cannot be ignored, but it also plays a key role in many cases.
View Article and Find Full Text PDFWhether or not chiral interaction exists between the optical orbital angular momentum (OAM) and a chiral molecule remains unanswered. So far, such an interaction has not been observed experimentally. Here we present a T-matrix method to study the interaction between optical OAM and the chiral molecule in a cluster of nanoparticles.
View Article and Find Full Text PDFWe report on the chiroptical transfer and amplification effect observed in plasmonic polymers consisting of achiral gold nanorod monomers linked by cysteine chiral molecules in an end-to-end fashion. A new strategy for controlling the hot spots based circular dichroism (CD)-active sites in plasmonic polymers was developed to realize tailored and reproducible chiroptical activity in a controlled way. We showed that by regulating the bond angles between adjacent nanorods and the degree of polymerization in the linear plasmonic polymer, weak molecular chirality in the ultraviolet spectral region can be amplified by more than two orders of magnitude via the induced CD response in the visible/near infrared region.
View Article and Find Full Text PDFThin films of molecular gels formed in a confined space have potential applications in transdermal delivery, artificial skin, molecular electronics, etc. The microstructures and properties of thin gel films can be significantly different from those of their bulk counterparts. However, so far a comprehensive understanding of the effects of spatial confinement on the molecular gelation kinetics, fiber network structure and related mechanical properties is still lacking.
View Article and Find Full Text PDFRecently, there are great interest in studying the interaction between chiral molecules and plasmonic particles, because a weak circular dichroism (CD) signal in the ultraviolet (UV) region from chiral molecules can be both enhanced and transferred to the visible wavelength range by using plasmonic particles. Thus, ultrasensitive probe of tiny amounts of chiral substance by CD are worth waiting for. Here we present another way to strongly enhance CD of chiral molecules by using plasmonic particle cluster, which need not transfer to the visible wavelength.
View Article and Find Full Text PDFWe fabricate the linear chains of twisted gold nanorods by a facile chiral molecular templating method. In such a chiral plasmonic system, particle-particle separation distances are in the order of the light wavelength and are much larger than the sizes of individual particles. As a result, the inter-particle interactions in this chiral system are mediated mainly by a relatively weak far-field plasmonic coupling, rather than a strong near-field coupling.
View Article and Find Full Text PDFUnderstanding the role of kinetics in fiber network microstructure formation is of considerable importance in engineering gel materials to achieve their optimized performances/functionalities. In this work, we present a new approach for kinetic-structure analysis for fibrous gel materials. In this method, kinetic data is acquired using a rheology technique and is analyzed in terms of an extended Dickinson model in which the scaling behaviors of dynamic rheological properties in the gelation process are taken into account.
View Article and Find Full Text PDFWe present a new generic strategy to fabricate nanoparticles in the "cages" within the fibrous networks of supramolecular soft materials. As the cages can be acquired by a design-and-production manner, the size of nanoparticles synthesized within the cages can be tuned accordingly. To implement this idea, both selenium and silver were chosen for the detailed investigation.
View Article and Find Full Text PDFThe formation of most organogels requires the compatibility of both the gelator and solvent. It is very desirable if the rheological properties of a gel can be manipulated to achieve the desired performance. In this paper, a novel organogel was developed and its rheological properties and fiber network were engineered by controlling the thermal processing conditions.
View Article and Find Full Text PDFA new approach of engineering of molecular gels was established on the basis of a nucleation-initiated network formation mechanism. A variety of gel network structures can be obtained by regulating the starting temperature of the sol-gel transition. This enables us to tune the network from the spherulitic domains pattern to the extensively interconnected fibrillar network.
View Article and Find Full Text PDFLow-molecular mass organic gelators self-organizing into three-dimensional fiber networks within organic solvents have attracted much attention in recent years. However, to date, how the microstructure of fiber network is formed in a gelation process and the key factors that govern the topological structure of a gel network remain to be determined. In this work, we address these issues by investigating the in situ formation of the gel networks in the N-lauroyl-l-glutamic acid di-n-butylamide (GP-1)/propylene glycol (PG) system.
View Article and Find Full Text PDFThe architecture of a biocompatible organogel formed by gelation of a small molecule organic gelator, N-lauroyl-L-glutamic acid di-n-butylamide, in isostearyl alcohol was investigated based on a supersaturation-driven crystallographic mismatch branching mechanism. By controlling the supersaturation of the system, the correlation length that determines the mesh size of the fiber network was finely tuned and the rheological properties of the gel were engineered. This approach is of considerable significance for many gel-based applications, such as controlled release of drugs that requires precise control of the mesh size.
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