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Heterogeneous Growth of Continuous ZIF-8 Films on Low-Temperature Amorphous Silicon
摘要： Thin amorphous silicon films, deposited at low temperature by Inductively Coupled Plasma Chemical Vapor Deposition, have, for the first time, been employed as substrate for ZIF-8 growth. In order to investigate the role of the surface chemistry on the nucleation process, films have also been grown on other silicon-based substrates such as H-terminated Si(100), SiO2 and quartz. Film preparation was carried out at room temperature using a mixed Zn nitrate and imidazole solution in methanol or ethanol. Using methanol, continuous ZIF-8 films were obtained on amorphous Si and H-terminated Si(100), while less homogeneous films were formed on the other surfaces. In ethanol, slower growth rates occurred and thinner films, compared to the ones in methanol, were obtained. These slower rates highlight the different effects of the four surfaces on the growth process. These differences have been related to the silanol density of the surfaces and to the Lewis basic strength which affect imidazole moiety deprotonation. H-terminated Si(100) and amorphous Si turned out to be the most reactive surfaces, whereas on quartz and, especially, on SiO2 reactivity was much lower. Experimental results have been validated by the DFT modelling of the proton exchange, which takes place between the imidazole group and the surface. Finally, the VOCs adsorption capability of ZIF-8 films grown on amorphous silicon has been evaluated through temperature desorption experiments.
关键词： a-Si layer,ZIF-8 coating,growth mechanisms,VOCs adsorption,surface chemistry
更新于2025-11-21 11:03:25
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Post-synthesis phase and shape evolution of CsPbBr3 colloidal nanocrystals: The role of ligands
摘要： The surface chemistry of colloidal cesium lead bromide (CsPbBr3) nanocrystals is decisive in determining the stability and the final morphology of this class of materials, characterized by ionic structure and a high defect tolerance factor. Here, the high sensitivity of purified colloidal nanocubes of CsPbBr3 to diverse environmental condition (solvent dilution, ageing, ligands post synthetic treatment) in ambient atmosphere is investigated by means of a comprehensive morphological (electron microscopy), structural (θ/2θ X-ray diffraction (XRD) and grazing incidence wide angle scattering (GIWAXS)), and spectroscopic chemical (1H nuclear magnetic resonance (NMR), nuclear Overhauser effect spectroscopy (NOESY), absorption and emission spectroscopy) characterization. The aging and solvent dilution contribute to modify the nanocrystal morphology, due to a modification of the ligand dynamic. Moreover, we establish the ability of aliphatic carboxylic acids and alkyl amines ligands to induce, even in a post preparative process at room temperature, structural, morphological and spectroscopic variations. Upon post synthesis alkyl amine addition, in particular of oleyl amine and octyl amine, the highly green emitting CsPbBr3 nanocubes effectively turn into one-dimensional (1D) thin tetragonal nanowires or lead halide deficient rhombohedral zero-dimensional (0D) Cs4PbBr6 structures with a complete loss of fluorescence. The addition of an alkyl carboxylic acid, as oleic and nonanoic acid, produces the transformation of nanocubes into still emitting orthorombic two-dimensional (2D) nanoplates. The acid/base equilibrium between the native and added ligands, the adsorbed/free ligands dynamic in solution and the ligand solubility in non-polar solvent contribute to render CsPbBr3 particularly sensitive to environmental and processing conditions and, therefore prone to undergo to structural, morphological and, hence spectroscopic, transformations.
关键词： lead halide perovskite nanocrystals,surface chemistry,ligands equilibria,long term stability
更新于2025-11-21 11:01:37
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Effect of counter-surface chemistry on defect-free material removal of monocrystalline silicon
摘要： To bring light on material removal remains fundamental for promoting the advancement of nanotechnology. In this study, nanoscratching test on silicon surface against Al2O3 microsphere was performed using an atomic force microscope, and the material removal by SiO2 microsphere sliding was taken as a comparison. It was found that nanochannels can be produced on silicon surface by Al2O3 microsphere scratching under much lower contact pressure than the yield limit for plastic deformation, which can be ascribed to water-participated tribochemical reactions. The tribochemical removal was verified by high resolution transmission electron microscope (HRTEM) detection. Further analysis indicates that the tribochemical reactions on silicon surface are strongly affected by the counter-surface chemistry. It is noted that counter-surface chemistry influences the tribochemical reactions via altering the activation energy barrier for forming bonding bridge, and has little influence on decreasing the activation energy barrier for the rupture of Si-Si backbonds in silicon substrate. Compared with SiO2 tip, Al2O3 tip has longer working life span, and the nanochannels fabricated by Al2O3 tip under the same processing conditions exhibit better uniformity even in KOH solution. The results provide useful knowledge for chemical mechanical polishing and tip-based nanomanufacturing processes, and shed new light for enriching the basic theory of nanotribology.
关键词： Tribochemical removal,Nanoscratching,Counter-surface chemistry,Alumina/silicon pair
更新于2025-11-14 17:03:37
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High-Performance Chromatographic Characterization of Surface Chemical Heterogeneities of Fluorescent Organic–Inorganic Hybrid Core–Shell Silica Nanoparticles
摘要： In contrast to small-molar-mass compounds, detailed structural investigations of inorganic core–organic ligand shell hybrid nanoparticles remain challenging. The assessment of batch-reaction-induced heterogeneities of surface chemical properties and their correlation with particle size has been a particularly long-standing issue. Applying a combination of high-performance liquid chromatography (HPLC) and gel permeation chromatography (GPC) to ultra-small (<10 nm diameter) poly(ethylene glycol)-coated (PEGylated) fluorescent core–shell silica nanoparticles, we elucidate here previously unknown surface heterogeneities resulting from varying dye conjugation to nanoparticle silica cores and surfaces. Heterogeneities are predominantly governed by dye charge, as corroborated by molecular dynamics simulations. We demonstrate that this insight enables the development of synthesis protocols to achieve PEGylated and targeting ligand-functionalized PEGylated silica nanoparticles with dramatically improved surface chemical homogeneity, as evidenced by single-peak HPLC chromatograms. Because surface chemical properties are key to all nanoparticle interactions, we expect these methods and fundamental insights to become relevant to a number of systems for applications, including bioimaging and nanomedicine.
关键词： surface chemistry heterogeneity,high-performance liquid chromatography,nanoparticle characterization,nanoparticle surface functionalization,fluorescence correlation spectroscopy,molecular dynamics,nanoparticle heterogeneity
更新于2025-09-23 15:23:52
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Heat-Assisted Photoacidic Oxidation Method for Tailoring the Surface Chemistry of Polymer Dielectrics for Low-Power Organic Soft Electronics
摘要： The use in low-power soft electronics of the appropriate insulating polymer materials with a high dielectric constant (k) is considered a practical alternative to that of inorganic dielectric materials, which are brittle and have high processing temperatures. However, the polar surfaces of typical high-k polymer insulators are problematic. Further, it is a huge challenge to control their surface properties without damage because of their soft and chemically fragile nature. Here, a heat-assisted photoacidic oxidation method that can be used to effectively oxidize the outermost surfaces of high-k rubbery polymer films without degradation is presented. The oxidized surfaces prepared with the developed method contain large numbers of hydroxyl groups that enable the subsequent growth of dense and ordered self-assembled monolayers (SAMs) consisting of organosilanes. The whole process modifies the surface characteristics of polymer dielectrics effectively. The mechanisms of the oxidation of polymer surfaces and the subsequent SAM growth process are investigated. The resulting surface-tailored rubbery dielectrics exhibit superior electrical characteristics when used in organic transistors. These results demonstrate that this method can be used to realize practical soft organic electronics based on high-k polymer dielectrics.
关键词： self-assembled monolayers,organic semiconductors,polymer gate dielectric,polymer oxidation,surface chemistry
更新于2025-09-23 15:23:52
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Surface potential tailoring of PMMA fibers by electrospinning for enhanced triboelectric performance
摘要： Triboelectric generators rely on contact-generated surface charge transfer between materials with different electron affinities to convert mechanical energy into useful electricity. The ability to modify the surface chemistry of polymeric materials can therefore lead to significant enhancement of the triboelectric performance. Poly(methyl methacrylate) (PMMA) is a biocompatible polymer commonly used in medical applications, but its central position on the triboelectric series, which empirically ranks materials according to their electron-donating or electron accepting tendencies, renders it unsuitable for application in triboelectric generators. Here, we show that the surface potential of PMMA fibers produced by electrospinning can be tailored through the polarity of the voltage used during the fabrication process, thereby improving its triboelectric performance, as compared to typically spin-coated PMMA films. The change in surface chemistry of the electrospun PMMA fibers is verified using X-ray photoelectron spectroscopy, and this is directly correlated to the changes in surface potential observed by Kelvin probe force microscopy. We demonstrate the enhancement of triboelectric energy harvesting capability of the electrospun PMMA fibers, suggesting that this surface potential modification approach can be more widely applied to other materials as well, for improved triboelectric performance.
关键词： Energy harvesting,Triboelectric generator,Surface chemistry,Kelvin probe force microscopy,Electrospinning,Poly(methyl methacrylate)
更新于2025-09-23 15:23:52
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Understanding the Sensing Mechanism of Rh2O3 loaded In2O3
摘要： The effect of Rh loading on CO sensing was studied for the case of In2O3. This was done by performing measurements with sensors based on loaded and unloaded materials that were performed at an operation temperature of 300 °C in the presence of low background oxygen concentration according to an experimental procedure that was demonstrated to help clarify the reception/transduction functions of loaded Semiconducting Metal Oxides (SMOX). The experimental investigation methods were DC resistance and Diffuse Reflectance Infrared Fourier Transform Spectroscopy (DRIFTS). The results indicate that in the case of Rh2O3 loaded In2O3 the reaction primary takes place on the Rh2O3 cluster and the electrical properties of the In2O3 are controlled by the pinning of the SMOX Fermi-level to the one of the Rh2O3 cluster.
关键词： SMOX,surface chemistry,gas sensors,operando,Rh2O3 loading,DRIFTS,In2O3
更新于2025-09-23 15:23:52
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X-ray photoelectron spectroscopy and Raman microscopy of a ferroan platinum crystal from the Kondyor Massif, Russian Far East
摘要： X-ray Photoelectron Spectroscopy was used to study a ferroan platinum crystal from the Kondyor Massif, Russian Far East. Prior to the X-ray Photoelectron Spectroscopic analyses, the nature of the crystal was confirmed by X-ray diffraction. The survey scan showed mainly the presence of Pt and Fe, with smaller amounts of O and Si. The high resolutions spectra of the Pt 4f and Fe 2p showed 18.3 atom% Fe in the crystal, which puts the composition on the lower boundary for ferroan platinum and confirms earlier analyses using other methods such as Scanning Electron Microscopy-Energy Dispersive X-ray analysis/microprobe. The binding energy of the Pt 4f5/2 was 74.0 eV and Pt 4f7/2 70.5 eV, while the Fe 2p3/2 for metallic Fe was observed at 707.2 eV. The Fe 2p3/2 for metallic Fe was significantly sharper than that of Fe 2p3/2 at 710.7 eV associated with surface material. The Raman spectrum was dominated by the Pt–Pt stretching mode at 253 cm?1. Changed orientation resulted in the observation of two bands at 127 and 139 cm?1, interpreted as being due to stretching modes of two Pt–Pt bonds with the third bond to Fe and Pt fixed. The presence of Ca-Fe-Al-Mg-Si-O on the surface was probably associated with the presence of a clinopyroxene. These minerals can be expected since the crystal came originally from a clinopyroxenite-dunite matrix. The spectra showed a variety of interferences, e.g. Al 2p with Pt 4f, Mg 2p with Fe 3p, and Ca 2p1/2 with Mg Auger, making exact determinations of the ratios of these elements difficult.
关键词： surface chemistry,platinum group minerals,X-ray photoelectron spectroscopy,Raman spectroscopy,Platinum
更新于2025-09-23 15:23:52
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Graphene veils: A versatile surface chemistry for sensors
摘要： Thin spun-coat films (~4 nm thick) of graphene oxide (GO) constitute a versatile surface chemistry compatible with a broad range of technologically important sensor materials. Countless publications are dedicated to the nuances of surface chemistries that have been developed for sensors, with almost every material having unique characteristics. There would be enormous value in a surface chemistry that could be applied generally with functionalization and passivation already optimized regardless of the sensor material it covered. Such a film would need to be thin, conformal, and allow for multiple routes toward covalent linkages. It is also vital that the film permit the underlying sensor to transduce. Here we show that GO films can be applied over a diverse set of sensor surfaces, can link biomolecules through multiple reaction pathways, and can support cell growth. Application of a graphene veil atop a magnetic sensor array is demonstrated with an immunoassay. We also present biosensing and material characterization data for these graphene veils.
关键词： film,biosensor,graphene oxide,surface chemistry,coating
更新于2025-09-23 15:22:29
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Fingerprints of sp1 Hybridized C in the Near-Edge X-ray Absorption Spectra of Surface-Grown Materials
摘要： Carbon structures comprising sp1 chains (e.g., polyynes or cumulenes) can be synthesized by exploiting on-surface chemistry and molecular self-assembly of organic precursors, opening to the use of the full experimental and theoretical surface-science toolbox for their characterization. In particular, polarized near-edge X-ray absorption fine structure (NEXAFS) can be used to determine molecular adsorption angles and is here also suggested as a probe to discriminate sp1/sp2 character in the structures. We present an ab initio study of the polarized NEXAFS spectrum of model and real sp1/sp2 materials. Calculations are performed within density functional theory with plane waves and pseudopotentials, and spectra are computed by core-excited C potentials. We evaluate the dichroism in the spectrum for ideal carbynes and highlight the main differences relative to typical sp2 systems. We then consider a mixed polymer alternating sp1 C4 units with sp2 biphenyl groups, recently synthesized on Au(111), as well as other linear structures and two-dimensional networks, pointing out a spectral line shape specifically due to the presence of linear C chains. Our study suggests that the measurements of polarized NEXAFS spectra could be used to distinctly fingerprint the presence of sp1 hybridization in surface-grown C structures.
关键词： density functional theory,self-assembly,carbynes,on-surface chemistry,near edge X-ray absorption spectroscopy,C 1s absorption
更新于2025-09-23 15:22:29