Solution-processed colloidal III-V semiconductor-based quantum dots (QDs) represent promising and environmentally-friendly alternatives to Cd-based QDs in the realms of optoelectronics and biological applications. While InP-based core-shell QDs have demonstrated efficient light-emitting diode (LED) performance in the visible region, achieving deep-red emission (above 700 nm) with a narrow linewidth has proven challenging. Herein, the study presents a novel strategy for synthesizing InP/ZnSe/ZnS core-shell-shell QDs tailored for emission in the first biological transparency window.
View Article and Find Full Text PDFBismuth iodide perovskite nanocrystals are considered a viable alternative to the Pb halide ones due to their reduced toxicity and increased stability. However, it is still challenging to fabricate nanocrystals with a small and controlled size, and their electronic properties are not well understood. Here, we propose the growth of Bi iodide perovskite nanocrystals using different mesoporous silica with ordered pores of controlled diameter as templates.
View Article and Find Full Text PDFElectrode-confined molecular catalysts are promising systems to enable the efficient conversion of CO to useful products. Here, we describe the development of an original molecular cathode for CO reduction to CO based on the noncovalent integration of a tetraazamacrocyclic Co complex to a carbon nanotube-based matrix. Aqueous electrochemical characterization of the modified electrode allowed for clear observation of a change of redox behavior of the Co center as surface concentration was tuned, highlighting the impact of the catalyst microenvironment on its redox properties.
View Article and Find Full Text PDFWe present a new open-loop implementation of Kelvin probe force microscopy (KPFM) that provides access to the Fourier spectrum of the time-periodic surface electrostatic potential generated under optical (or electrical) pumping with an atomic force microscope. The modulus and phase coefficients are probed by exploiting a double heterodyne frequency mixing effect between the mechanical oscillation of the cantilever, modulated components of the time-periodic electrostatic potential at harmonic frequencies of the pump, and an ac bias modulation signal. Each harmonic can be selectively transferred to the second cantilever eigenmode.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
November 2023
Solution-processed quantum dot (QD) based blue emitters are of paramount importance in the field of optoelectronics. Despite large research efforts, examples of efficient deep blue/near UV-emitting QDs remain rare due to lack of luminescent wide band gap materials and high defect densities in the existing ones. Here, we introduce a novel type of QDs based on heavy metal free gallium sulfide (Ga S ) and their core/shell heterostructures Ga S /ZnS as well as Ga S /ZnS/Al O .
View Article and Find Full Text PDFHalide perovskite materials possess excellent optoelectronic properties and have shown great potential for direct X-ray detection. Perovskite wafers are particularly attractive among various detection structures due to their scalability and ease of preparation, making them the most promising candidates for X-ray detection and array imaging applications. However, device instability and current drift caused by ionic migration are persistent challenges for perovskite detectors, especially in polycrystalline wafers with numerous grain boundaries.
View Article and Find Full Text PDFMixed lead-tin (PbSn) perovskite solar cells (PSCs) possess low toxicity and adjustable bandgap for both single-junction and all-perovskite tandem solar cells. However, the performance of mixed PbSn PSCs still lags behind the theoretical efficiency. The uncontrollable crystallization and the resulting structural defect are important reasons.
View Article and Find Full Text PDFMolecular hydrogen (H) is considered one of the most promising fuels to decarbonize the industrial and transportation sectors, and its photocatalytic production from molecular catalysts is a research field that is still abounding. The search for new molecular catalysts for H production with simple and easily synthesized ligands is still ongoing, and the terpyridine ligand with its particular electronic and coordination properties, is a good candidate to design new catalysts meeting these requirements. Herein, we have isolated the new mono-terpyridyl rhodium complex, [Rh(tpy)(CHCN)Cl](CFSO) (), and shown that it can act as a catalyst for the light-induced proton reduction into H in water in the presence of the [Ru(bpy)]Cl () photosensitizer and ascorbate as sacrificial electron donor.
View Article and Find Full Text PDFB-site doping is an emerging strategy for tuning the emission wavelength of cesium lead halide ABX nanocrystals. We present a simple method for the postsynthetic doping of CsPbBr nanocrystals with aluminum at room temperature by exposing them to a solution of AlBr in dibromomethane. Despite the much smaller ionic radius of Al compared to that of Pb, nominal doping levels in a range from 8.
View Article and Find Full Text PDFThe production of hydrogen by efficient, low-cost, and integrated photoelectrochemical water splitting processes represents an important target for the ecological transition. This challenge can be addressed thanks to bioinspired chemistry and artificial photosynthesis approaches by designing dye-sensitized photocathodes for hydrogen production, incorporating bioinspired first-row transition metal-based catalysts. The present work describes the preparation and photoelectrochemical characterization of a NiO photocathode sensitized with a phosphonate-derivatized ruthenium tris-diimine photosensitizer covalently linked to a cobalt diimine dioxime hydrogen-evolving catalyst.
View Article and Find Full Text PDFTin oxide (SnO ) is an emerging electron transport layer (ETL) material in halide perovskite solar cells (PSCs). Among current limitations, open-circuit voltage (V ) loss is one of the major factors to be addressed for further improvement. Here a bilayer ETL consisting of two SnO nanoparticle layers doped with different amounts of ammonium chloride is proposed.
View Article and Find Full Text PDFSilicon (Si) is the most promising anode candidate for the next generation of lithium-ion batteries but difficult to cycle due to its poor electronic conductivity and large volume change during cycling. Nanostructured Si-based materials allow high loading and cycling stability but remain a challenge for process and engineering. We prepare a Si nanowires-grown-on-graphite one-pot composite (Gt-SiNW) a simple and scalable route.
View Article and Find Full Text PDFA facile hydrothermal method to synthesize water-soluble copper indium sulfide (CIS) nanocrystals (NCs) at 150 °C is presented. The obtained samples exhibited three distinct photoluminescence peaks in the red, green and blue spectral regions, corresponding to three size fractions, which could be separated by means of size-selective precipitation. While the red and green emitting fractions consist of 4.
View Article and Find Full Text PDFEu is used to replace toxic Pb in metal halide perovskite nanocrystals (NCs). The synthesis implies injection of cesium oleate into a solution of europium (ii) bromide at an experimentally determined optimum temperature of 130 °C and a reaction time of 60 s. Structural analysis indicates the formation of spherical CsEuBr nanoparticles with a mean size of 43 ± 7 nm.
View Article and Find Full Text PDFCdTe/CdS core/shell quantum dots (QDs) are formed in aqueous synthesis via the partial decomposition of hydrophilic thiols, used as surface ligands. In this work, we investigate the influence of the chemical nature (functional group and chain length) of the used surface ligands on the shell formation. Four different surface ligands are compared: 3-mercaptopropionic acid, MPA, thioglycolic acid, TGA, sodium 3-mercaptopropanesulfonate, MPS, and sodium 2-mercaptoethanesulfonate, MES.
View Article and Find Full Text PDFHydrogen production through direct sunlight-driven water splitting in photo-electrochemical cells (PECs) is a promising solution for energy sourcing. PECs need to fulfill three criteria: sustainability, cost-effectiveness and stability. Here we report an efficient and stable photocathode platform for H evolution based on Earth-abundant elements.
View Article and Find Full Text PDF[NiFe]-hydrogenase enzymes are efficient catalysts for H evolution but their synthetic models have not been reported to be active under aqueous conditions so far. Here we show that a close model of the [NiFe]-hydrogenase active site can work as a very active and stable heterogeneous H evolution catalyst under mildly acidic aqueous conditions. Entry in catalysis is a Ni Fe complex, with electronic structure analogous to the Ni-L state of the enzyme, corroborating the mechanism modification recently proposed for [NiFe]-hydrogenases.
View Article and Find Full Text PDFThe motion of CHNH cations in the low-temperature phase of the promising photovoltaic material methylammonium lead triiodide (CHNHPbI) is investigated experimentally as well as theoretically, with a particular focus on the activation energy. Inelastic and quasi-elastic neutron scattering measurements reveal an activation energy of ∼48 meV. Through a combination of experiments and first-principles calculations, we attribute this activation energy to the relative rotation of CH against an NH group that stays bound to the inorganic cage.
View Article and Find Full Text PDFTernary metal chalcogenide nanocrystals (NCs) offer exciting opportunities as novel materials to be explored on the nanoscale showing optoelectronic properties tunable with size and composition. CuInS (CIS) NCs are the most widely studied representatives of this family as they can be easily prepared with good size control and in high yield by reacting the metal precursors (copper iodide and indium acetate) in dodecanethiol (DDT). Despite the widespread use of this synthesis method, both the reaction mechanism and the surface state of the obtained NCs remain elusive.
View Article and Find Full Text PDFSilicon nanowires were coated by a 1-5 nm thin alumina layer by atomic layer deposition (ALD) in order to replace poorly reproducible and unstable native silicon oxide by a highly conformal passivating alumina layer. The surface coating enabled probing the behavior of symmetric devices using such electrodes in the EMI-TFSI electrolyte, allowing us to attain a large cell voltage up to 6 V in ionic liquid, together with very high cyclability with less than 4% capacitance fade after 10 charge/discharge cycles. These results yielded fruitful insights into the transition between an electrochemical double-layer capacitor behavior and an electrolytic capacitor behavior.
View Article and Find Full Text PDFRecent progress in quantum dot (QD) sensitized solar cells has demonstrated the possibility of low-cost and efficient photovoltaics. However, the standard device structure based on n-type materials often suffers from slow hole injection rate, which may lead to unbalanced charge transport. We have fabricated efficient p-type (inverted) QD sensitized cells, which combine the advantages of conventional QD cells with p-type dye sensitized configurations.
View Article and Find Full Text PDFACS Appl Mater Interfaces
July 2016
A versatile and robust hierarchically multifunctionalized nanostructured material made of poly(3,4-(ethylenedioxy)thiophene) (PEDOT)-coated diamond@silicon nanowires has been demonstrated to be an excellent capacitive electrode for supercapacitor devices. Thus, the electrochemical deposition of nanometric PEDOT films on diamond-coated silicon nanowire (SiNW) electrodes using N-methyl-N-propylpyrrolidinium bis((trifluoromethyl)sulfonyl)imide ionic liquid displayed a specific capacitance value of 140 F g(-1) at a scan rate of 1 mV s(-1). The as-grown functionalized electrodes were evaluated in a symmetric planar microsupercapacitor using butyltrimethylammonium bis((trifluoromethyl)sulfonyl)imide aprotic ionic liquid as the electrolyte.
View Article and Find Full Text PDFTin sulfide nanoparticles have a great potential for use in a broad range of applications related to solar energy conversion (photovoltaics, photocatalysis), electrochemical energy storage, and thermoelectrics. The development of chemical synthesis methods allowing for the precise control of size, shape, composition, and crystalline phase is essential. We present a novel approach giving access to monodisperse square SnS nanoplatelets, whose dimensions can be adjusted in the range of 4-15 nm (thickness) and 15-100 nm (edge length).
View Article and Find Full Text PDFThe synthesis and X-ray crystal structure of the ligand L (4,7-dicarbazol-9-yl-[1,10]-phenanthroline) are reported, as well as those of the molecular complex, [Eu(tta)(3)(L)] (1), (tta = 2-thenoyl trifluoroacetylacetonate). Their photophysical properties have been investigated both in solution and in the solid state. It was shown that the ligands used for designing 1 are well-suited for sensitizing the Eu(III) ion emission, thanks to a favorable position of the triplet state as investigated in the Gd(III) complex [Gd(tta)(3)(L)], (2).
View Article and Find Full Text PDFEthanol-mediated metal transfer printing (mTP) is a soft method, which allows to efficiently deposit metals onto various organic surfaces for applications in organic electronics. This simple approach in based on the stronger adhesion of the metals to the organic materials in the presence of thin ethanol layer between the metallized PDMS and the substrate due to the capillary action. Patterns with a resolution of at least 20 μm have been obtained on organic polymeric materials and photoresists without heating or applied pressure.
View Article and Find Full Text PDF