RESUMEN
Dual-atom catalytic sites on conductive substrates offer a promising opportunity for accelerating the kinetics of multistep hydrogen and oxygen evolution reactions (HER and OER, respectively). Using MXenes as substrates is a promising strategy for depositing those dual-atom electrocatalysts, if the efficient surface anchoring strategy ensuring metal-substrate interactions and sufficient mass loading is established. We introduce a surface-modification strategy of MXene substrates by preadsorbing L-tryptophan molecules, which enabled attachment of dual-atom Co/Ni electrocatalyst at the surface of Ti3C2Tx by forming N-Co/Ni-O bonds, with mass loading reaching as high as 5.6 wt %. The electron delocalization resulting from terminated O atoms on MXene substrates, N atoms in L-tryptophan anchoring moieties, and catalytic metal atoms Co and Ni provides an optimal adsorption strength of intermediates and boosts the HER and OER kinetics, thereby notably promoting the intrinsic activity of the electrocatalyst. CoNi-Ti3C2Tx electrocatalyst displayed HER and OER overpotentials of 31 and 241 mV at 10 mA cm-2, respectively. Importantly, the CoNi-Ti3C2Tx electrocatalyst also exhibited high operational stability for both OER and HER over 100 h at an industrially relevant current density of 500 mA cm-2. Our study provided guidance for constructing dual-atom active metal sites on MXene substrates to synergistically enhance the electrochemical efficiency and stability of the energy conversion and storage systems.
RESUMEN
The development of ultraviolet circularly polarized light (UVCPL) sources has the potential to benefit plenty of practical applications but remains a challenge due to limitations in available material systems and a limited understanding of the excited state chirality transfer. Herein, by constructing hybrid structures of the chiral perovskite CsPbBr3 nanoplatelets and organic molecules, excited state chirality transfer is achieved, either via direct binding or triplet energy transfer, leading to efficient UVCPL emission. The underlying photophysical mechanisms of these two scenarios are clarified by comprehensive optical studies. Intriguingly, UVCPL realized via the triple energy transfer, followed by the triplet-triplet annihilation upconversion processes, demonstrates a 50-fold enhanced dissymmetry factor glum . Furthermore, stereoselective photopolymerization of diacetylene monomer is demonstrated by using such efficient UVCPL. This study provides both novel insights and a practical approach for realizing UVCPL, which can also be extended to other material systems and spectral regions, such as visible and near-infrared.
RESUMEN
A large volume, scalable synthesis procedure of HgTe quantum dots (QDs) capped initially with short-chain conductive ligands ensures ligand exchange-free and simple device fabrication. An effective n- or p-type self-doping of HgTe QDs is achieved by varying cation-anion ratio, as well as shifting the Fermi level position by introducing single- or double-cyclic thiol ligands, that is, 2-furanmethanethiol (FMT) or 2,5-dimercapto-3,4-thiadiasole (DMTD) in the synthesis. This allows for preserving the intact surface of the HgTe QDs, thus ensuring a one order of magnitude reduced surface trap density compared with HgTe subjected to solid-state ligand exchange. The charge carrier diffusion length can be extended from 50 to 90 nm when the device active area consists of a bi-layer of cation-rich HgTe QDs capped with DMTD and FMT, respectively. As a result, the responsivity under 1340 nm illumination is boosted to 1 AW-1 at zero bias and up to 40 AW-1 under -1 V bias at room temperature. Due to high noise current density, the specific detectivity of these photodetectors reaches up to 1010 Jones at room temperature and under an inert atmosphere. Meanwhile, high photoconductive gain ensures a rise in the external quantum efficiency of up to 1000% under reverse bias.
RESUMEN
The co-doping of double perovskites is a useful approach in terms of improving their stability and photoluminescence quantum yield. Herein, Bi3+ and Te4+ cations have been co-doped into Cs2AgInCl6 nanocrystals. Doping with Te4+ cations promotes radiative recombination of self-trapped excitons due to increased defect formation energies of silver and indium vacancies, according to experimental and theoretical results. When used in excess, the TeO2 precursor would generate residual TeO2, Te2O3Cl2, R2TeO, or all three of them, which confined undesired chlorine ions on oxygen vacancies to counteract the pull from the Cs2AgInCl6 host, resulting in improved coordination with surface oleic acid ligands. As a result, 1% Bi and 8% Te co-doped Cs2AgInCl6 nanocrystals reach a high photoluminescence quantum yield of 34% and show an improved stability, maintaining over 70% of their original emission intensity after storage for more than 1 month. These findings are important in the context of producing high-performance properly doped double perovskite nanocrystals for optoelectronic applications.
RESUMEN
Lead-free two-dimensional metal halide perovskites have recently emerged as promising light-emitting materials due to their improved stability and attractive optical properties. Herein, a facile room temperature wet milling method has been developed to make Dion-Jacobson (DJ) phase ODASnBr4 perovskite microcrystals, whose crystallization was accomplished via the aid of introduced primary alcohols: ethanol, butanol, pentanol, and hexanol. Due to the strong intermolecular hydrogen bonding, the use of ethanol promoted the formation of non-doped ODASnBr4 microcrystals, with an emission peaked at 599 nm and a high photoluminescence quantum yield (PL QY) of 81%. By introducing other primary alcohols with weaker intermolecular hydrogen bonding such as butanol, pentanol, and hexanol, [SnBr6]4- octahedral slabs of the DJ perovskite microcrystals experienced various degrees of expansion while forming O-H Br hydrogen bonds. This resulted in the emission spectra of these alcohol-doped microcrystals to be adjusted in the range from 572 to 601 nm, while keeping the PL QY high, at around 89%. Our synthetic strategy provides a viable pathway towards strongly emitting lead-free DJ perovskite microcrystals with an improved stability.
