Understanding the oxidation chemistry of Ti_(3)C_(2)T_(x)(MXene)sheets and their catalytic performances

Transition metal carbides and nitrides(MXenes)nanosheets are attractive two-dimensional(2D)materials,but they suffer from oxidation/degradation issues during storage and/or applications due to their sensitivity to water and oxygen.Despite the great research progress,the exact oxidation kinetics of Ti_(3)C_(2)T_(x)(MXene)and their final products after oxidation are not fully understood.Herein,we systematically tracked the oxidation process of few-layer Ti_(3)C_(2)T_(x) nanosheets in an aqueous solution at room temperature over several weeks.We also studied the oxidation effects on the electrocatalytic properties of Ti_(3)C_(2)T_(x) for hydrogen evolution reaction and found that the overpotential to achieve a current density of 10 mA cm^(-2)increases from 0.435 to 0.877 V after three weeks of degradation,followed by improvement to stabilized values of around 0.40 V after eight weeks.These results suggest that severely oxidized MXene could be a promising candidate for designing efficient catalysts.According to our detailed experimental characterization and theoretical calculations,unlike previous studies,black titanium oxide is formed as the final product in addition to white Ti(IV)oxide and disordered carbons after the complete oxidation of Ti_(3)C_(2)T_(x).This work presents significant advancements in better understanding of 2D Ti_(3)C_(2)T_(x)(MXene)oxidation and enhances the prospects of this material for various applications.

Surface Treatment of Inorganic CsPbI_(3) Nanocrystals with Guanidinium Iodide for Efficient Perovskite Light-Emitting Diodes with High Brightness

The remarkable evolution of metal halide perovskites in the past decade makes them promise for next-generation optoelectronic material.In particular,nanocrystals(NCs)of inorganic perovskites have demonstrated excellent performance for light-emitting and display applications.However,the presence of surface defects on the NCs negatively impacts their performance in devices.Herein,we report a compatible facial post-treatment of CsPbI_(3) nanocrystals using guanidinium iodide(GuI).It is found that the GuI treatment effectively passivated the halide vacancy defects on the surface of the NCs while offering effective surface protection and exciton confinement thanks to the beneficial contribution of iodide and guanidinium cation.As a consequence,the film of treated CsPbI_(3) nanocrystals exhibited significantly enhanced luminescence and charge transport properties,leading to high-performance light-emitting diode with maximum external quantum efficiency of 13.8%with high brightness(peak luminance of 7039 cd m^(−2) and a peak current density of 10.8 cd A^(−1)).The EQE is over threefold higher than performance of untreated device(EQE:3.8%).The operational half-lifetime of the treated devices also was significantly improved with T50 of 20 min(at current density of 25 mA cm^(−2)),outperforming the untreated devices(T50~6 min).

Efficient CO_(2)Reduction to Formate on CsPbI_(3) Nanocrystals Wrapped with Reduced Graphene Oxide

Transformation of greenhouse gas(CO_(2))into valuable chemicals and fuels is a promising route to address the global issues of climate change and the energy crisis.Metal halide perovskite catalysts have shown their potential in promoting CO_(2)reduction reaction(CO_(2)RR),however,their low phase stability has limited their application perspective.Herein,we present a reduced graphene oxide(rGO)wrapped CsPbI_3 perovskite nanocrystal(NC)CO_(2)RR catalyst(CsPbI_3/rGO),demonstrating enhanced stability in the aqueous electrolyte.The CsPbI_3/rGO catalyst exhibited>92%Faradaic efficiency toward formate production at a CO_(2)RR current density of~12.7 mA cm^(-2).Comprehensive characterizations revealed the superior performance of the CsPbI_3/rGO catalyst originated from the synergistic effects between the CsPbI_3 NCs and rGO,i.e.,rGO stabilized theα-CsPbI_3 phase and tuned the charge distribution,thus lowered the energy barrier for the protonation process and the formation of~*HCOO intermediate,which resulted in high CO_(2)RR selectivity toward formate.This work shows a promising strategy to rationally design robust metal halide perovskites for achieving efficient CO_(2)RR toward valuable fuels.

Blue emitting exciplex for yellow and white organic light‑emitting diodes

White organic light-emitting diodes(WOLEDs)have several desirable features,but their commercialization is hindered by the poor stability of blue light emitters and high production costs due to complicated device structures.Herein,we investigate a standard blue emitting hole transporting material(HTM)N,N'-bis(naphthalen-1-yl)-N,N'-bis(phenyl)benzidine(NPB)and its exciplex emission upon combining with a suitable electron transporting material(ETM),3-(biphenyl-4-yl)-5-(4-tert-butylphenyl)-4-phenyl-4H-1,2,4-triazole(TAZ).Blue and yellow OLEDs with simple device structures are developed by using a blend layer,NPB:TAZ,as a blue emitter as well as a host for yellow phosphorescent dopant iridium(III)bis(4-phenylthieno[3,2-c]pyridinato-N,C2')acetylacetonate(PO-01).Strategic device design then exploits the ambipolar charge transport properties of tetracene as a spacer layer to connect these blue and yellow emitting units.The tetracene-linked device demonstrates more promising results compared to those using a conventional charge generation layer(CGL).Judicious choice of the spacer prevents exciton difusion from the blue emitter unit,yet facilitates charge carrier transport to the yellow emitter unit to enable additional exciplex formation.This complementary behavior of the spacer improves the blue emission properties concomitantly yielding reasonable yellow emission.The overall white light emission properties are enhanced,achieving CIE coordinates(0.36,0.39)and color temperature(4643 K)similar to daylight.Employing intermolecular exciplex emission in OLEDs simplifes the device architecture via its dual functionality as a host and as an emitter.

An external quantum efficiency of>20%from solutionprocessed poly(dendrimer)organic light-emitting diodes

Controlling the orientation of the emissive dipole has led to a renaissance of organic light-emitting diode(OLED)research,with external quantum efficiencies(EQEs)of>30%being reported for phosphorescent emitters.These highly efficient OLEDs are generally manufactured using evaporative methods and are comprised of small-molecule heteroleptic phosphorescent iridium(III)complexes blended with a host and additional layers to balance charge injection and transport.Large area OLEDs for lighting and display applications would benefit from low-cost solution processing,provided that high EQEs could be achieved.Here,we show that poly(dendrimer)s consisting of a non-conjugated polymer backbone with iridium(III)complexes forming the cores of firstgeneration dendrimer side chains can be co-deposited with a host by solution processing to give highly efficient devices.Simple bilayer devices comprising the emissive layer and an electron transport layer gave an EQE of>20%at luminances of up to≈300 cd/m^(2),showing that polymer engineering can enable alignment of the emissive dipole of solution-processed phosphorescent materials.

On the unipolarity of charge transport in methanofullerene diodes

Fullerenes are electron transporting organic semiconductors with a wide range of applications.In particular,methanofullerenes have been the preferred choice for solution-processed solar cells and photodiodes.The wide applicability of fullerenes as both‘ntype’transport materials and electron acceptors is clear.However,what is still a matter of debate is whether the fullerenes can also support efficient transport of holes,particularly in diode geometries.In this letter,we utilize a number of recently developed experimental methods for selective electron and hole mobility measurements.We show for the two most widely used solution processable fullerenes,PC70-and-PC60BM,that whilst both exhibit electron mobilities as high as 10^(−3)cm^(2)/Vs,their hole mobilities are<10^(−9)cm^(2)/Vs.Thus charge transport in these fullerenes can be considered predominantly unipolar in diode configurations.