Stable photocatalysts with excellent optical adsorption and low reaction barrier are the key for the water splitting. Here, we find that a two-dimensional Janus WSSe monolayer possesses the compelling photocatalytic properties from density functional theory simulations, which can be well modulated with strain deformation. Comprehensive investigations indicate that the Janus material not only exhibits strong optical absorbance in the visible spectrum, suitable band edge potentials, high carrier separation, and transfer efficiency but also has adequate driving forces of photoexcited carrier for water redox reaction and good resistance against photoinduced corrosion. Janus WSSe is therefore predicted to be a promising photocatalyst for water splitting. Moreover, we also find that tensile strains could further improve the photocatalytic performance for water splitting by effectively increasing the energy conversion efficiency and reducing the exciton binding energy. Our results not only predict a photocatalyst, which can utilize the visible light for overall water splitting, but also propose an effective path to extend the absorption spectra and raise the photocatalytic efficiency.
electrical conductivity of the MOF NSs limit their electrocatalytic activity far from practical applications. In addition, timeconsuming coating procedures are always needed to attach powdered MOF NSs onto the surface of the electrode with the assistance of polymeric binders, which may decrease their original activity and cause mechanical stability problems.To address these issues, one effective and feasible way is directly growing the ultrathin BMNSs on self-supported 3D macroporous conductive substrates. In this kind of hierarchical structure, first, the oriented and close arrangement of the ultrathin MOF NSs can avoid the restacking and guarantee the fully exposed electroactive sites. Second, the hierarchical pore structure of the electrode can not only enhance the mass transfer but also facilitate bubble dissipating in gas-generated reactions. [8] Moreover, the close and strong binding of ultrathin MOF NSs with the underlying conductive support gains more efficient electron transfer between them and guarantees the ultrahigh structural stability of the electrodes. [5a,9] However, until now, the controllable growth of different ultrathin BMNSs on various conductive substrates, especially the chemical inert substrates (such as carbon cloth (CC) and carbon fiber paper (CFP)), still remains a challenge because there are only few nucleation sites on the substrates and MOFs tend to form bulk crystals under conventional synthetic conditions. [10] Therefore, it is of great significance to develop a general and effective synthesis strategy to directly grow different ultrathin BMNSs on various conductive substrates to accelerate the practical application of MOFs in electrocatalysis.Herein, we report a general strategy to synthesize various ultrathin BMNSs arrays on different conductive substrates through the in situ transformation of presynthesized layered double hydroxides (LDHs) NSs arrays, which provide an appropriate dissolution rate of metal ions in a mixed solvent. This strategy with LDHs as precursor is adaptable to bimetal-MOFs with different organic ligands and metal ions (such as NiCo-BDC (BDC = 1,4-dicarboxybenzene), NiCo-NDC (NDC = naphthalene-2,6-dicarboxylic acid), NiCo-TDA (TDA = 2,5-thiophenedicarboxylic acid), ZnCo-BDC BMNSs) on various substrates (such as nickel foam (NF), CC, and CFP, benefiting from the multimetal tunability and flexibility of LDHs. In addition, trimetal-MOF NSs Structure engineering of ultrathin metal-organic framework (MOF) nanosheets to self-supporting and well-aligned MOF superstructures is highly desired for diverse applications, especially important for electrocatalysis. In this work, a facile layered double hydroxides in situ transformation strategy is developed to synthesize ultrathin bimetal-MOF nanosheets (BMNSs) arrays on conductive substrates. This approach is versatile, and applicable to obtain various BMNSs or even trimetal-MOF nanosheets arrays on different substrates. As a proof of concept application, the obtained ultrathin NiCo-BDC BMNSs array exhibits an excellent...
SSCI-VIDE+CARE+JSH:MPI:YDU:RCI:LTI:SRS:CGOInternational audienceOrganosulfates are tracers for secondary organic aerosol (SOA) formation. We propose a new mechanism of organosulfur product formationin the atmosphere, in which sulfur dioxide (SO2) reacts directly withalkenes. The experiments were conducted at the gas-liquid interface witha coated-wall flow tube reactor. It was shown, for the first time, thatSO2 reacts efficiently with the unsaturated bond in oleic acid underatmospheric conditions (without ozone), leading to the formation of C-9and C-18 organosulfur products. The associated uptake coefficients werein excess of 10(-6), decreasing with initial SO2 concentration andincreasing with humidity. These results might explain a fraction oforganosulfur products detected in atmospheric particles. This work tendsto elucidate the role of organosulfates' interfacial chemistry as apotentially unrecognized pathway for their contribution to SOAformation; however, it remains to be determined how significant thispathway is to the overall organosulfate abundances measured in ambientaerosol
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