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Fabricating carbon nitride (g-C3N4) based photocatalysts with high visible-light utilization efficiency and rapid photogenerated carrier migration rate is crucial for the improvement of photocatalytic hydrogen production. Herein, we designed and prepared Z-scheme O-CNS/MoS2 hybrid composites via a two-step combining with ultrasound sonication method. The obtained O-CNS/MoS2 composites possessed boosting visible-light absorption capacity, revealed by the results of the diffused reflectance spectra (DRS). In contrast to bulk g-C3N4 (u-CNB) and O-CNS samples, the obtained O-CNS/MoS2 composites displayed significantly enhanced photocatalytic hydrogen behavior. Specifically, the O-CNS/MoS2 photocatalysts with 5 wt% loading of MoS2 exhibited the highest hydrogen production rate (HPR), which was respectively 26.5 and 1.97 times bigger than that of u-CNB and O-CNS sample correspondingly. This promoted photocatalytic hydrogen behavior was plausibly attributed to the synergistic effect of the porous structure, improved light absorption capacity, and enhanced photoactivated carrier migration rate. Based on comprehensive analysis, the migration and separation pathway of photoactivated carriers were proposed for interpreting the enhancement mechanism of the photocatalytic hydrogen behavior. Our work will open up an innovative strategy for the design and construction of novel g-C3N4 hybrid photocatalysts with boosting photocatalytic hydrogen production behavior. [ABSTRACT FROM AUTHOR]

Tailoring the selectivity at the electrode‐electrolyte interface is one of the greatest challenges for heterogeneous electrocatalysis, and complementary strategies to catalyst structural designs need to be developed. Herein, we proposed a new strategy of controlling the electrocatalytic pathways by lateral adsorbate interaction for the bio‐polyol oxidation. Redox‐innocent 1,1,1,3,3,3‐hexafluoro‐2‐propanol (HFIP) anion possesses the alcoholic property that facilely adsorbs on the nickel oxyhydroxide catalyst, but is resistant to oxidation due to the electron‐withdrawing trifluoromethyl groups. The alien HFIP adsorbents can compete with bio‐polyols and form a mixed adsorbate layer that creates lateral adsorbate interaction via hydrogen bonding, which achieved a >2‐fold enhancement of the oxalate selectivity to 55 % for the representative glycerol oxidation and can be extended to various bio‐polyol substrates. Through in situ spectroscopic analysis and DFT calculation on the glycerol oxidation, we reveal that the hydrogen‐bonded adsorbate interaction can effectively tune the adsorption energies and tailor the oxidation capabilities toward the targeted products. This work offers an additional perspective of tuning electrocatalytic reactions via introducing redox‐innocent adsorbates to create lateral adsorbate interactions. [ABSTRACT FROM AUTHOR]

Molecular nanotechnology promises to offer privileged access to developing NIR‐II materials with precise structural and functional manipulation for transformable theranostic applications. However, the lack of an affordable, yet general, method makes this goal currently inaccessible. By virtue of the intriguing nucleic acid chemistry, here we present an artificial base‐directed topological single‐strand DNA encoding design that enables one‐step synthesis of valence‐controlled NIR‐II molecular nanostructures and spatial assembly of these nanostructures to modulate their behaviors in living systems. As proof‐of‐concept studies, we construct ultrasmall Ag2S quantum dots and pH‐responsive, size‐tunable CuS assemblies for in vivo NIR‐II fluorescence imaging and deep tumor photothermal therapy. This work paves a new way for creating functionally diversified architectures and broadens the scope of DNA‐encoded material engineering. [ABSTRACT FROM AUTHOR]

C40H34N4O6SZn, triclinic P1̅ (no. 2), a = 11.157(2) Å, b = 11.867(2) Å, c = 14.141(3) Å, α = 75.30(3)°, β = 86.09(3)°, γ = 84.91(3)°, V = 1801.8(6) Å3, Z = 2, Rgt(F) = 0.0419, ωRref(F2) = 0.1063, T = 293(2) K.

The structure of C22H19N2O7Zn, has a triclinic(P-1) symmetry. a = 8.1731(16) Å, b = 8.7150(17) Å, c = 15.396(3) Å, α = 75.40(3)°, β = 79.26(3)°, γ = 71.82(3)°, V = 1001.3(3) Å3, Z = 2, Rgt(F) = 0.0320, wRref(F2) = 0.0768, T = 293(2) K.