It has been a long-standing demand to design hetero-nanostructures for charge-flow steering in semiconductor systems. Multi-component nanocrystals exhibit multifunctional properties or synergistic performance, and are thus attractive materials for energy conversion, medical therapy, and photoelectric catalysis applications. Herein we report the design and synthesis of binary and ternary multi-node sheath hetero-nanorods in a sequential chemical transformation procedure. As verified by first-principles simulations, the conversion from type-I ZnS-CdS heterojunction into type-II ZnS-(CdS/metal) ensures well-steered collections of photo-generated electrons at the exposed ZnS nanorod stem and metal nanoparticles while holes at the CdS node sheaths, leading to substantially improved photocatalytic hydrogen-evolution performance.
It has been along-standing demand to design heteronanostructures for charge-flow steering in semiconductor systems.Multi-component nanocrystals exhibit multifunctional properties or synergistic performance,a nd are thus attractive materials for energy conversion, medical therapy, and photoelectric catalysis applications.Herein we report the design and synthesis of binary and ternary multi-node sheath heteronanorods in as equential chemical transformation procedure. As verified by first-principles simulations,the conversion from type-I ZnS-CdS heterojunction into type-II ZnS-(CdS/metal) ensures well-steered collections of photo-generated electrons at the exposed ZnS nanorod stem and metal nanoparticles while holes at the CdS node sheaths,l eading to substantially improved photocatalytic hydrogen-evolution performance.Atn anoscale,m aterial shape and composition directly influence function.[1] Fabricating multiple components in as ingle nanosystem has recently attracted great interest as result of the multifunctional properties or synergistic performance induced by heterointerfaces of the nanostructure.[2]Multi-component nanocrystals (hetero-nanostructures) with heterojunctions,a llowing electron and hole transport and confinement to be controlled independently,form the basis of several optoelectronic applications.[3] Type-II heterojunctions, enabling accumulation of opposite charges at two sides,allow efficient electron-hole separation for optoelectronic applications.T he development of hybrid nanostructures increases the level of structural-architectural sophistication.[4] The colloidal technique,b enefitting from adjusting the energy of solution/solid interface induced by various ligands,p romotes the synthesis of elaborate hetero-nanostructures in the solution.[5]Cation exchange strategy has proven to be particularly powerful for accessing the nanocrystals which are difficult to obtain by direct hot-injection synthetic methods.[6] In particular, the partial cation-exchange reaction, which circumvents separate nucleation and transfers aportion of the nanocrystal into an ew composition, is av ersatile method to prepare heterostructured ionic nanocrystals.[7] To date,s everal heterostructured nanocrystals based on wurtize (WZ) cadmium chalcogenide have been prepared by partial cation exchange.[8] Nevertheless,t od evelop ag eneral and summative partial-exchange strategy for the synthesis of novel and well-defined multi-component metal sulfide nanocrystals remains elusive.F urthermore,t he construction of more sophisticated colloidal hetero-nanostructures with targeted performance requires ahigh degree of synthetic ingenuity and creativity.Herein, we constructed unique one-dimensional (1D) binary -[S1-S2]-S1-[S1-S2]-S1-and ternary -[S1-(S2/M)]-S1-[S1-(S2/M)]-S1-hetero-nanorods with segmented node sheaths S2 decorated by M( S1 = ZnS;S 2= CdS;M = Au, Pd, Pt) through the colloidal technique.T he ternary hybrids were prepared by the post-synthetic modification of binary multi-node sheath -[ZnS-CdS]-ZnS-[ZnS-C...
A 3D organic-inorganic hybrid compound, (2-MepyH)3[{Fe(1,10-phen)3}3][{Pr4Sb12O18(OH)Cl(11.5)}(TDC)(4.5)({Pr4Sb12O18(OH)Cl(9.5)} Cl)]·3(2-Mepy)·28H2O (1; 2-Mepy=2-methylpyridine, 1,10-phen=1,10-phenanthroline, H2TDC=thiophene-2,5-dicarboxylic acid), was hydrothermally synthesized and structurally characterized. Unusually, two kinds of high-nuclearity clusters, namely [(Pr4Sb12O18(OH)Cl11)(COO)5](5-) and [(Pr4Sb12O18(OH)Cl9)Cl(COO)5](4-), coexist in the structure of compound 1; two of the latter clusters are doubly bridged by two μ2-Cl(-) moieties to form a new centrosymmetric dimeric cluster. An unprecedented spontaneous and reversible single-crystal-to-single-crystal transformation was observed, which simultaneously involved a notable organic-ligand movement between the metal ions and an alteration of the bridging ion in the dimeric cluster, induced by guest-release/re-adsorption, thereby giving rise to the interconversion between compound 1 and the compound (2-MepyH)3[{Fe(1,10-phen)3}3][{Pr4Sb12O18(OH)Cl(11.5)}(TDC)4({Pr4Sb12O18Cl(10.5)(TDC)(0.5)(H2O)(1.5)}O(0.5))]·25H2O (1'). The mechanism of this transformation has also been discussed in great detail. Photocatalytic H2-evolution activity was observed for compound 1' under UV light with Pt as a co-catalyst and MeOH as a sacrificial electron donor.
Metal nanoparticles decorate the segmented node sheaths of a unique 1D ternary hetero‐nanorod [structure shown in the picture; nanorod: ZnS (Zn blue, S yellow); node sheaths: CdS (Cd orange); nanoparticles: gold (Au purple)]. In their Communication on J. Jiang, S.‐H. Yu, and co‐workers show how this system is constructed by a sequential chemical‐transformation strategy and that this arrangement enables steered charge flow for electron–hole separation and hence efficient photocatalysis.
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