The surface electron density significantly affects the photocatalytic efficiency, especially the photocatalytic CO2 reduction reaction, which involves multi-electron participation in the conversion process. Herein, we propose a conceptually different mechanism for surface electron density modulation based on the model of Au anchored CdS. We firstly manipulate the direction of electron transfer by regulating the vacancy types of CdS. When electrons accumulate on vacancies instead of single Au atoms, the adsorption types of CO2 change from physical adsorption to chemical adsorption. More importantly, the surface electron density is manipulated by controlling the size of Au nanostructures. When Au nanoclusters downsize to single Au atoms, the strong hybridization of Au 5d and S 2p orbits accelerates the photo-electrons transfer onto the surface, resulting in more electrons available for CO2 reduction. As a result, the product generation rate of AuSA/Cd1-xS manifests a remarkable at least 113-fold enhancement compared with pristine Cd1-xS.

/pdf/modulating-electron-density-of-vacancy-site-by-single-au-2yt3dvk4oz.pdf

Modulating electron density of vacancy site by single Au atom for effective CO2 photoreduction

Rational design hybrid nanostructure photocatalysts with efficient charge separation and transfer, and good solar light harvesting ability have critical significance for achieving high solar‐to‐chemical conversion efficiency. Here a highly active and stable composite photocatalyst is reported by integrating ultrathin ZnIn2S4 nanosheets on surface of hollow CdS cube to form the cube‐in‐cube structure. Experimental results combined with density functional theory calculations confirm that the Z‐scheme ZnIn2S4/CdS heterojunction is formed, which highly boosts the charge separation and transfer under the local‐electric‐field at semiconductor/semiconductor interface, and thus prolongs their lifetimes. Moreover, such a structure affords the highly enhanced light‐harvesting property. The optimized ZnIn2S4/CdS nanohybrids exhibit superior H2 generation rate under visible‐light irradiation (λ ≥ 420 nm) with excellent photochemical stability during 20 h continuous operation.

Constructing Direct Z‐Scheme Heterostructure by Enwrapping ZnIn2S4 on CdS Hollow Cube for Efficient Photocatalytic H2 Generation

Stacking Engineering of Semiconductor Heterojunctions on Hollow Carbon Spheres for Boosting Photocatalytic CO2 Reduction

Spatial distribution of ZnIn2S4 nanosheets on g-C3N4 microtubes promotes photocatalytic CO2 reduction

The hollow core–shell Co 9 S 8 @ZnIn 2 S 4 /CdS nanoreactors are fabricated by growing ZnIn 2 S 4 nanosheets and CdS quantum dots on hollow Co 9 S 8 nanocages for photocatalytic CO 2 reduction and H 2 generation. Because of unique structural and compositional advantages, Co 9 S 8 @ZnIn 2 S 4 /CdS exhibits a significant photocatalytic BPA degradation of 90.62%, CO production of 82.10 μmol g −1 h −1 , and H 2 evolution rate up to 1419.14 μmol g −1 h −1 . Excellent photocatalytic performances are attributed to unique core-shell architecture, which can improve the scattering and refraction efficiency of incident light, and the separation and migration of photoinduced carriers. Furthermore, Co 9 S 8 @ZnIn 2 S 4 /CdS possesses a broad absorption spectrum facilitating outstanding photothermal performance. The photocatalytic mechanism for the nanoreactor has been discussed in detail. • The hollow core-shell CoS@ZIS/CdS nanoreactor is successfully prepared. • The hollow structure promotes multiple reflections and fast mass transfer. • The nanoreactor displays obvious broad spectrum response and photothermal effect. • The energy band and internal electric field are verified by simulated calculations. • It shows excellent photocatalytic CO 2 reduction and H 2 evolution efficiencies. 

Hollow Core−Shell Co9S8@ZnIn2S4/CdS Nanoreactor for Efficient Photothermal Effect and CO2 Photoreduction

Metal sulfide based materials as photocatalysts for energy conversion are essential to produce value-added chemical fuels, but their intrinsically slow carrier dynamics and low activity are yet to be resolved. Herein, we developed a unique heterogeneously nanostructured ZnIn2S4-CdS heterostructure that involves zero-dimensional (0D) CdS quantum dots uniformly confined on three-dimensional (3D) ZnIn2S4 nanoflowers, which achieves an excellent catalytic performance of CO2 photoconversion under visible-light irradiation. The obtained hierarchical heterostructure can significantly enhance the light harvesting, shorten the migration distance of carriers, and obviously accelerate the transport of electrons. As evidenced by the ultrafast transient absorption spectroscopy, the formed interface can effectively facilitate charge separation and transport. This work opens up a new avenue to carefully design the elaborate heterostructures for achieving optimal charge separation efficiency by lowering interfacial kinetic barriers and energy losses at the interface.

A hierarchical heterostructure of CdS QDs confined on 3D ZnIn2S4 with boosted charge transfer for photocatalytic CO2 reduction

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A hierarchical heterostructure of CdS QDs confined on 3D ZnIn2S4 with boosted charge transfer for photocatalytic CO2 reduction