Indium oxide (In2O3) is a promising semiconductor used for various photocatalytic reactions, yet the green and template-free synthesizing the different micro/nanostructured In2O3 with tunable morphology is still full of challenge. In this study, the three morphological In2O3 with 3D micro-cubelike (In2O3-MC), 3D micro-ricelike (In2O3-MR), and 2D nano-platelike (In2O3-NP) were successfully fabricated through a facile hydrothermal strategy without any organic template additives. Owing to the enlarged specific surface area, promoted charge migration rate and suitable surface oxygen vacancies density, the unique 3D ricelike In2O3-MR exhibited the best photocatalytic H2 generation activity from biomass glucose solution, which was 1.9-fold and 1.7-fold higher than that of In2O3-MC and In2O3-NP under the same experimental conditions. In addition, the optimum photoactivity of In2O3-MR was achieved under the alkaline environment with pH = 11 and 1.0 wt% Pt cocatalyst loading, which was better than the most of previously reported In2O3-based photocatalysts. Simultaneously, the possible photocatalytic mechanism for solar H2 evolution from glucose solution was also discussed. Our work will bring about potential application in preparation of other photocatalysts with controlling morphology for renewable photocatalysis. 

Facile template-free fabrication of different micro/nanostructured In2O3 for photocatalytic H2 production from glucose solution

The selective photoreduction of CO2 into hydrocarbon fuels, such as CH4, is highly desirable for sustainable energy but remains a significant challenge due to slow proton-electron transfer processes and competing intermediates. Herein, a novel NiO/MgAl-LDH (NMA-x, LDH represents layered double hydroxide) step-scheme (S-scheme) heterojunction has been engineered via in-situ anchoring MgAl-LDH nanoplates on metal–organic frameworks (MOFs) derived NiO microrods, which improves the CO2 adsorption capability and specific surface area of NiO. The steered internal electric field in the p-n heterointerface promotes charge separation and attracts a high electron density center on the catalyst surface to favor CH4 production. Meanwhile, S-scheme photogenerated charge transfer mechanism is proposed by in-situ X-ray photoelectron spectroscopy (XPS), in-situ diffuse reflectance infrared Fourier transform (DRIFT) spectra and density functional theory (DFT) calculation. In this process, photogenerated electrons are transferred from the conduction band (CB) of MgAl-LDH to the valence band (VB) of NiO, facilitating the CHO* species serve as the critical intermediate for producing CH4 through desired photocatalytic CO2 reduction. Using pure water as a proton source, the NMA-2 catalyst achieved a high CH4 selectivity of 91.2% and a yield of 8.98 μmol∙g−1∙h−1, representing significant potential for practical applications. This catalyst outperformed pristine and revitalized NiO by 4.23 and 2.07 times, respectively. 

Engineering the S-scheme heterojunction between NiO microrods and MgAl-LDH nanoplates for efficient and selective photoreduction of CO2 to CH4

Metal single-atoms (SA) are considered as an effective cocatalyst in photocatalyst for their unsaturated coordination and distinguished activity. However, the precious metal single-atoms catalyst (SACs) approach the maximum activity limit, how to further improve the catalytic efficiency is challenging. In this work, an atomic-level photocatalyst was designed to use the synergy between Pd and Cu dual-SA constructed on TiO2 surface. The synthesized PdCu/TiO2 photocatalyst achieves ultrahigh and stable photocatalytic activity with H2 production of 94.35 mmol∙g−1∙h−1 by splitting water, which is 2.65 and 2.78 times to the PdSA/TiO2 and CuSA/TiO2, respectively, which also higher than most reported photocatalysts. Furthermore, the apparent quantum efficiency (AQE) reaches 83.81 % at 365 nm. Detailed investigations indicate that the outstanding activity of PdCu/TiO2 is mainly attributed to the Pd-O-Cu dimer-site formed in the photocatalyst, which can not only effectively facilitate the photoelectrons transfer to the active site and inhibit the recombination, but also balance the H* adsorption–desorption during the photocatalytic H2 evolution (PHE) process, thus greatly promoting the splitting water reaction. This work provides a new insight for developing bimetallic SACs with high PHE efficiency. 

Cu and Pd dual-single-atoms anchored titanium dioxide for remarkable photocatalytic H2 evolution efficiency

We present CdSe@CdS nanorods coated with a redox-active polydopamine (PDA) layer functionalized with cobaloxime-derived photocatalysts for efficient solar-driven hydrogen evolution in aqueous environments. The PDA-coating provides reactive groups for the functionalization of the nanorods with different molecular catalysts, facilitates charge separation and transfer of electrons from the excited photosensitizer to the catalyst, and reduces photo-oxidation of the photosensitizer. X-ray photoelectron spectroscopy (XPS) confirms the successful functionalization of the nanorods with cobalt-based catalysts, whereas the catalyst loading per nanorod is quantified by total reflection X-ray fluorescence spectrometry (TXRF). A systematic comparison of different types of cobalt-based catalysts was carried out, and their respective performance was analyzed in terms of the number of nanorods and the amount of catalyst in each sample [turnover number, (TON)]. This study shows that the performance of these multicomponent photocatalysts depends strongly on the catalyst loading and less on the specific structure of the molecular catalyst. Lower catalyst loading is advantageous for increasing the TON because the catalysts compete for a limited number of charge carriers at the nanoparticle surface. Therefore, increasing the catalyst loading relative to the absolute amount of hydrogen produced does not lead to a steady increase in the photocatalytic activity. In our work, we provide insights into how the performance of a multicomponent photocatalytic system is determined by the intricate interplay of its components. We identify the stable attachment of the catalyst and the ratio between the catalyst and photosensitizer as critical parameters that must be fine-tuned for optimal performance. 

Screening Cobalt-based Catalysts on Multicomponent CdSe@CdS Nanorods for Photocatalytic Hydrogen Evolution in Aqueous Media

High-performance self-powered ultraviolet photodetector based on a ZnO/CuPc inorganic/organic heterojunction

The development of visible‐light‐induced photocatalysts is one of the critically important issues because it offers a green and sustainable route for solar energy conversion. Herein, In‐doped ZnO@In2O3 hybrid photocatalysts are designed and constructed through a one‐pot metal‐organic frameworks (MOFs)‐encapsulation‐derived method. The photocatalytic activity of the sample photocatalysts is systematically investigated by photocatalytic hydrogen evolution under visible light irradiation. The composition of the hybrid photocatalysts is also controlled to find the best photocatalytic activities. Interestingly, using a visible‐light irradiation source, the optimized In‐doped ZnO@In2O3 photocatalyst shows an H2 evolution rate of 417 µmol∙g−1∙h−1, which is nearly 20 times higher than that of the In‐doped ZnO sample and also exceeds most ZnO‐based catalysts ever reported. The enhanced catalytic performance is ascribed to the increased visible‐light response and enhanced charge separation efficiency by the synergistic effects of electron‐trapped In doping and electron‐donated In2O3 coupling. This work presents a promising pathway for fabricating MOFs‐encapsulation derived visible‐light‐driven composites for high photocatalytic performance towards hydrogen evolution.

One‐Pot MOFs‐Encapsulation Derived In‐Doped ZnO@In2O3 Hybrid Photocatalyst for Enhanced Visible‐Light‐Driven Photocatalytic Hydrogen Evolution

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One‐Pot MOFs‐Encapsulation Derived In‐Doped ZnO@In2O3 Hybrid Photocatalyst for Enhanced Visible‐Light‐Driven Photocatalytic Hydrogen Evolution