The photocatalytic CO reduction reaction (CRR) represents a promising route for the clean utilization of stranded renewable resources, but poor selectivity resulting from the competing hydrogen evolution reaction (HER) in aqueous solution limits its practical applicability. In the present contribution a photocatalyst with hydrophobic surfaces was fabricated. It facilitates an efficient three-phase contact of CO (gas), H O (liquid), and catalyst (solid). Thus, concentrated CO molecules in the gas phase contact the catalyst surface directly, and can overcome the mass-transfer limitations of CO , inhibit the HER because of lowering proton contacts, and overall enhance the CRR. Even when loaded with platinum nanoparticles, one of the most efficient HER promotion cocatalysts, the three-phase photocatalyst maintains a selectivity of 87.9 %. Overall, three-phase photocatalysis provides a general and reliable method to enhance the competitiveness of the CRR.
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http://dx.doi.org/10.1002/anie.201908058 | DOI Listing |
Adv Mater
November 2024
Zhejiang Key Laboratory of Petrochemical Environmental Pollution Control, Marine Science and Technology College, Zhejiang Ocean University, Zhoushan, 316004, P. R. China.
The interfacial photothermal-photocatalytic systems can generate clean water while purifying wastewater containing organic pollutants, but the impact of thermal convection on synergistic effects remains unexplored. This paper aims to regulate the thermal convection at the interface to significantly enhance the synergistic effect of interfacial photothermal-photocatalytic systems. A novel heterogeneous structure comprising iron-based metal-organic frameworks and multi-walled carbon nanotubes with a gelatin-polyvinyl alcohol (PVA) double network hydrogel (MWCNTs@NM88B/PVA/gelatin hydrogel, denoted as MMH) is developed and employed in the construction of the solar-driven interfacial evaporation (SIE) system.
View Article and Find Full Text PDFNanoscale
December 2024
Department of Quantum System Engineering, Jeonbuk National University, Republic of Korea.
This review delves into the latest advancements in controlling three-phase boundaries (TPBs) in photocatalytic systems, with a focus on photo(electro)catalytic processes for nitrogen reduction, oxygen reduction, and water reduction. We critically analyze various strategies and advanced materials designed to enhance TPB performance, evaluating their impact on catalytic efficiency and identifying gaps in the existing literature. By examining sophisticated triphasic systems that integrate superwetting materials, we emphasize their essential role in improving light absorption, charge separation, and mass transfer.
View Article and Find Full Text PDFACS Appl Mater Interfaces
November 2024
Key Laboratory of Applied Surface and Colloid Chemistry, Ministry of Education, Xi'an Key Laboratory of Organometallic Material Chemistry, Xi'an Key Laboratory of Polymeric Soft Matter, School of Chemistry and Chemical Engineering, Shaanxi Normal University, Xi'an 710119, P. R. China.
Modification of g-CN with metal-free biomaterials through an environmentally friendly, low-energy, facile, and rapid single-step method is desired for the preparation of photocatalysts with efficient activity and high selectivity of CO reduction but remains a great challenge. Herein, we develop a phase-transitioned protein modification strategy for photocatalysts through superfast amyloid-like protein assembly on surfaces using a one-step sequential coating method. Metal-free carbon nitride/protein heterojunction composite photocatalysts (the phase-transitioned lysozyme (PTL), phase-transitioned bovine serum albumin (PTB), and phase-transitioned ovalbumin (PTO)-coated carbon nitride@SiO (CN@SiO) and bioinspired carbon nitride hollow nanospheres (CN-HS) obtained by etching of CN@SiO) are prepared using lysozyme, bovine serum albumin, and ovalbumin.
View Article and Find Full Text PDFChem Sci
August 2024
MIIT Key Laboratory of Semiconductor Microstructure and Quantum Sensing, Engineering Research Center of Semiconductor Device Optoelectronic Hybrid Integration in Jiangsu Province, Nanjing University of Science and Technology Nanjing 210094 P. R. China
The conversion of CO and HO into ethanol with high selectivity photocatalysis is greatly desired for effective CO resource utilization. However, the sluggish and challenging C-C coupling hinders this goal, with the behavior of *CO holding the key. Here, a nanoconfined and tandem three-phase reaction system is established to simultaneously enhance the *CO concentration and interaction time, achieving an outstanding ethanol selectively of 94.
View Article and Find Full Text PDFJ Colloid Interface Sci
December 2024
School of Mechanical and Manufacturing Engineering, University of New South Wales, Sydney, NSW 2052, Australia. Electronic address:
Prospective photocatalytic ammonia synthesis process has received more attentions but quite challenging with the low visible light utilization and weak N molecule absorption ability around the photocatalysts. Herein, interface reconstruction of MXene-TiC/CeO composites with high-concentration active sites through the carbon-doped process are presented firstly, and obvious transition zones with the three-phase reaction interface are formed in the as-prepared catalysts. The optimal co-doped sample demonstrates an excellent photo response in the visible light region, the strongest chemisorption activity and the most active sites.
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