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Recently, various attempts have been made for light-to-fuels conversion, often with limited performance. Herein we report active and lasting three-factored hierarchical photocatalysts consisting of plasmon Au, ceria semiconductor, and graphene conductor for hydrogen production. The Au@CeO/Gr entity (graphene outer shell thickness of 2.0 nm) under visible-light irradiation exhibits a colossal achievement (8.0 μmol mg h), which is 2.2- and 14.3-fold higher than those of binary Au@CeO and free-standing CeO species, outperforming the currently available catalysts. Yet, it delivers a high maximum quantum yield efficiency of 38.4% at an incident wavelength of 560 nm. These improvements are unambiguously attributed to three indispensable effects: (1) the plasmon resonant energy is light-excited and transferred to produce hot electrons localizing near the surface of Au@CeO, where (2) the high-surface-area Gr conductive shell will capture them to direct hydrogen evolution reactions, and (3) the active graphene hybridized on the defect-rich surface of Au@CeO favorably adsorbs hydrogen atoms, which all bring up thorough insight into the working of a ternary Au@CeO/Gr catalyst system in terms of light-to-hydrogen conversion.
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http://dx.doi.org/10.1021/acsnano.2c00509 | DOI Listing |
ACS Catal
December 2024
Institute of Systems, Molecular and Integrative Biology, University of Liverpool, Liverpool L69 7ZB, U.K.
Synthetic photobiocatalysts are promising catalysts for valuable chemical transformations by harnessing solar energy inspired by natural photosynthesis. However, the synergistic integration of all of the components for efficient light harvesting, cascade electron transfer, and efficient biocatalytic reactions presents a formidable challenge. In particular, replicating intricate multiscale hierarchical assembly and functional segregation involved in natural photosystems, such as photosystems I and II, remains particularly demanding within artificial structures.
View Article and Find Full Text PDFSmall
December 2024
Department of Fiber Convergence Material Engineering, Dankook University, Gyeonggi-Do, 16890, Republic of Korea.
Approximately 2 billion people still lack access to clean drinking water. Extensive efforts are underway to develop semiconductor photocatalysts for water disinfection and environmental remediation, but conventional liquid-solid diphase interfacial photocatalysts face challenges like low diffusion coefficients and limited solubility of dissolved oxygen. This study introduces freestanding copper oxide fluffy pine needle structures (CO-FPNs) with tunable water pollutants-gas-solid (WGS) triple-phase interfaces that enhance oxygen enrichment and reactive oxygen species (ROS) production.
View Article and Find Full Text PDFChem Sci
December 2024
Department of Intelligent Systems, Delft University of Technology Delft 2629 HZ The Netherlands
The demand for innovative synthetic polymers with improved properties is high, but their structural complexity and vast design space hinder rapid discovery. Machine learning-guided molecular design is a promising approach to accelerate polymer discovery. However, the scarcity of labeled polymer data and the complex hierarchical structure of synthetic polymers make generative design particularly challenging.
View Article and Find Full Text PDFEnviron Sci Pollut Res Int
December 2024
Department of Organic Chemistry, Faculty of Chemistry, Alzahra University, Tehran, Iran.
The efficient utilization of light and the prolonged lifetime of photo-induced charge carriers are essential elements that contribute to superior photocatalytic activity. Yolk-shell nanostructures with porous shells and mobile cores offer significant structural advantages in achieving these goals. However, designing yolk-shell multicomponent nanocomposites with diverse architectures remains a persistent challenge.
View Article and Find Full Text PDFInorg Chem
December 2024
School of Chemistry and Chemical Engineering, Jiangsu University, Zhenjiang 212013, P. R. China.
Reasonable construction of atomically accurate photocatalysts is the key to building efficient photocatalytic systems. Herein, we propose a collective effects strategy that enables the consolidation of both cobalt single atoms (Co) and nickel nanoparticles (Ni) in hierarchical porous MOFs for the foundational features for the preparation of high-performance photocatalysts. Among them, the optimal sample Co/Al-bpydc/Ni achieved a CO generation rate of 12.
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