Enzyme-inspired single-atom photocatalysis for oxygen reduction to hydrogen peroxide

. 2025 Dec 07 ; 16 (1) : 10949. [epub] 20251207

Status PubMed-not-MEDLINE Jazyk angličtina Země Velká Británie, Anglie Médium electronic

Typ dokumentu časopisecké články

Perzistentní odkaz   https://www.medvik.cz/link/pmid41354741
Odkazy

PubMed 41354741
PubMed Central PMC12686429
DOI 10.1038/s41467-025-67189-3
PII: 10.1038/s41467-025-67189-3
Knihovny.cz E-zdroje

Photocatalysis presents a promising route for generating sustainable, high-energy-density fuels. However, conventional photocatalysts based on rigid binary metal compounds face significant limitations, including fixed band gaps, rapid charge recombination, and non-specific reaction pathways - ultimately leading to limited selectivity and yield. Critically, they lack the site-specific selectivity characteristic of enzymatic systems, a feature essential for achieving high efficiency, control, and precision. Inspired by cytochrome c oxidase, we report the development of Cu-single-atom-enhanced carbon dots as the enzymatic-like photocatalyst. By mimicking enzyme´s site-specific electron transfer cascade, these carbon dots enable the selective photocatalytic reduction of oxygen to hydrogen peroxide under ambient conditions. This study introduces a strategy for translating enzymatic precision into photocatalytic materials design, bridging molecular and materials catalysis for sustainable energy and chemical transformations.

Zobrazit více v PubMed

Yin, J., Molini, A. & Porporato, A. Impacts of solar intermittency on future photovoltaic reliability. PubMed DOI PMC

Dogutan, D. K. & Nocera, D. G. Artificial photosynthesis at efficiencies greatly exceeding that of natural photosynthesis. PubMed DOI

Tao, X., Zhao, Y., Wang, S., Li, C. & Li, R. Recent advances and perspectives for solar-driven water splitting using particulate photocatalysts. PubMed DOI

Pastor, E. et al. Electronic defects in metal oxide photocatalysts. DOI

Li, X.-B., Tung, C.-H. & Wu, L.-Z. Semiconducting quantum dots for artificial photosynthesis. DOI

Wu, Q. et al. A metal-free photocatalyst for highly efficient hydrogen peroxide photoproduction in real seawater. PubMed DOI PMC

He, B. et al. Cooperative coupling of H PubMed DOI

He, Y. et al. Efficient photocatalytic H DOI

Li, X. et al. Boosting photocatalytic H DOI

Sun, M. et al. Bifunctional Pd-Ox Center at the liquid–solid–gas triphase interface for H DOI

Zhang, X. et al. Enhancing photocatalytic H PubMed DOI PMC

Qiu, J. et al. COF/In PubMed DOI

Yue, J. Y. et al. Phenanthridine-based covalent organic frameworks for boosting overall solar H PubMed

Yan, H. et al. Enhancing photosynthesis efficiency of hydrogen peroxide by modulating side chains to facilitate water oxidation at low-energy barrier sites. PubMed DOI

Shiraishi, Y. et al. Resorcinol-formaldehyde resins as metal-free semiconductor photocatalysts for solar-to-hydrogen peroxide energy conversion. PubMed DOI

Li, Z. et al. Dipole field in nitrogen-enriched carbon nitride with external forces to boost the artificial photosynthesis of hydrogen peroxide. PubMed DOI PMC

Liu, W. et al. Unraveling the mechanism on ultrahigh efficiency photocatalytic H DOI

Teng, Z. et al. Atomically dispersed antimony on carbon nitride for the artificial photosynthesis of hydrogen peroxide. DOI

Pelicano, C. M. et al. Rational design of a carbon/potassium poly(heptazine imide) heterojunction for enhanced photocatalytic H DOI

Chi, W. et al. A photocatalytic redox cycle over a polyimide catalyst drives efficient solar-to-H PubMed DOI PMC

Yu, W. et al. Photocatalytic hydrogen peroxide evolution: what is the most effective strategy?

Ishigami, I. et al. Structural insights into functional properties of the oxidized form of cytochrome c oxidase. PubMed DOI PMC

Kolbe, F. et al. Cryo-EM structures of intermediates suggest an alternative catalytic reaction cycle for cytochrome c oxidase. PubMed DOI PMC

Ethordevic, L., Arcudi, F., Cacioppo, M. & Prato, M. A multifunctional chemical toolbox to engineer carbon dots for biomedical and energy applications. PubMed DOI

Zdražil, L. et al. Magnetic polaron states in photoluminescent carbon dots enable hydrogen peroxide photoproduction. PubMed DOI

Han, W. et al. Surface engineered carbon quantum dots for efficient photocatalytic hydrogen peroxide production.

Gu, M. et al. Solar-to-hydrogen peroxide conversion of photocatalytic carbon dots with anthraquinone: unveiling the dual role of surface functionalities.

Xia, C. et al. General synthesis of single-atom catalysts with high metal loading using graphene quantum dots. PubMed DOI

Ganjkhanlou, Y. et al. Dual fluorescence in glutathione-derived carbon dots revisited. PubMed DOI PMC

Auwarter, W., Ecija, D., Klappenberger, F. & Barth, J. V. Porphyrins at interfaces. PubMed DOI

Pan, L., Sun, S., Zhang, L., Jiang, K. & Lin, H. Near-infrared emissive carbon dots for two-photon fluorescence bioimaging. PubMed DOI

Xiong, Y., Schneider, J., Ushakova, E. V. & Rogach, A. L. Influence of molecular fluorophores on the research field of chemically synthesized carbon dots. DOI

Ghorai, N. et al. Ultrafast insights into full-colour light-emitting C-Dots. PubMed DOI

Sayyad, U. S., Bhatt, H., Ghosh, H. N. & Mondal, S. Delineating the core and surface state heterogeneity of carbon dots during electron transfer. PubMed DOI

Cadranel, A. et al. Screening supramolecular interactions between carbon nanodots and porphyrins. PubMed DOI

Scharl, T. et al. Fine-tuning the assemblies of carbon nanodots and porphyrins. PubMed DOI

Scharl, T. et al. Charge transfer in graphene quantum dots coupled with tetrathiafulvalenes. PubMed DOI

Ferrer-Ruiz, A. et al. Assessing the photoinduced electron-donating behavior of carbon nanodots in nanoconjugates. PubMed

He, Y., Liu, S., Priest, C., Shi, Q. & Wu, G. Atomically dispersed metal-nitrogen-carbon catalysts for fuel cells: advances in catalyst design, electrode performance, and durability improvement. PubMed DOI

Liang, H. W. et al. Molecular metal-Nx centres in porous carbon for electrocatalytic hydrogen evolution. PubMed DOI PMC

Hall, M. N., Lee, M., Root, T. W., Davies, H. M. L. & Stahl, S. S. Heterogeneous Fe-N-C catalyst for aerobic dehydrogenation of hydrazones to diazo compounds used for carbene transfer. PubMed DOI PMC

Heppe, N. et al. Applying nuclear forward scattering as in situ and operando tool for the characterization of FeN(4) moieties in the hydrogen evolution reaction. PubMed DOI PMC

Fu, R. et al. XPS study of copper-doped carbon aerogels. DOI

Saha, P., Amanullah, S., Barman, S. & Dey, A. Electrochemical reduction of CO PubMed

Agrachev, M. et al. Electron paramagnetic resonance spectroscopy for the analysis of single-atom catalysts.

Ding, Y. et al. Emerging semiconductors and metal-organic-compounds-related photocatalysts for sustainable hydrogen peroxide production. DOI

Pellegrin, Y. & Odobel, F. Sacrificial electron donor reagents for solar fuel production. DOI

Bakandritsos, A. et al. Mixed-valence single-atom catalyst derived from functionalized graphene. PubMed DOI

Kalytchuk, S. et al. Carbon dots detect water-to-ice phase transition and act as alcohol sensors via fluorescence turn-off/on mechanism. PubMed DOI

Buettner, G. R. Spin trapping: ESR parameters of spin adducts. PubMed DOI

Freese, T., Meijer, J. T., Feringa, B. L. & Beil, S. B. An organic perspective on photocatalytic production of hydrogen peroxide. DOI

Prescott, C. & Bottle, S. E. Biological relevance of free radicals and nitroxides. PubMed DOI

Sadowska-Bartosz, I. & Bartosz, G. The cellular and organismal effects of nitroxides and nitroxide-containing nanoparticles. PubMed DOI PMC

Yu, Y. et al. Carbon dots based photoinduced reactions: advances and perspective. PubMed DOI PMC

Macairan, J. R., Jaunky, D. B., Piekny, A. & Naccache, R. Intracellular ratiometric temperature sensing using fluorescent carbon dots. PubMed DOI PMC

Arcudi, F. et al. Porphyrin antennas on carbon nanodots: excited state energy and electron transduction. PubMed DOI

Joseph et al. Long-lived charge carrier photogeneration in a cooperative supramolecular double-cable polymer. PubMed PMC

van Stokkum, I. H., Larsen, D. S. & van Grondelle, R. Global and target analysis of time-resolved spectra. PubMed DOI

Mullen, K. M. & Stokkum, I. H. M. v. TIMP: AnRPackage for modeling multi-way spectroscopic measurements.

Snellenburg, J. J., Laptenok, S. P., Seger, R., Mullen, K. M. & Stokkum, I. H. M. v. Glotaran: AJava-Based Graphical User Interface for theRPackageTIMP.

Jančík-Procházková, A. et al. Precision engineering of nanorobots: toward single atom decoration and defect control for enhanced microplastic capture. DOI

Stoll, S. & Schweiger, A. EasySpin, a comprehensive software package for spectral simulation and analysis in EPR. PubMed DOI

Queffelec, C. et al. Investigation of copper oxidation states in plasmonic nanomaterials by XAS and Raman spectroscopy. PubMed DOI

Ankudinov, A. L., Ravel, B., Rehr, J. J. & Conradson, S. D. Real-space multiple-scattering calculation and interpretation of x-ray-absorption near-edge structure. DOI

Senge, M. O. & Kalisch, W. W. Synthesis and structural characterization of nonplanar tetraphenylporphyrins and their metal complexes with graded degrees of beta-ethyl substitution. PubMed DOI

Zong, S. et al. Structure of the intact 14-subunit human cytochrome c oxidase. PubMed DOI PMC

Margraf, J. T., Strauss, V., Guldi, D. M. & Clark, T. The electronic structure of amorphous carbon nanodots. PubMed DOI

Najít záznam

Citační ukazatele

Pouze přihlášení uživatelé

Možnosti archivace

Nahrávání dat ...