Faced with the new stage of water oxidation by molecular catalysts (MCs) in artificial photosynthesis to overcome the bottle neck issue, the "Photon-flux density problem of sunlight," a two-electron oxidation process forming HO in place of the conventional four-electron oxidation evolving O has attracted much attention. The molecular characteristics of tin(IV)-tetrapyridylporphyrin (SnTPyP), as one of the most promising MCs for the two-electron water oxidation, has been studied in detail. The protolytic equilibria among nine species of SnTPyP, with eight p values on the axial ligands' water molecules and peripheral pyridyl nitrogen atoms in both the ground and excited states, have been clarified through the measurements of UV-vis, fluorescence, H NMR, and dynamic fluorescence decay behaviour. The oxidation potentials in the Pourbaix diagram and spin densities by DFT calculation of the one-electron oxidized form of each nine species have predicted that the fully deprotonated species ([SnTPyP(O)]) and the singly deprotonated one ([SnTPyP(OH)(O)]) serve as the most favourable MCs for visible light-induced two-electron water oxidation when they are adsorbed on TiO for H formation or SnO for Z-scheme CO reduction in the molecular catalyst sensitized system of artificial photosynthesis.
Download full-text PDF |
Source |
|---|---|
| http://www.ncbi.nlm.nih.gov/pmc/articles/PMC9963784 | PMC |
| http://dx.doi.org/10.3390/molecules28041882 | DOI Listing |
Publication Analysis
Top Keywords
Similar Publications
Growing in red: impact of different light spectra and lighting conditions on lentil microgreens growth in vertical farming.
Front Plant Sci
December 2024
Laboratory of Advanced Studies in Vertical Agriculture, Goiano Federal Institute of Education, Science and Technology, Rio Verde, Brazil.
Vertical Farming Systems (VFS) emerge as an approach to optimize plant growth in urban and controlled environments, by enabling sustainable and intensive production in reduced spaces. VFS allow for greater control over growing conditions, such as light, temperature and humidity, resulting in higher quality crops and with less use of resources, such as water and fertilizers. This research investigates the effects of different lighting regimes (Constant and Gaussian) and spectral qualities (white, RBW, blue and red) on the growth, photosynthesis, and biomass accumulation of lentil microgreens () in VFS.
View Article and Find Full Text PDFCarbon nitride caught in the act of artificial photosynthesis.
Nat Commun
January 2025
Max Planck Institute of Colloids and Interfaces, Colloid Chemistry Department, Am Mühlenberg 1, 14476, Potsdam, Germany.
Covalent semiconductors of the carbon nitride family are among the most promising systems to realize "artificial photosynthesis", that is exploiting synthetic materials which use sunlight as an energy source to split water into its elements or converting CO into added value chemicals. However, the role of surface interactions and electronic properties on the reaction mechanism remain still elusive. Here, we use in-situ spectroscopic techniques that enable monitoring surface interactions in carbon nitride under artificial photosynthetic conditions.
View Article and Find Full Text PDFFloatable artificial leaf to couple oxygen-tolerant CO conversion with water purification.
Nat Commun
January 2025
Key Laboratory of Photochemistry, Institute of Chemistry Chinese Academy of Sciences, Beijing National Laboratory for Molecular Sciences, Beijing, PR China.
To enable open environment application of artificial photosynthesis, the direct utilization of environmental CO via an oxygen-tolerant reductive procedure is necessary. Herein, we introduce an in situ growth strategy for fabricating two-dimensional heterojunctions between indium porphyrin metal-organic framework (In-MOF) and single-layer graphene oxide (GO). Upon illumination, the In-MOF/GO heterostructure facilitates a tandem CO capture and photocatalytic reduction on its hydroxylated In-node, prioritizing the reduction of dilute CO even in the presence of air-level O.
View Article and Find Full Text PDFTracking the correlation between spintronic structure and oxygen evolution reaction mechanism of cobalt-ruthenium-based electrocatalyst.
Nat Commun
January 2025
State Key Laboratory of Fine Chemicals, Frontiers Science Center for Smart Materials Oriented Chemical Engineering, School of Chemical Engineering, Dalian University of Technology, Dalian, China.
Regulating the spintronic structure of electrocatalysts can improve the oxygen evolution reaction performance efficiently. Nonetheless, the effects of tuning the spintronic structure for the oxygen evolution reaction mechanisms have rarely been discussed. Here, we show a ruthenium-cobalt-tin oxide with optimized spintronic structure due to the quantum spin interaction of Ru and Co.
View Article and Find Full Text PDFIn Situ Integration of Metallic Catalytic Sites and Photosensitive Centers within Covalent Organic Frameworks for the Enhanced Photocatalytic Reduction of CO.
Small
January 2025
State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou, Fujian, 350002, P. R. China.
Covalent organic frameworks (COFs) are a promising platform for heterogeneous photocatalysis due to their stability and design diversity, but their potential is often restricted by unmanageable targeted excitation and charge transfer. Herein, a bimetallic COF integrating photosensitizers and catalytic sites is designed to facilitate locally ultrafast charge transfer, aiming to improve the photocatalytic reduction of CO. The strategy uses a "one-pot" method to synthesize the bimetallic COF (termed PBCOF) through in situ Schiff-base condensation of Pyrene with MBpy (M = Ru, Re) units.
View Article and Find Full Text PDFWant AI Summaries of new PubMed Abstracts delivered to your In-box?
Enter search terms and have AI summaries delivered each week - change queries or unsubscribe any time!