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Tailoring Grain Boundary Chemistry of Polymeric Carbon Nitride for Enhanced Solar H2 Production and CO2 Reduction
摘要： Photocatalytic water splitting is a promising and clean way to mimic the plant photosynthesis in a sustainable manner. Improvements of the quantum efficiency and optical absorption in the relevant range are certainly the further steps to approach practicality. Here, we reported that these issues can be readily addressed when 5-aminotetrazole, a monomer with still higher nitrogen content, is used for the synthesis of carbon nitride. The molten salt mixture NaCl/KCl is used as a high temperature solvent to tailor the grain boundary structure and chemistry. Visible light quantum efficiency for H2 production of 0.65 could be obtained in the presence of K2HPO4 as double layer modifier. This value is very high, considering that this number is a convolute of light to charge couple conversion, charge localization, as well as a successful oxidation and reduction reaction.
关键词： H2 production,Grain boundary,Polymeric carbon nitride,Photocatalysis,Salt melt
更新于2025-09-23 15:22:29
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Tailoring Grain Boundary Chemistry of Polymeric Carbon Nitride for Enhanced Solar H2 Production and CO2 Reduction
摘要： Photocatalytic water splitting is a promising and clean way to mimic the plant photosynthesis in a sustainable manner. Improvements of the quantum efficiency and optical absorption in the relevant range are certainly the further steps to approach practicality. Here, we reported that these issues can be readily addressed when 5-aminotetrazole, a monomer with still higher nitrogen content, is used for the synthesis of carbon nitride. The molten salt mixture NaCl/KCl is used as a high temperature solvent to tailor the grain boundary structure and chemistry. Visible light quantum efficiency for H2 production of 0.65 could be obtained in the presence of K2HPO4 as double layer modifier. This value is very high, considering that this number is a convolute of light to charge couple conversion, charge localization, as well as a successful oxidation and reduction reaction.
关键词： Grain boundary,Salt melt,Photocatalysis,H2 production,Polymeric carbon nitride
更新于2025-09-23 15:22:29
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Direct functionalization of methane into ethanol over copper modified polymeric carbon nitride via photocatalysis
摘要： Direct valorization of methane to its alcohol derivative remains a great challenge. Photocatalysis arises as a promising green strategy which could exploit hydroxyl radical (·OH) to accomplish methane activation. However, both the excessive ·OH from direct H2O oxidation and the neglect of methane activation on the material would cause deep mineralization. Here we introduce Cu species into polymeric carbon nitride (PCN), accomplishing photocatalytic anaerobic methane conversion for the first time with an ethanol productivity of 106 μmol gcat?1 h?1. Cu modified PCN could manage generation and in situ decomposition of H2O2 to produce ·OH, of which Cu species are also active sites for methane adsorption and activation. These features avoid excess ·OH for overoxidation and facilitate methane conversion. Moreover, a hypothetic mechanism through a methane-methanol-ethanol pathway is proposed, emphasizing the synergy of Cu species and the adjacent C atom in PCN for obtaining C2 product.
关键词： methane conversion,photocatalysis,polymeric carbon nitride,ethanol production,copper modification
更新于2025-09-19 17:15:36