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Realizing Synergistic Effect of Electronic Modulation and Nanostructure Engineering over Graphitic Carbon Nitride for Highly Efficient Visible-Light H2 Production Coupled with Benzyl Alcohol Oxidation
摘要： Photocatalytic H2 production based on g-C3N4 faces enormous challenging issues including limited visible-light absorption, poor separation and transfer abilities of photo-generated electron-hole pairs. Herein, we realize the synergistic effect of nanostructure engineering and electronic modulation with a supramolecular assembly mediated synthesis of heteroatom doped g-C3N4 hierarchical mesoporous spheres. The favorable doping site and possible effect on electronic structure are disclosed by DFT calculation with supporting experimental analysis. Impressively, S-doped g-C3N4 delivers a 13.2 times higher H2 production rate than bulk g-C3N4 under visible-light. More importantly, as the dual functional photocatalyst for H2 production and selective oxidation of benzyl alcohol, it can exhibit outstanding activity with a H2/benzaldehyde production rate of 3.76/3.87 μmol h-1, respectively. This work not only provide a new rationale for photocatalytic performance enhancement, but also shed new light on the highly efficient utilization of solar energy by coupling H2 generation with value added chemical production.
关键词： graphitic carbon nitride,hierarchical mesoporous spheres,DFT calculation,benzyl alcohol oxidation,photocatalytic hydrogen production
更新于2025-09-23 15:19:57
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Unraveling the impact of the Pd nanoparticle@BiVO <sub/>4</sub> /S-CN heterostructure on the photo-physical & opto-electronic properties for enhanced catalytic activity in water splitting and one-pot three-step tandem reaction
摘要： Pd nanoparticles embedded SBVCN-37 heterostructure photocatalyst is synthesized and employed in the water splitting reaction and for the synthesis of imines via one-pot tandem reaction involving photocatalytic reduction of nitrobenzene, oxidation of benzyl alcohol, followed by condensation reaction between them. Embedded Pd nanoparticles (mean diameter ~ 5-7 nm) act as an electron mediator and enhance the catalytic activity during oxidation and reduction reactions. Experimental results confirm that the light induced holes owing to its favourable redox potential oxidize N2H4 to N2 and liberate H+ ions that subsequently react with photogenerated electrons and facilitate the nitrobenzene reduction. The obtained quantum yield for benzyl alcohol oxidation and nitrobenzene reduction are calculated to be (2.08 %) and (6.53 %) at λ = 420 nm light illumination. The obtained apparent quantum yields for OER and HER are calculated to be 10.22 % and 12.72 % at 420 nm indicating the excellent potentiality of the presently investigated photocatalyst for solar fuel production. Photoelectrochemical (PEC) and time resolved & steady state photoluminescence measurements reveal that an optimum amount of Pd nanoparticles over SBVCN-37 is the crucial factor for achieving the highest photocurrent response, the lowest charge transfer resistance, and the efficient carrier’s mobility alteration leading to a prominent catalytic activity. Further, Mott-Schottky (M-S) analysis confirms that the deposition of Pd nanoparticles effectively reduces the over-potential and fine-tunes the band edge potential required for HER and OER reactions, independently.
关键词： Tandem Reaction,BiVO4,Benzyl Alcohol Oxidation,Apparent Quantum Yield,Nitrobenzene Reduction,g-C3N4,Photocatalytic H2 and O2 Production
更新于2025-09-19 17:15:36