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Theoretical and experimental insights into the effects of oxygen-containing species within CNTs towards triiodide reduction
摘要： Heteroatom-doped micro/nano-structured carbon materials feature unique superiorities for replacement of noble metal Pt counter electrode (CE) in dye-sensitized solar cells. Nevertheless, the effects of oxygen-containing species on/within carbon matrix on its electrocatalytic activity are seldomly considered and concerned, which will be hindered by a trade off between oxygen defects and conductivity. Herein, we present activated carbon nanotubes (P-CNTs) with abundant active edge sites and oxygen species for simultaneous achieving the activation of sidewalls and open ends. Also, the positive effects of oxygen species are decoupled by experimental data together with theoretical analysis. When capitalizing on the P-CNTs as the CE of DSSCs, the device delivers a high power conversion efficiency of 8.35% and an outstanding electrochemical stability, outperforming that of Pt reference (8.04%). The density functional theory calculation reveals that compared with the carboxylic groups, the hydroxyl groups and carbonyl groups on the surface of CNTs can greatly reduce the ionization energy of reaction, accelerate the electron transfer from external circuit to triiodide, thus being responsible for an enhanced electrocatalytic performance. This work demonstrates that a certain amount of oxygen atoms within carbon materials is also indispensable for the improvement in the reactivity of the triiodide.
关键词： Counter electrodes,Triiodide reduction,Defective carbon nanotubes,Ionization energy,Electrochemical stability,Oxygen species
更新于2025-09-23 15:23:52
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SiNW/C@Pt Arrays for High-Efficiency Counter Electrodes in Dye-Sensitized Solar Cells
摘要： Modern energy needs and the pressing issue of environmental sustainability have driven many research groups to focus on energy-generation devices made from novel nanomaterials. We have prepared platinum nanoparticle-decorated silicon nanowire/carbon core–shell nanomaterials (SiNW/C@Pt). The processing steps are relatively simple, including wet chemical etching to form the silicon nanowires (SiNWs), chemical vapor deposition to form the carbon shell, and drop-casting and thermal treatment to embed platinum nanoparticles (Pt NPs). This nanomaterial was then tested as the counter electrode (CE) in dye-sensitized solar cells (DSSCs). SiNW/C@Pt shows potential as a good electrocatalyst based on material characterization data from Raman spectroscopy and X-ray photoelectron spectroscopy (XPS). Raman spectroscopy shows that the surface reactivity of the SiNW/C is increased by the decoration of Pt NPs. These data also show that the carbon shell included both graphitic (sp2 hybridization) and defective (sp3 hybridization) phases of carbon. We achieved the minimum charge-transfer resistance of 0.025 ? · cm2 and the maximum ef?ciency of 9.46% with a symmetric dummy cell and DSSC device fabricated from the SiNW/C@Pt CEs, respectively.
关键词： core–shell,defective carbon,electrocatalytic activity,dye-sensitized solar cells (DSSCs),counter electrodes (CEs),silicon nanowires (SiNWs)
更新于2025-09-16 10:30:52