Scrutinizing Defects and Defect Density of Selenium‐Doped Graphene for High‐Efficiency Triiodide Reduction in Dye‐Sensitized Solar Cells

• Published in: Angewandte Chemie International Edition Vol. 57; no. 17; pp. 4682 - 4686
• Main Authors: Meng, Xiangtong, Yu, Chang, Song, Xuedan, Iocozzia, James, Hong, Jiafu, Rager, Matthew, Jin, Huile, Wang, Shun, Huang, Longlong, Qiu, Jieshan, Lin, Zhiqun
• Format: Journal Article
• Language: English
• Published: Germany Wiley Subscription Services, Inc 16.04.2018
• Edition: International ed. in English
• Subjects: Annealing; Catalysis; Catalytic activity; Chemical reduction; Defect annealing; Defects; Density; Dye-sensitized solar cells; Dyes; Efficiency; Electrocatalysts; Electrodes; Electrolytic cells; Electron transfer; Graphene; Ionization; ionization energy; Photovoltaic cells; Selenium; selenium-doped graphene; Solar cells; Temperature effects; triiodide reduction; triiodide reduction; selenium-doped graphene; ionization energy; dye-sensitized solar cells; defects
• ISSN: 1433-7851; 1521-3773
• DOI: 10.1002/anie.201801337

Understanding the impact of the defects/defect density of electrocatalysts on the activity in the triiodide (I3−) reduction reaction of dye‐sensitized solar cells (DSSCs) is indispensable for the design and construction of high‐efficiency counter electrodes (CEs). Active‐site‐enriched selenium‐doped graphene (SeG) was crafted by ball‐milling followed by high‐temperature annealing to yield abundant edge sites and fully activated basal planes. The density of defects within SeG can be tuned by adjusting the annealing temperature. The sample synthesized at an annealing temperature of 900 °C exhibited a superior response to the I3− reduction with a high conversion efficiency of 8.42 %, outperforming the Pt reference (7.88 %). Improved stability is also observed. DFT calculations showed the high catalytic activity of SeG over pure graphene is a result of the reduced ionization energy owing to incorporation of Se species, facilitating electron transfer at the electrode–electrolyte interface. Going solar: Active‐site‐enriched selenium‐doped graphene (SeG) was crafted by ball‐milling followed by high‐temperature annealing. The SeG formed at 900 °C (SeG‐900) as an electrocatalyst for DSSCs delivered a high efficiency of 8.42 %, outperforming the Pt reference (7.88 %). The high electrocatalytic activity can be ascribed to the reduced ionization energy owing to the incorporation of Se species and improved charge transfer capability.