Global GET-Future Lab & Department of Advanced Materials Chemistry, Korea University, 2511 Sejong-ro, Sejong 339-700, Korea.
Nanoscale. 2020 Jan 23;12(3):1602-1616. doi: 10.1039/c9nr09019c.
The development of a highly active, long-lasting, and cost-effective electrocatalyst as an alternative to platinum (Pt) is a vital issue for the commercialization of dye-sensitized solar cells. In this study, Ru-N-doped template-free mesoporous carbon (Ru-N-TMC) was prepared by the direct stabilization and carbonization of the poly(butyl acrylate)-b-polyacrylonitrile (PBA-b-PAN) block copolymer and ruthenium(iii) acetylacetonate [Ru(acac)3]. During the stabilization process, microphase separation occurred in the PBA-b-PAN block copolymer due to the incompatibility between the two blocks, and the PAN block transformed to N-doped semi-graphitic carbon. In the carbonization step, the PBA block was eliminated as a porous template, creating hierarchal mesopores/micropores. Meanwhile, Ru(acac)3 was decomposed to Ru, which was homogeneously distributed over the carbon substrate and anchored through N and O heteroatoms. The resulting Ru-N-TMC showed ultra-low charge transfer resistance (Rct = 0.034 Ω cm2) in the Co(bipyridine)33+/2+ reduction reaction, indicating very high electrocatalytic ability. Even though it is a transparent counter electrode (CE, average visible transmittance of 42.25%), covering a small fraction of the fluorine doped tin oxide (FTO)/glass substrate with Ru-N-TMC, it led to lower charge transfer resistance (Rct = 0.55 Ω cm2) compared to Pt (Rct = 1.00 Ω cm2). The Ru-N-TMC counter electrode exhibited a superior power conversion efficiency (PCE) of 11.42% compared to Pt (11.16%) when employed in SGT-021/Co(bpy)33+/2+ based dye-sensitized solar cells (DSSCs). Furthermore, a remarkable PCE of 10.13% and 8.64% from front and rear illumination, respectively, was obtained when the Ru-N-TMC counter electrode was employed in a bifacial DSSC. The outstanding catalytic activity and PCE of Ru-N-TMC were due to the high surface area of Ru-N-TMC, which contained numerous active species (Ru and N), easily facilitated to redox ions through the hierarchical microporous/mesoporous structure.
作为商业化染料敏化太阳能电池的替代物,开发高效、长寿命且经济实用的电催化剂是一个至关重要的问题。在本研究中,通过直接稳定和碳化聚(丁烯丙烯酯)-b-聚丙烯腈(PBA-b-PAN)嵌段共聚物和三氯化钌[Ru(acac)3]制备了 Ru-N 掺杂无模板介孔碳(Ru-N-TMC)。在稳定化过程中,由于两个嵌段之间的不兼容性,PBA-b-PAN 嵌段共聚物发生微相分离,而 PAN 嵌段转化为 N 掺杂半石墨碳。在碳化步骤中,PBA 嵌段作为多孔模板被消除,形成分级介孔/微孔。同时,Ru(acac)3 分解为 Ru,均匀分布在碳基底上,并通过 N 和 O 杂原子锚定。所得的 Ru-N-TMC 在 Co(bipyridine)33+/2+还原反应中表现出超低的电荷转移电阻(Rct=0.034 Ω cm2),表明其具有极高的电催化能力。尽管它是透明的对电极(CE,平均可见光透射率为 42.25%),仅用一小部分 Ru-N-TMC 覆盖氟掺杂氧化锡(FTO)/玻璃基底,但与 Pt(Rct=1.00 Ω cm2)相比,它导致更低的电荷转移电阻(Rct=0.55 Ω cm2)。当用于 SGT-021/Co(bpy)33+/2+基染料敏化太阳能电池(DSSCs)时,Ru-N-TMC 对电极表现出 11.42%的优异功率转换效率(PCE),优于 Pt(11.16%)。此外,当 Ru-N-TMC 对电极用于双面 DSSC 时,从前部和后部照明分别获得了 10.13%和 8.64%的显著 PCE。Ru-N-TMC 的出色催化活性和 PCE 归因于其高比表面积,其中包含大量活性物质(Ru 和 N),通过分级微孔/介孔结构,很容易促进氧化还原离子的迁移。