The catalytic activity of materials is highly dependent on their composition and surface structure, especially the density of low-coordinated surface atoms. In this work, we have prepared two-dimensional hexagonal FeS...The catalytic activity of materials is highly dependent on their composition and surface structure, especially the density of low-coordinated surface atoms. In this work, we have prepared two-dimensional hexagonal FeS with high-energy （001） facets （FeS-HE-001） via a solution-phase chemical method. Nanosheets （NSs） with exposed high-energy planes usually possess better reaction activity, so FeS-HE-001 was used as a counter electrode （CE） material for dye-sensitized solar ceils （DSSCs）. FeS-HE-001 achieved an average power conversion efficiency （PCE） of 8.88% （with the PCE of champion cells being 9.10%）, which was almost 1.15 times higher than that of the Pt-based DSSCs （7.73%） measured in parallel. Cyclic voltammetry and Tafel polarization measurements revealed the excellent electrocatalytic activities of FeS-HE-001 towards the I-3/I- redox reaction. This can be attributed to the promotion of photoelectron transfer, which was measured by electrochemical impedance spectroscopy and scanning Kelvin probe, and the strong I-3 adsorption and reduction activities, which were investigated using first-principles calculations. The presence of high-energy （001） facets in the NSs was an important factor for improving the catalytic reduction of I-3. We believe that our method is a promising way for the design and synthesis of advanced CE materials for energy harvesting.展开更多
基金We gratefully acknowledge the support of this research by the National Natural Science Foundation of China （Nos. 21473051 and 21371053）, Application Technology Research and Development Projects in Harbin （No. 2013AE4BW051） and International Science ＆ Technology Cooperation Program of China （No. 2014DFR41110）.
文摘The catalytic activity of materials is highly dependent on their composition and surface structure, especially the density of low-coordinated surface atoms. In this work, we have prepared two-dimensional hexagonal FeS with high-energy （001） facets （FeS-HE-001） via a solution-phase chemical method. Nanosheets （NSs） with exposed high-energy planes usually possess better reaction activity, so FeS-HE-001 was used as a counter electrode （CE） material for dye-sensitized solar ceils （DSSCs）. FeS-HE-001 achieved an average power conversion efficiency （PCE） of 8.88% （with the PCE of champion cells being 9.10%）, which was almost 1.15 times higher than that of the Pt-based DSSCs （7.73%） measured in parallel. Cyclic voltammetry and Tafel polarization measurements revealed the excellent electrocatalytic activities of FeS-HE-001 towards the I-3/I- redox reaction. This can be attributed to the promotion of photoelectron transfer, which was measured by electrochemical impedance spectroscopy and scanning Kelvin probe, and the strong I-3 adsorption and reduction activities, which were investigated using first-principles calculations. The presence of high-energy （001） facets in the NSs was an important factor for improving the catalytic reduction of I-3. We believe that our method is a promising way for the design and synthesis of advanced CE materials for energy harvesting.
