Research Article


2021, 14(11): 4025–4032


Tuned single atom coordination structures mediated by polarization force and sulfur anions for photovoltaics

Hongyu Jing1,2,§, Zhengyan Zhao1,§, Chunyang Zhang1, Wei Liu1, Danyang Wu1, Chao Zhu3 (✉), Ce Hao1, Jiangwei Zhang4 (✉), and Yantao Shi1 (✉)

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1 State Key Laboratory of Fine Chemicals, Department of Chemistry, School of Chemical Engineering, Dalian University of Technology, Dalian 116024, China
2 Department of Chemistry, Tsinghua University, Beijing 100084, China
3 SEU-FEI Nano-Pico Center, Key Laboratory of MEMS of Ministry of Education, Collaborative Innovation Center for Micro/Nano Fabrication, Device and System, Southeast University, Nanjing 210096, China
4 State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China
§ Hongyu Jing and Zhengyan Zhao contributed equally to this work

Keywords: inorganic sulfur ions, coordination structure regulating, anti-sintering, dye-sensitized solar cells
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Impeding high temperature sintering is challengeable for synthesis of carbon-supported single-atom catalysts (C-SACs), which requires high-cost precursor and strictly-controlled procedures. Herein, by virtue of the ultrastrong polarity of salt melts, sintering of metal atoms is effectively suppressed. Meanwhile, doping with inorganic sulfur anions not only produces sufficient anchoring sites to achieve high loading of atomically dispersed Co up to 13.85 wt.%, but also enables their electronic and geometric structures to be well tuned. When served as a cathode catalyst in dye-sensitized solar cells, the C-SAC with Co-N4-S2 moieties exhibits high activity towards the iodide reduction reaction (IRR), achieving a higher power conversion efficiency than that of conventional Pt counterpart. Density function theory (DFT) calculations revealed that the superior IRR activity was ascribed to the unique structure of Co-N4-S2 moieties with lower reaction barriers and moderate binding energy of iodine on the Co center, which was beneficial to I2 dissociation.
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Tuned single atom coordination structures mediated by polarization force and sulfur anions for photovoltaics. Nano Res. 2021, 14(11): 4025–4032

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