4.8 Article

Zwitterions in 3D Perovskites: Organosulfide-Halide Perovskites

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出版社

AMER CHEMICAL SOC
DOI: 10.1021/jacs.2c09382

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资金

  1. Brown Science Foundation
  2. Stanford Interdisciplinary Graduate Fellowship
  3. Office of Energy Efficiency and Renewable Energy (EERE)
  4. John Fell Oxford University Press (OUP) Research Fund
  5. UK Engineering and Physical Sciences Research Council (EPSRC) [EP/V010840/1]
  6. EPSRC [EP/R029431]
  7. National Science Foundation (NSF) [ECCS-1542152]
  8. DOE Office of Science [DE-AC02-06CH11357]
  9. STROBE, a NSF Science & Technology Center [DMR 1548924]
  10. Arnold O. Beckman Postdoctoral Fellowship in the Chemical Sciences
  11. Camille and Henry Dreyfus Foundation's Postdoctoral Program in Environmental Chemistry
  12. David and Lucile Packard Foundation Fellowship for Science and Engineering
  13. Camille and Henry Dreyfus Teacher-Scholar Award

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This study demonstrates the synthesis of halide perovskites using organosulfides under milder conditions, showcasing the unique properties of (CYS)PbX2 and its potential applications in tandem solar cells. The combination of A+ and X- sites with zwitterions may lead to further exploration of mixed-anion 3D hybrid perovskites in the future.
Although sulfide perovskites usually require high-temperature syntheses, we demonstrate that organosulfides can be used in the milder syntheses of halide perovskites. The zwitterionic organosulfide, cysteamine (CYS; +NH3(CH2)2S-), serves as both the X- site and A+ site in the ABX3 halide perovskites, yielding the first examples of 3D organosulfide-halide perovskites: (CYS)PbX2 (X- = Cl- or Br-). Notably, the band structures of (CYS)PbX2 capture the direct bandgaps and dispersive bands of APbX3 perovskites. The sulfur orbitals compose the top of the valence band in (CYS)PbX2, affording unusually small direct bandgaps of 2.31 and 2.16 eV for X- = Cl- and Br-, respectively, falling in the ideal range for the top absorber in a perovskite-based tandem solar cell. Measurements of the carrier dynamics in (CYS)PbCl2 suggest carrier trapping due to defects or lattice distortions. The highly desirable bandgaps, band dispersion, and improved stability of the organosulfide perovskites demonstrated here motivate the continued expansion and exploration of this new family of materials, particularly with respect to extracting photocurrent. Our strategy of combining the A+ and X- sites with zwitterions may offer more members in this family of mixed-anion 3D hybrid perovskites.

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