Bandgap Tunable Ternary Cd <sub/><i>x</i> </sub> Sb <sub/> 2– <i>y</i> </sub> S <sub/>3?δ</sub> Nanocrystals for Solar Cell Applications

摘要： We report the synthesis and photovoltaic performance of a new nonstoichiometric ternary metal sulfide alloyed semiconductor?CdxSb2?yS3?δ nanocrystals prepared by the two-stage sequential ionic layer adsorption reaction technique. The synthesized CdxSb2?yS3?δ nanocrystals retain the orthorhombic structure of the host Sb2S3 with Cd substituting a fraction (x = 0?0.15) of the cationic element Sb. The CdxSb2?yS3?δ lattice expands relative to the host, Sb2S3, with its lattice constant a increasing linearly with Cd content x. Optical and external quantum efficiency (EQE) spectra revealed that the bandgap Eg of CdxSb2?yS3?δ decreased from 1.99 to 1.69 eV (i.e., 625?737 nm) as x increased from 0 to 0.15. Liquid-junction CdxSb2?yS3?δ quantum dot-sensitized solar cells were fabricated using the polyiodide electrolyte. The best cell yielded a power conversion efficiency (PCE) of 3.72% with the photovoltaic parameters of Jsc = 15.97 mA/cm2, Voc = 0.50 V, and FF = 46.6% under 1 sun. The PCE further increased to 4.86%, a respectable value for a new solar material, under a reduced light intensity of 10% sun. The PCE (4.86%) and Jsc (15.97 mA/cm2) are significantly larger than that (PCE = 1.8%, Jsc = 8.55 mA/cm2) of the Sb2S3 host. Electrochemical impedance spectroscopy showed that the ZnSe passivation coating increased the electron lifetime by three times. The EQE spectrum of CdxSb2?yS3?δ has a maximal EQE of 82% at λ = 350 nm and covers the spectral range of 300?750 nm, which is significantly broader than that (300?625 nm) of the Sb2S3 host. The EQE-integrated current density yields a Jph of 11.76 mA/cm2. The tunable bandgap and a respectable PCE near 5% suggest that CdxSb2?yS3?δ could be a potential candidate for a solar material.