Low-temperature noninjection approach to homogeneously-alloyed PbSe xS1-x colloidal nanocrystals for photovoltaic applications

Kui Yu, Jianying Ouyang, Yanguang Zhang, Hsien Tse Tung, Shuqiong Lin, Robbert A.L. Nagelkerke, David Kingston, Xiaohua Wu, Donald M. Leek, Diana Wilkinson, Chunsheng Li, In Gann Chen, Ye Tao

研究成果: Article同行評審

40 引文 斯高帕斯(Scopus)

摘要

Homogeneously alloyed PbSexS1-x nanocrystals (NCs) with their excitonic absorption peaks in wavelength shorter than 1200 nm were developed for photovoltaic (PV) applications. Schottky-type solar cells fabricated with our PbSe0.3S0.7 NCs as their active materials reached a high power conversion efficiency (PCE) of 3.44%, with an open circuit voltage (Voc) of 0.49 V, short circuit photocurrent (Jsc) of 13.09 mA/cm2, and fill factor (FF) of 0.54 under Air Mass 1.5 global (AM 1.5G) irradiation of 100 mW/cm2. The syntheses of the small-sized colloidal PbSexS1-x NCs were carried out at low temperature (60 °C) with long growth periods (such as 45 min) via a one-pot noninjection-based approach in 1-octadecene (ODE), featuring high reaction yield, high product quality, and high synthetic reproducibility. This low-temperature approach employed Pb(oleate)2 as a Pb precursor and air-stable low-cost thioacetamide (TAA) as a S source instead of airsensitive high-cost bis(trimethylsilyl)sulfide ((TMS)2S), with n-tributylphosphine selenide (TBPSe) as a Se precursor instead of n-trioctylphosphine selenide (TOPSe). The reactivity difference of TOPSe made from commercial TOP 90% and TBPSe made from commercial TBP 97% and TBP 99% was addressed with in situ observation of the temporal evolution of NC absorption and with 31P nuclear magnetic resonance (NMR). Furthermore, the addition of a strong reducing/nucleation agent diphenylphosphine (DPP) promoted the reactivity of the Pb precursor through the formation of a Pb-P complex, which is much more reactive than Pb(oleate)2. Thus, the reactivity of TBPSe was increased more than that of TAA. The larger the DPP-to-Pb feed molar ratio, the more the Pb-P complex, the higher the Se amount in the resulting homogeneously alloyed PbSexS1-x NCs. Therefore, the use of DPP allowed reactivity match of the Se and S precursors and led to sizable nucleation at low temperature so that long growth periods became feasible. The present study brings insight into the formation mechanism of monomers, nucleation/growth of colloidal composition-tunable NCs, and materials design and synthesis for next-generation low-cost and high-efficiency solar cells.

原文English
頁(從 - 到)1511-1520
頁數10
期刊ACS Applied Materials and Interfaces
3
發行號5
DOIs
出版狀態Published - 2011 五月 25

All Science Journal Classification (ASJC) codes

  • Materials Science(all)

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