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Low-temperature noninjection approach to homogeneously-alloyed PbSexS1\u2212x colloidal nanocrystals for photovoltaic applications

机译:用于光伏应用的均匀合金化PbSexS1 \ u2212x胶态纳米晶体的低温非注入方法

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摘要

Homogeneously alloyed PbSexS1\u2212x 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\u2212x NCs were carried out at low temperature (60 \ub0C) 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 air-sensitive 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\u2212P 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\u2212P complex, the higher the Se amount in the resulting homogeneously alloyed PbSexS1\u2212x 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.
机译:均质合金化的PbSexS1 \ u2212x纳米晶体(NCs)的激子吸收峰的波长短于1200 nm,已开发用于光伏(PV)应用。以我们的PbSe0.3S0.7 NC作为活性材料制造的肖特基型太阳能电池,具有3.44%的高功率转换效率(PCE),开路电压(Voc)为0.49 V,短路光电流(Jsc)为在100 mW / cm2的空气质量1.5全局辐射(AM 1.5G)照射下,填充系数(FF)为13.09 mA / cm2,填充因子(FF)为0.54。小型胶体PbSexS1 \ u2212x NC的合成是通过在1-十八碳烯(ODE)中基于非注入的一锅法在低温(60 \ ub0C)和长的生长周期(例如45分钟)下进行的,具有高反应收率,高产品质量和高合成重现性的特点。这种低温方法采用Pb(油酸酯)2作为Pb前体,并使用空气稳定的低成本硫代乙酰胺(TAA)作为S源,而不是对空气敏感的低成本双(三甲基甲硅烷基)硫化物((TMS)2S),用正三丁基膦硒化物(TBPSe)作为硒前体,而不是正三辛基膦硒化物(TOPSe)。通过现场观察NC吸收的时间演变和31P核磁共振(NMR)解决了由商用TOP 90%制成的TOPSe和由商用TBP 97%和TBP 99%制成的TBPSe的反应性差异。此外,添加强还原剂/成核剂二苯膦(DPP)通过形成Pb \ u2212P配合物来促进Pb前体的反应性,该配合物比Pb(油酸酯)2具有更高的反应活性。因此,TBPSe的反应性比TAA的增加更多。 DPP与Pb的进料摩尔比越大,Pb \ u2212P络合物越多,则在所得的均匀合金化的PbSexS1 \ u2212x NC中,硒含量越高。因此,使用DPP可以使Se和S前体的反应性匹配,并在低温下导致相当大的成核作用,因此长的生长期变得可行。本研究使人们深入了解单体的形成机理,胶体组成可调NC的成核/生长以及下一代低成本和高效率太阳能电池的材料设计与合成。

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