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Probing the Key Roles of the Back Interface in the Performance of Carbon-Based Hole-Transport-layer Free Perovskite Solar Cells

Xinwei Li,Nianqing Fu, Xiaocao Peng, Hehui Lin, Jiaang Cheng,Ziming Chen,Peng Lin,Jun Du

JOURNAL OF MATERIALS CHEMISTRY A(2024)

South China Univ Technol

Cited 0|Views11
Abstract
Carbon electrodes have gained widespread attention as a sustainable, stable, and low-cost alternative to metal electrodes in perovskite solar cells (PSCs). However, the power conversion efficiency (PCE) of carbon electrode-based PSCs (C-PSCs) without the hole-transport-layer (HTL) lags far behind their metal-electrode-based counterparts (M-PSCs), and the key factors causing this PCE downgrading have not been comprehensively elucidated. Herein, we study the photovoltaic performance of various HTL-free C-PSCs employing four typical absorbers, namely MAPbI(3) (MA = CH3NH3), FAPbI(3) (FA = CH(NH2)(2)) , one-step processed FA(0.85)MA(0.15)PbI(3) (FA/MA-OS), and two-step processed FA1-xMAxPbI(3) (FA/MA-TS). Unexpectedly, we found that the PCE of C-PSCs follows the order MAPbI3 > FAPbI3 > FA/MA-TS > FA/MA-OS, quite different from that of devices with the Ag-electrode (FAPbI3 > FA/MA-TS > FA/MA-OS > MAPbI3). The in-depth studies reveal that the remarkable differences in surface roughness, surface potential (SP) distribution, and local built-in potential (Vbi) of the four absorber films directly affect both the physical and electrical contacts between the perovskite and carbon electrode, which finally determine the efficiency of C-PSCs. Among them, the MAPbI(3) films possess the smallest roughness and minimum SP gaps between the grain boundaries (GBs) and the grain interiors (GIs), which enable compact contact at the perovskite/carbon interface and higher Vbi within the C-PSCs for fast charge transfer, significantly suppressed nonradiative recombination, and thus the highest PCE (15.42%). Based on these findings, we provide some promising approaches for the development of high-efficiency C-PSCs, especially for the ones employing FA-based perovskite absorbers which have performed excellently in M-PSCs.
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要点】:研究揭示了碳电极基钙钛矿太阳能电池(C-PSCs)无空穴传输层(HTL)时,背界面对光伏性能的关键作用,并基于此提出了提升效率的新方法。

方法】:通过研究不同吸光材料的C-PSCs的光伏性能,并深入分析表面粗糙度、表面电位分布和局部内置电势对钙钛矿与碳电极间物理和电接触的影响。

实验】:实验采用了四种典型吸光材料(MAPbI3、FAPbI3、FA/MA-OS、FA/MA-TS),发现PCE的排序与银电极基钙钛矿太阳能电池(M-PSCs)不同,并确定了MAPbI3薄膜因其最小的表面粗糙度和最小的表面电位差距而具有最高效率(15.42%),基于此结果提出了优化策略。