陳江照&臧志剛&丁黎明EcoMat,通過新型鏻鎓鹽鈍化介面缺陷實現高效穩定無甲銨鈣鈦礦太陽能電池

介面缺陷引起的載流子非輻射複合損失阻礙了電池效能的進一步提升。鑒於此,重慶大學陳江照研究員、臧志剛教授和國家納米中心丁黎明研究員等人創新性地採用含PF6-對陰離子的新型鏻鎓鹽來修飾鈣鈦礦/Spiro-OMeTAD介面。有機鏻鎓鹽中的陰陽離子與鈣鈦礦不僅發生離子作用而且發生配比特作用。

介面缺陷引起的載流子非輻射複合損失阻礙了電池效能的進一步提升。鑒於此,重慶大學陳江照研究員、臧志剛教授和國家納米中心丁黎明研究員等人創新性地採用含PF6-對陰離子的新型鏻鎓鹽(ClTPPPF6和BrTPPPF6)來修飾鈣鈦礦/Spiro-OMeTAD介面。

有機鏻鎓鹽中的陰陽離子與鈣鈦礦不僅發生離子作用而且發生配比特作用。無甲銨鈣鈦礦薄膜表面及晶界的陰陽離子空位缺陷能够分別被有機鏻鎓鹽中陰陽離子填充,導致缺陷密度减小,載流子壽命新增。有趣的是,溴取代陽離子的BrTPPPF6與鈣鈦礦之間的作用力强於氯取代的ClTPPPF6。BrTPPPF6更强的化學作用有利於更好地鈍化表面及介面缺陷。

結果,基於ClTPPPF6和BrTPPPF6修飾的電池分別實現了21.73%和22.15%的效率,遠遠高於對照器件的效率(20.6%)。未封裝的基於BrTPPPF6改性的電池60℃老化1320小時後仍然保持初始效率的98.2%,空氣中老化2016小時後仍然保持初始效率的96.4%。

FIGURE 1(a)Chemical structures of ClTPPPF6 andBrTPPPF6.(b)Device configuration in the present work.(c)Schematically illustrated diagram of defect passivation by BrTPPPF6.XPS spectra of the pristine and modified perovskite films along with ClTPPPF6 and BrTPPPF6:(d)Pb 4f,(e)F 1s,and(f)N 1s spectra ofperovskite films modified with or without.PVSK represents perovskite layer.

FIGURE2 The optimized structures for the ground-state FAPbI3(001)-BrTPPPF6(ClTPPPF6)interfaces.(a)Interfaces for the inorganic PbI2 plane with/without iodine defect and lead cluster in contact with BrTPPPF6 and ClTPPPF6,respectively.The inset shows atomic colors: H(white),C(grey),N(blue),F(violet),P(cyan),Cl(green),Br(brown),I(yellow)and Pb(black).(b)The binding energies(Eb)of the PbI2 plane with/without iodine defect and lead cluster of FAPbI3perovskite in contact with BrTPPPF6(ClTPPPF6)organicsalts.

FIGURE3 The calculated density of states for the ground-state FAPbI3 perovskite with different planes and BrTPPPF6(ClTPPPF6),respectively.Fermi level is set to zero.

FIGURE 4(a)XRD patterns of the perovskite films without and with ClTPPPF6 and BrTPPPF6 modification.(b)SSPL and(c)TRPL spectra of the perovskite films without and with interface modification deposited on non-conductive glass.PL mapping images of(d)the pristine perovskite film and perovskite films modified by(e)ClTPPPF6and(f)BrTPPPF6.Conductive AFM images of the perovskite films(g)without modification and with(h)ClTPPPF6 and(i)BrTPPPF6 modification.Dark I-V curves of the devices with the structure of(j)ITO/perovskite/Au,(k)ITO/perovskite/ClTPPPF6,and(l)ITO/perovskite/BrTPPPF6.PVSK stands for perovskite layer.

FIGURE 5(a)Energy level diagram.(b)TRPL spectra ofthe perovskite films without and with ClTPPPF6 and BrTPPPF6 modification covered with Spiro-OMeTAD(denoted as HTM).PVSK and HTL represent perovskite layer and Spiro-OMeTAD,respectively.(c)TPC and(d)TPV curves of the devices without and with ClTPPPF6 and BrTPPPF6 modification.(e)Voc depending on light intensities for the control device,ClTPPPF6-modified and BrTPPPF6-modifie ddevices.(f)Nyquist plots of the control device,ClTPPPF6-modified and BrTPPPF6-modified devices which was measured in the frequency range of 1 MHz to 0.1 Hz at a bias of 0.8 V under one sun illumination.

FIGURE 6(a)Statistical distribution diagram of PCEsfor the devices without and with ClTPPPF6 and BrTPPPF6 modification.The data were obtained from 20 cells.(b)J-V curves and(c)IPCE spectra of the champion devices without and with ClTPPPF6 and BrTPPPF6 modification.(d)Steady-state current density and PCE versus time for the best-performing control,ClTPPPF6-modified and BrTPPPF6-modified devices measured at the maximum power point.(e)Moisture stability of the unencapsulated control,ClTPPPF6-modified and BrTPPPF6-modified devices aged under a relative humidity of 10-20% at room temperature in the dark.(f)Thermal stability of the unencapsulated control,ClTPPPF6- modified and BrTPPPF6-modified devices aged at 60°C in the dark in the nitrogen-filled glovebox.

參考文獻:

Dongmei He #,Tingwei Zhou #,Baibai Liu,Le Bai,Wenqi Wang,Hongkuan Yuan,Cunyun Xu,Qunliang Song,Donghwa Lee,Zhigang Zang*,Liming Ding*,Jiangzhao Chen*.Interfacial defect passivation by novel phosphonium salts yields 22% efficiency perovskite solar cells: experimental and theoretical evidence.EcoMat 2021,4(1),e12158.

https://doi.org/10.1002/eom2.12158.

本文標題: 陳江照&臧志剛&丁黎明EcoMat,通過新型鏻鎓鹽鈍化介面缺陷實現高效穩定無甲銨鈣鈦礦太陽能電池
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