重庆大学臧志刚教授团队在Advanced Materials期刊发表题为“Iodide Management and Oriented Crystallization Modulation for High-Performance All-Air Processed Perovskite Solar Cells”的研究论文,团队成员杨海超为论文第一作者,臧志刚教授为论文通讯作者。
核心亮点:本文提出一种埋地界面优化策略,实现了全空气加工器件(Rb0.02(FA0.95Cs0.05)0.98PbI2.91Br0.03Cl0.06)PCE的最高值(25.13%)和高开路电压(1.191 V)。
埋底界面卤化物相关缺陷不仅会引起非辐射复合,而且会严重影响钙钛矿太阳能电池(PSCs)的长期稳定性。基于上述问题,重庆大学臧志刚教授课题组提出了一种涉及多位点抗氧化剂麦角硫因(EGT)的自下而上、一体化改性技术来优化钙钛矿的埋底界面的策略,以管理碘离子并操纵结晶动力学。优化后的全空气加工器件(Rb0.02(FA0.95Cs0.05)0.98PbI2.91Br0.03Cl0.06)的功率转换效率(PCE)达到了25.13%,是空气加工器件的最高值之一,同时具有1.191 V的超高开路电压(VOC)和84.9%的填充因子(FF)。优化后的无封装器件在ISOS协议下具有较强的湿度、热稳定性和操作稳定性。具体来说,该器件在65°C下热老化1512 h后的初始效率保持在90.12%,在模拟AM1.5照明下连续最大功率点跟踪(MPPT) 930 h后的初始效率保持在90.14%。
Figure 1. a) Diagrammatic representation of the mechanism for defect formation and passivation through EGT modification. b) Electron mobility of the pristine SnO2 and EGT-modified SnO2. Conductive AFM images of c) SnO2 and d) SnO2/EGT. e) Sn 3d XPS spectra of SnO2 and SnO2/EGT films. XPS spectra of O 1s for f) pristine SnO2 and g) EGT-modified SnO2 films. h) 13C NMR spectra of SnO2 solutions containing EGT and pure EGT. FTIR spectra in the wavenumber ranges of i) 2250–2450 cm−1 and j) 1550–1700 cm−1 of SnO2, SnO2 mixed with EGT and pure EGT.
Figure 2. a) Pb 4f and b) I 3d XPS spectra of the control and EGT-modified perovskite. c) FTIR spectra of PbI2, PbI2 combined with EGT and pure EGT in the region of 1520−1750 cm−1. GIXRD patterns of the perovskite films prepared on d) SnO2 and e) SnO2/EGT. f) Dependence of the d-spacing values on grazing incidence angle of perovskite films. GIWAXS patterns of the g) control and h) EGT-modified perovskite films. In situ PL analyses of the control perovskite films over i) spinning and j) annealing process. In situ PL analyses of the EGT-modified perovskite films over k) spinning and l)
annealing process. In situ UV–vis absorption measurements of the m) control and n) EGT-modified perovskite films during the annealing process. XRD patterns of o) control and p) EGT-modified perovskite films with different annealing times.
Figure 3. a) Photographs of FAI solutions and FAI powders without and with EGT that were aged under ambient conditions. UV–vis absorption spectra of b) pure FAI and c) FAI containing EGT that were aged under ambient conditions. d) UV–vis absorption spectra of I2 and I2 with EGT. FTIR spectra of I2, I2 with EGT, and pure EGT in the regions of e) 3050‒3250 cm−1 and f) 1450‒1750 cm−1. g) Pb 4f XPS spectra of aged perovskite films. UV–vis absorbance spectra of the toluene soaked with h) control and i) EGT-modified perovskite films exposed to light soaking and 65 °C heating treatment. j) TGA plots of weight loss of perovskite without and with EGT.
Figure 4. a) Top-view and b) cross-sectional SEM morphology, as well as c) normal distribution of particle sizes for the perovskite-based on SnO2. d) Top-view and e) cross-sectional SEM morphology, as well as f) normal distribution of particle sizes for the perovskite-based on SnO2/EGT. KPFM measurements of the g) control and h) EGT-modified perovskite films, as well as the i) line sweep curves. j) Schematic diagram of morphology and defect passivation of perovskite films before and after EGT optimization.
Figure 5. a) PL and b) TRPL spectra of the perovskite films prepared on glass or glass/EGT. PL mapping measurements of the perovskite films deposited on c) glass or d) glass/EGT. e) PL and f) TRPL spectra of the perovskite films based on ITO/SnO2 or ITO/SnO2/EGT. PL mapping images of the perovskite films synthesized on SnO2 g) without or h) with EGT modification. i) PLQY of perovskite films. j) Transient photovoltage decay curves of the devices based on SnO2 or SnO2/EGT. k,l) SCLC versus voltage of the electron-only devices. m) Energy level diagram of each part in the device. n) Transient photocurrent decay measurements of both devices. o) Nyquist plots of the PSCs based on SnO2 and SnO2/EGT. p) Mott–Schottky analysis of the devices.
Figure 6. a) Normal distribution of the PCEs for the devices without or with EGT modification, consisted of twenty independent cells for each device. b) J–V curves of the champion devices based on SnO2 or SnO2/EGT. c) J–V curves of the champion EGT-modified device with PEAI post-treatment. d) J–V curves of the target device with an active area of 1 cm2. e) Steady-state output measurements for the champion PSCs without or with EGT modification. f) IPCE spectra of the best-performing device. g) Humidity stability of the unencapsulated devices under an ambient environment with 30 ± 5% RH. h)
Thermal stability of the unencapsulated devices heated at 65 °C. i) Operational stabilities of the unencapsulated PSCs at maximum power point under one-sun illumination at 25 ± 5 °C.
Figure 7. a) Photo images of perovskite films aged for12 days under 65% RH. UV–vis absorption spectra of b) control and c) target perovskite films after ageing at 65% RH for different times. XRD patterns of d) control and e) target perovskite films after ageing at 65% RH for different times. SEM images of f) control and g) EGT-modified perovskite films heated at 65 °C and under continuous one-sun illumination for 10 h.
本文来源:DOI: 10.1002/adma.202411721
https://doi.org/10.1002/adma.202411721