反式CsFA基无甲铵钙钛矿电池有潜力同时实现高的效率和优异的稳定性。然而，不可控的结晶过程和差的薄膜质量阻碍了光伏性能和稳定性的进一步提升。鉴于此，昆明理工大学陈江照、于月、大湾区大学于华、河北工业读大学陈聪、皖西学院张甲甲等人提出了基于羰基功能化的间隔阳离子的钙钛矿结晶和缺陷协同调控策略。将L-丙氨酸苄酯盐酸盐（L-ABEHCl）加入钙钛矿前驱液中，增加成核速率和延缓晶体生长速率，从而增加晶粒尺寸和结晶度。进一步使用L-ABEHCl处理制备的钙钛矿薄膜，在钙钛矿薄膜表界生成了2D钙钛矿。结果，L-ABEHCl以有机盐的形式钝化了晶界缺陷，以2D钙钛矿的形式钝化了界面缺陷。由于显著降低的非辐射复合损失，基于协同调控策略的反式电池取得了25.59%的认证效率，这是真空闪蒸技术制备电池报道的最高效率之一。未封装的目标电池在最大功率点工作2300小时后仍然保持初始效率的90.85%。

Figure 1.Crystallization modulation by L-ABEHCl.DLS spectra of the perovskite precursor solutions (a) without and (b) with adding L-ABEHCl. The in-situ absorption spectra of the wet perovskite films (c) without and (d) with incorporating L-ABEHCl during spin-coating process. The in-situ PL spectra of the perovskite films (e) without and (f) with L-ABEHCl during annealing. (g) Top: UV-vis absorption intensity evolution at the wavelength of 780 nm for the perovskite films during the annealing. Bottom: Corresponding nucleation ratescalculated from the UV-vis spectra using the first derivative. XRD patterns of the perovskite films (h) without and (i) with L-ABEHCl annealed at 100 ℃ for different times (0, 1, 5, 10, 30, 60 and 300 s). δdenotes the yellow non-perovskite phase.

Figure 2.Investigation on perovskite crystal phase.(a) XRD patterns of the control, L-ABEHCl(A), L-ABEHCl(I) and L-ABEHCl(A@I) perovskite films. (b) Formation energy of (L-ABEHCl)2(CsFA)n-1Pbn(I1-xClx)3n+12D perovskites with different n values by DFT calculation. GIWAXS of the (c) control and (d) L-ABEHCl(I) perovskite films. XRD patterns of (L-ABEHCl)2Pb(I1-xClx)4with excess different ratios of (e) CsI and (f) FAI.

Figure 3.Mechanisms of crystallization modulation and synergistic passivation of grain boundaries and interface.Schematic illustration of perovskite nucleation and growth of the perovskite films (a) without and (b) with L-ABEHCl additive. (c) Schematic of the synergistic passivation of grain boundaries and interface.

Figure 4.Characterizations of perovskite film quality.SEM images of the (a) control, (b) L-ABEHCl(A), (c) L-ABEHCl(I) and (d) L-ABEHCl(A@I) perovskite films. PL mappings of the (e) control, (f) L-ABEHCl(A), (g) L-ABEHCl(I) and (h) L-ABEHCl(A@I) perovskite films. (i) PL and (j) TRPL spectra of the control, L-ABEHCl(A), L-ABEHCl(I) and L-ABEHCl(A@I) perovskite films deposited on bare glass substrate. (k) Defect density of the four perovskite films for electron- and hole-only devices.

Figure 5.Investigation on carrier dynamics.(a) Energy level arrangement plot of devices. (b) TRPL curves of the four perovskite films with the structure of glass/perovskite/PCBM. (c) TPC and (d) TPV decay curves of the control, L-ABEHCl(A), L-ABEHCl(I), and L-ABEHCl(A@I) PSCs. (e) Light-intensity-dependent VOC for the control, L-ABEHCl(A), L-ABEHCl(I), and L-ABEHCl(A@I) PSCs. q is electron charge. KB is Boltzmann constant. T is kelvin temperature.

Figure 6.Photovoltaic performance and long-term stability.(a) J-Vcurves of the champion control, L-ABEHCl(A), L-ABEHCl(I) and L-ABEHCl(A@I) devices prepared by anti-solvent method. (b) J-Vcurves of the champion control, L-ABEHCl(A), L-ABEHCl(I) and L-ABEHCl(A@I) devices prepared by vacuum flash evaporation in ambient air. (c) PCE of the unencapsulated four devices measured at MPP under continuous one-sun illumination in N2atmosphere. (d) Air storing stability evolution of the unencapsulated devices held at 25%~30% relative humidity. (e) Thermal stability evolution of the unencapsulated devices held at 85 ℃ in N2.

论文链接：

Shiying Tang#, Zuolin Zhang#, Yue Yu*, Xinxing Liu, Dongmei He, Xuxia Shai, Jiajia Zhang*, Jing Feng, Jianhong Yi, Cong Chen*, Hua Yu*, Jiangzhao Chen*. Crystallization modulation and comprehensive defect passivation by carbonyl functionalized spacer cation towards high-performance inverted perovskite solar cells. Angewandte Chemie International Edition 2025, e202425605.

https://onlinelibrary.wiley.com/doi/10.1002/anie.202425605

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