In this work, we reveal the role of non-covalent interactions, which are known to play important roles in supramolecular phenomena, in achieving efficient perovskite surface and grain boundary passivation. By using a series of pseudohalides, we find that trifluoroacetate (TFA⁻) provides the strongest binding to iodide vacancies by means of non-covalent hydrogen bonding and dispersion interactions. By exploiting additional non-covalent dispersion and hydrophobic interactions in aromatic 3,3-diphenylpropylammonium (DPA⁺), we present a dual-ion passivation strategy that not only minimizes the non-radiative recombination center and local chemical inhomogeneities but also induces preferentially oriented growth of α-FAPbI₃ lattice. This leads to an outstanding power conversion efficiency (PCE) of 25.63% with an exceptional open-circuit voltage of 1.191 V in a perovskite solar cell with a small area, while perovskite solar mini modules with aperture areas of 25 and 64 cm² achieved PCE of 22.47% (quasi-steady-state [QSS]-certified 20.50%) and 20.88%, respectively, with outstanding stability under high-humidity conditions.

在这项工作中，我们揭示了非共价相互作用在超分子现象中发挥重要作用，在实现有效的钙钛矿表面和晶界钝化方面的作用。通过使用一系列拟卤化物，我们发现三氟乙酸盐（TFA ^- ）通过非共价氢键和色散相互作用提供与碘化物空位最强的结合。通过利用芳香族 3,3-二苯基丙基铵 (DPA ⁺ )中额外的非共价分散和疏水相互作用，我们提出了一种双离子钝化策略，不仅最大限度地减少非辐射复合中心和局部化学不均匀性，而且还诱导优先定向生长α-FAPbI ₃晶格。这使得小面积钙钛矿太阳能电池具有 25.63% 的出色功率转换效率 (PCE) 和 1.191 V 的优异开路电压，而孔径面积为 25 和 64 cm ²的钙钛矿太阳能微型组件则实现了 PCE分别为 22.47%（准稳态 [QSS] 认证的 20.50%）和 20.88%，在高湿度条件下具有出色的稳定性。