The heterointerfaces between perovskite and charge-transporting layers pose a major limitation to the durability of perovskite solar cells (PSCs), largely due to complex and conflicting chemical and mechanical interactions. Here we introduce an effective debonding technique to thoroughly analyse heterointerface behaviour during both crystal growth and ageing phases of PSCs. Our analysis reveals a strong correlation between interface bonding (fracture energy ranging from ~2.49 J m⁻² to ~0.38 J m⁻²), proton transfer interactions and degradation, highlighting a critical trade-off between mechanical and chemical stability in PSCs. To address these stability challenges, we mixed Me-4PACz and DCZ-4P molecules, which introduced additional phosphonic acid anchoring groups to enhance bonding at both the metal oxide and the perovskite interfaces. With a high efficiency of 25.6%, the devices retained 90% of their initial performance after 1,000 h of testing under ISOS-L-1I and ISOS-D-2I standard protocols. Under thermal cycling conditions, our PSCs sustained 95% of their efficiency over 500 cycles, exceeding the IEC 61215 and ISOS-T-3I standards.

钙钛矿和电荷传输层之间的异质界面对钙钛矿太阳能电池 （PSC） 的耐用性构成了重大限制，这主要是由于复杂且相互冲突的化学和机械相互作用。在这里，我们介绍了一种有效的解键技术，以彻底分析 PSC 晶体生长和老化阶段的异质界面行为。我们的分析揭示了界面键合（断裂能量范围从 ~2.49 J ^m-2 到 ~0.38 J ^m-2）、质子转移相互作用和降解之间的强相关性，突出了 PSC 中机械稳定性和化学稳定性之间的关键权衡。为了应对这些稳定性挑战，我们混合了 Me-4PACz 和 DCZ-4P 分子，引入了额外的膦酸锚定基团，以增强金属氧化物和钙钛矿界面的键合。这些设备具有 25.6% 的高效率，在 ISOS-L-1I 和 ISOS-D-2I 标准协议下经过 1000 小时的测试后，仍保留了 90% 的初始性能。在热循环条件下，我们的 PSC 在 500 次循环中保持了 95% 的效率，超过了 IEC 61215 和 ISOS-T-3I 标准。