一种用于将金属直接转化为光电级溴化物钙钛矿的通用多溴化物熔盐策略

中文摘要 AI 辅助

卤化物钙钛矿体系需要特定的金属氧化态（M²⁺或M⁺/M³⁺对），这限制了传统合成过程中的加工灵活性，并对Sn、Cu和Au等多价金属构成稳定性挑战。本研究确立了一种深刻的范式转变：一种通用的、单步的、无有机溶剂的合成平台，可将稳定的元素金属薄膜直接转化为溴化物钙钛矿及钙钛矿相关体系，用于多种（光）电子应用。该合成平台使用甲基铵多溴化物熔盐（PBM），在室温下与Pb、Sn、Au和Cu等不同元素金属反应，成功将它们转化为各自的溴钙钛矿相：MAPbBr₃、MASnBr₃、MA₂Au₂Br₆和MA₂CuBr₄。研究表明，PBM的化学活性可被调控，原位X射线衍射在两种情况下捕获了相演化过程中的瞬态中间相。对于易被过度氧化为Sn⁴⁺相的Sn，通过改变PBM的组成并结合金属Sn介导的归中反应，可抑制过度氧化，在环境条件下形成高质量的MASnBr₃薄膜。总体而言，氧化和歧化电位被发现是预测M:PBM反应结果的有用指标。在工业上，该方法应与卷对卷基础设施完全兼容，为下一代光电技术的规模化提供低门槛途径。

英文摘要

Halide perovskite systems require specific metal oxidation states (M2+ or M+/M3+ pairs), limiting processing flexibility during traditional synthesis and posing stability challenges for multivalent metals like Sn, Cu, and Au. This work anchors a profound paradigm shift: a universal, single-step, organic-solvent free synthetic platform that directly converts stable elemental metal films into bromide perovskite and perovskite-related systems for a wide variety of (opto)electronic applications. The synthetic platform uses methylammonium polybromide melt (PBM) that reacts at room temperature with different elemental metals, including Pb, Sn, Au, and Cu, successfully transforming them into their respective Br-perovskite phases: MAPbBr3, MASnBr3, MA2Au2Br6, and MA2CuBr4. It is shown that the PBMs chemical activity can be tuned, and in situ X-ray diffraction captures in two cases transient intermediate phases during phase evolution. For Sn, which tends towards overoxidation to Sn4+ phase, changes in the PBMs composition coupled with a metallic Sn mediated comproportionation reaction allowed suppressing overoxidation, and formation of high quality MASnBr3 films under ambient conditions. Overall, oxidation and disproportionation potentials are found to be useful metrics for predicting M:PBM reaction outcomes. Industrially, this approach should be fully compatible with roll-to-roll infrastructure, providing a low-barrier pathway to scale next-generation optoelectronic technologies.

发表机构

• Ben Gurion University of the Negev（本-古里安大学）
• Ilse Katz Institute for Nanoscale Science and Technology, Ben-Gurion University of the Negev（本-古里安大学伊尔斯·卡茨纳米科学与技术研究所）

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