Cao R; Shang W; Wang P; Wang K; Zhang T; Gao R; Zhang X; Lv Z; Han Y; Li S; Cai R; Dong Q; Qiu J; Shi Y · 2026 · Advanced materials (Deerfield Beach, Fla.)
Paper
Achieving compositionally homogeneous mixed-halide (I - and Br - ) wide-bandgap (WBG) perovskite films is crucial for high-performance perovskite/crystalline silicon tandem solar cells (TSCs), yet the disparate crystallization kinetics of iodide- and bromide-rich phases readily induce halide segregation and inhomogeneous elemental distribution, thereby compromising the performance of TSCs. Herein, we employ 3,4,5-trifluorobenzeneboronic acid (3FBBA) as a multifunctional modulator that synergistically interacts with both organic cations and lead-halide octahedra via complementary hydrogen-bonding and coordination interactions, by which 3FBBA fundamentally modulates the formation mechanism of α-phase perovskite. It transforms the spontaneous, uncontrolled direct crystallization pathway into a well-regulated phase-transition process mediated by highly ordered intermediate phases. These well-structured intermediates act as well-defined pre-structural frameworks to guide the formation of high-quality α-phase perovskite. Benefiting from this strategy, the resultant WBG perovskite films possess enlarged grain size and reduced defect density, which suppress nonradiative recombination loss and accelerate charge transfer kinetics. As a consequence, a single-junction 1.66 eV WBG perovskite solar cell (PSC) achieves a high-power conversion efficiency (PCE) of 24.09%, while a two-terminal perovskite/silicon TSC delivers a champion PCE of 33.6%. Notably, the unencapsulated TSC maintains over 90% of its initial PCE throughout 571 h of continuous maximum power point tracking (MPPT) under ambient atmospheric conditions.
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