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Heterojunction perovskite solar cells combine the stability of 2D perovskites and the high efficiency of 3D perovskites, making them an excellent photovoltaic candidate. While heterojunctions with intermixed or gradient perovskites can reduce surface recombination, the aggregation and phase distribution of 2D perovskite induce transport losses, thereby limiting device fill factors. Accordingly, a bulk in situ reconstruction (BISR) strategy is proposed to induce the reconstruction of 3D perovskites on a minim self‐assembled 2D crystal seed, forming heterojunction perovskite that runs through the entire active layer. This facilitates charge extraction, relieves tensile stress, and avoids the decomposition of perovskite on grain boundaries. As a result, the best‐performing heterojunction perovskite solar cells show a high‐power conversion efficiency (PCE) of 24.06% with 82.9% FF for the small‐area device (0.105 cm2) and a superior PCE of 19.2% for the large‐area module (5 × 5 cm2). Importantly, the unencapsulated device shows dramatically improved operational stability, maintaining 87% of its initial efficiency after 8000 h of storage under ambient atmosphere at room temperature. This work provides an effective and simple approach to establish heterojunction perovskite to simultaneously boost the efficiency and stability of PSCs. [ABSTRACT FROM AUTHOR]

The ability to develop bifunctional electrocatalysts for concurrent CO2 reduction reaction (CO2RR) and oxygen evolution reaction (OER) is the key to the practical application of CO2 splitting to produce CO. However, this remains a grand challenge. Herein, a robust strategy to rationally craft hierarchical structured bifunctional electrocatalysts composed of 3D CoS2 nanocages interconnected on 2D CoS2 nanosheet arrays (denoted hierarchical CoS2 nanocages) for high‐performance CO2 splitting is developed. The subsequent calcination removes the partial S edges of CoS2, thereby strongly suppressing the hydrogen evolution reaction (HER) of CoS2. By combining theoretic and experimental results, for the first time, it is discovered that the plane S of CoS2, instead of S edges, are highly active for CO2RR but inactive for HER, rendering the plane S as ideal active sites for CO2RR. Intriguingly, the composition tuning via calcination and the presence of a hierarchical architecture confer hierarchical CoS2 nanocages respective outstanding CO2RR and OER performance. Notably, the hierarchical CoS2 nanocages can be exploited as bifunctional electrocatalysts for overall CO2 splitting to yield the current density of 1 mA cm−2 at a small cell voltage of 1.92 V, much lower than the widely reported values (>2.5 V). [ABSTRACT FROM AUTHOR]