Expanding interspace and introducing vacancies are desired to promote the mobility of Zn ions and unlock the inactive sites of layered cathodes. However, this two‐point modulation has not yet been achieved simultaneously in vanadium phosphate. Here, a strategy is proposed for fabricating an alcohol‐based organic–inorganic hybrid material, VO1−xPO4·0.56C6H14O4, to realize the conjoint modulation of the d‐interspace and oxygen vacancies. Peculiar triglycol molecules with an inclined orientation in the interlayer also boost the improvement in the conversion rate of V5+ to V4+ and the intensity of the PO bond. Their synergism can ensure steerable adjustment for intercalation kinetics and electron transport, as well as realize high chemical reactivity and redox‐center optimization, leading to at least 200% increase in capacity. Using a water–organic electrolyte, the designed Zn‐ion batteries with an ultrahigh‐rate profile deliver a long‐term durability (fivefold greater than pristine material) and an excellent energy density of ≈142 Wh kg−1 (including masses of cathode and anode), thereby substantially outstripping most of the recently reported state‐of‐the‐art zinc‐ion batteries. This work proves the feasibility to realize the two‐point modulation by using organic intercalants for exploiting high‐performance new 2D materials.

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Post-treatment is a widely used strategy to reduce defects in perovskite films, but has been largely limited to the solution phase. Herein, the posttreatment tool kit and develop a universal amine salts (A I X I ) vapor healing strategy by taking advantage of the penetrating power of vapor and the soft-matter characteristics of halide perovskite is expanded. In a striking demonstration, the post-treatment of pristine perovskite layers allows simultaneous filling of the MA + and Ivacancies, passivation of both the cation and anion defects, and healing of the films to high order and high crystallinity required for high device performance, from the surface to the bulk and all the way down to the bottom. Experiments and DFT calculations revealed that charge extraction can be enhanced and non-radiative recombination can be reduced by regulating the energy levels and reducing the trap states via the A I X I vapor healing. Moreover, the diffusing A I X I can reach the NiO x surface to obstruct the undesirable interfacial reactions and passivate the interface defects, further reducing the opencircuit voltage (V oc ) loss. The vapor healing strategy substantially reduces the trap density from 4.76 × 10 15 to 1.04 × 10 15 cm -3 , and promots power conversion efficiency of the champion device from 17.92% to 20.48% with superior device consistency, V oc up to 1.114 V and the operational device stability.

Currently, the full potential of perovskite solar cells (PSCs) is limited by chargecarrier recombination owing to imperfect passivation methods. Here, the recombination loss mechanisms owing to the interfacial energy offset and defects are quantified. The results show that a favorable energy offset can reduce minority carriers and suppress interfacial recombination losses more effectively than chemical passivation. To obtain high‐efficiency PSCs, 2D perovskites are promising candidates, which offer powerful field effects and require only modest chemical passivation at the interface. The enhanced passivation and charge‐carrier extraction offered by the 2D/3D heterojunction PSCs has boosted their power conversion efficiency to 25.32% (certified 25.04%) for small‐size devices and to 21.48% for a large‐area module (with a designated area of 29.0 cm2). Ion migration is also suppressed by the 2D/3D heterojunction, such that the unencapsulated small‐size devices maintain 90% of their initial efficiency after 2000 h of continuous operation at the maximum power point.