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Summary In the realm of solar cells, currently, the carbon‐electrode‐based, all‐inorganic perovskite solar cells (C‐IPSCs) based on cesium lead mixed halide perovskites have drawn much attention. Band‐gap tunability and environmental stability of these perovskites (CsPbIBr2) have been gaining attraction as a suitable absorber material for device fabrication. Fabrication of a high‐performing and stable C‐IPSC based on CsPbIBr2 is a challenging process due to high‐temperature fabrication, poor solution deposition of perovskite film, and high recombination at perovskite/carbon interface. In this work, a simple single‐step deposition process was adopted to engineer a good quality perovskite film by replacing conventional precursors with DMSO‐adducts of lead halide (PbX2). Incorporation of the adduct‐based precursor enables crystallization of CsPbIBr2 at a low temperature (~150°C). This enhances the crystallinity of the film, improves the grain size and defects passivation which imparts endurance to the perovskite against phase change and thermal stress. Thereby, enhancing the light absorption and suppressing the non‐radiative recombination in CsPbIBr2 film. As a result, the open‐circuit voltage is enhanced up to 1.18 V and fill factor up to 57%, further improving the power conversion efficiency by 59.4% leading to a champion device efficiency of 5.9%. Adduct‐based C‐IPSC displayed substantial enhancement of ambient stability and the adduct‐based perovskite exhibited excellent thermal stability.

The asymmetric unit of the title salt, C4H12NO2 +·C6H2N3O7 −, contain two bis­(2-hy­droxy­eth­yl)ammonium cations and two picrate anions. An intra­molecular N—H⋯O hydrogen bond occurs in each cation. In the crystal, mol­ecules are linked via O—H⋯O and N—H⋯O hydrogen bonds, which generate two R 2 1(6), an R 2 2(10) and an R 2 2(13) graph-set ring motifs. There are also a number of C—H⋯O hydrogen bonds present. The sum of these inter­actions leads to the formation a three-dimensional structure.

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