Organic-inorganic hybrid perovskite solar cells (PSCs) have been extensively studied because of their outstanding performance: a power conversion efficiency exceeding 22% has been achieved. The most commonly used PSCs consist of CH3NH3PbI3 (MAPbI3) with a hole-selective contact, such as 2,2′,7,7′-tetrakis(N,N-di-p-methoxyphenylamine)-9,9-spiro-bifluorene (spiro-OMeTAD), for collecting holes. From the perspective of long-term operation of solar cells, the cell performance and constituent layers (MAPbI3, spiro-OMeTAD, etc.) may be influenced by external conditions like temperature, light, etc. Herein, we report the effects of temperature on spiro-OMeTAD and the interface between MAPbI3 and spiro-OMeTAD in a solar cell. It was confirmed that, at high temperatures (85 °C), I− and CH3NH3 + (MA+) diffused into the spiro-OMeTAD layer in the form of CH3NH3I (MAI). The diffused I− ions prevented oxidation of spiro-OMeTAD, thereby degrading the electrical properties of spiro-OMeTAD. Since ion diffusion can occur during outdoor operation, the structural design of PSCs must be considered to achieve long-term stability.

The effects of exchange current density, Tafel slope, system resistance, electrode area, light intensity, and solar cell efficiency were systematically decoupled at the converter-assisted photovoltaic–water electrolysis system. This allows key determinants of overall efficiency to be identified. On the basis of this model, 26.5% single-junction GaAs solar cell was combined with a membrane-electrode-assembled electrolysis cell (EC) using the dc/dc converting technology. As a result, we have achieved a solar-to-hydrogen conversion efficiency of 20.6% on a prototype scale and demonstrated light intensity tracking optimization to maintain high efficiency. We believe that this study will provide design principles for combining solar cells, ECs, and new catalysts and can be generalized to other solar conversion chemical devices while minimizing their power loss during the conversion of electrical energy into fuel.

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