Summary This work investigated the preparation and optimization of phosphor layer for radioluminescent nuclear battery, and analyzed the property change of the phosphor after irradiation. ZnS:(Cu, Al) with grain size of 5 μm was selected as the phosphor material, and AlGaInP semiconductor was used as the photovoltaic unit. Monte Carlo modeling was used to simulate energy deposition, absorbed dose, penetration of β particles in the phosphor. The optimized coupling scheme of radioisotope sources and phosphor layer was obtained based on comparison particle penetration depth and the output power of radioluminescent nuclear battery. The phosphor layer with 60Co γ‐radiation enhanced the luminescence property up to 50% at the radiation dose of 871 kGy, which is considered as an optimized method of phosphor layer preparation. The radiation of 10 MeV electron was conducted to study the degradation based on the microscopic lattice characteristics, morphological changes, optical and electrical properties. Phosphors have excellent radiation resistance. The output power of nuclear batteries has only declined by 43% even when electron radiation dose reaches 8.56 MGy. The prospect for utilizing ZnS:(Cu, Al) phosphor as radiant energy conversion materials in nuclear battery was also discussed. Results provided an effective guideline for predict the service conditions of radioluminescent nuclear battery.

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Low conversion efficiency and energy output are the main factors hindering the application of the radioluminescent nuclear battery in space. This study analyzes the energy conversion process and proposes a solution of performance promotion. It is found that the energy conversion efficiency of the photovoltaic units is enhanced with increasing incident light intensity. The efficiency of the AlGaInP unit is stable at 22% when the incident energy is at least 3 μW. As for the GaAs unit, the incident threshold value of the photovoltaic response sensitivity is greater than 120 μW. The overall efficiency of the radioluminescent nuclear battery is only 0.37%, consisting of an AlGaInP unit loaded with a low activity 63Ni and the ZnS:Cu phosphor layer. The efficiency increases to 0.87% when an electron radiation source with 270.27 mCi cm−2 is adopted. Moreover, the intense intensity source constitutes an extremely electromagnetic pulse radiation environment, which cause the batteries to fail. The radiation damage is introduced to the phosphor layer by radiation sources, producing agglomerations and cracks on the surface and resulting in the transmittance reduction. This study provides guidance for improving the electrical property and optimization solutions of radioluminescent nuclear battery.