Tailored Reaction Conditions and Automated Radiolabeling of [(177)Lu]Lu-PSMA-ALB-56 in a (68)Ga Setting: The Critical Impact of Antioxidant Concentrations

在 (68)Ga 环境下定制反应条件和 [(177)Lu]Lu-PSMA-ALB-56 的自动放射性标记:抗氧化剂浓度的关键影响

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Abstract

The growing use of experimental radiopharmaceuticals for targeted radionuclide therapy (TRT) highlights the need for robust "in house" radiolabeling protocols. Among these, PSMA-ALB-56 is a PSMA ligand incorporating an albumin-binding moiety to enhance pharmacokinetics, which showed promise for prostate cancer treatment. This study investigated manual radiolabeling conditions of this vector molecule with lutetium-177 and developed a corresponding automated synthesis protocol. Manual experiments on low activities explored buffer systems and antioxidants, identifying sodium acetate buffer and L-methionine as optimal, achieving radiochemical purities above 97% with excellent stability over 48 h. However, when these conditions were transposed directly to an automated process on a GAIA(®) module with activities > 2 GBq, radiochemical purity dropped below 70% due to significant radiolysis. This result emphasized that conditions optimized at low activities are not directly transferable to high-activity automated production, and highlighted the crucial role of antioxidant concentration. An optimized automated method was subsequently developed, integrating a solid-phase extraction purification step, higher antioxidant levels during radiolabeling and formulation, and a larger final product volume. These changes led to radiochemical purities above 98.9% and excellent product stability over 120 h for 3 test batches. The presence of high concentrations of methionine and ascorbic acid was essential to protect against radiolysis. This work underscores the importance of adjusting radiolabeling strategies during process scale-up and confirmed that antioxidant concentration is essential for successful (177)Lu radiolabeling. The optimized automated method developed here for [(177)Lu]Lu-PSMA-ALB-56 may also be adapted to other radiopharmaceuticals in development for TRT.

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