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This prospective proof-of-principle study aimed to determine whether [68Ga]Ga-Pentixafor uptake, which reflects CXCR4 expression, is higher in the bone marrow of chronic lymphocytic leukemia (CLL) than in other oncological diseases without bone marrow infiltration and can therefore be used for CLL imaging.Thirteen CLL patients and 20 controls (10 with pancreatic adenocarcinoma and 10 with mucosa-associated lymphoid tissue lymphoma) with histologically proven cancer underwent [68Ga]Ga-Pentixafor positron emission tomography/magnetic resonance imaging. Standardized [68Ga]Ga-Pentixafor uptake values (SUVmax, SUVmean) were measured in the bone marrow of the pelvis, the lumbar vertebra L4, and the bony structure with the visually highest tracer uptake (“hottest lesion”). Mean apparent diffusion coefficient values were also measured in the pelvis. Serum leukocyte count (gram per liter), lymphocyte percentage (percent), lactate dehydrogenase (unit per liter), β2-microglobulin (milligram per deciliter), and C-reactive protein (milligram per deciliter) were measured. Statistical analyses comprised analysis of variance with Games-Howell post hoc tests and Spearman correlation coefficients.SUVmax and SUVmean differed significantly between CLL and pancreatic adenocarcinoma in the pelvis (P = 0.032 and P = 0.008) and lumbar vertebra L4 (both P < 0.001). SUVmean also differed in the pelvis (P = 0.020) and L4 (P = 0.041), and SUVmax in L4 (P = 0.019), between CLL and mucosa-associated lymphoid tissue lymphoma. Receiver operating characteristic–based areas under the curve for separation of CLL from the control groups were greatest for the SUVmax of the bony structure with the strongest [68Ga]Ga-Pentixafor uptake (0.94) and the SUVmax of L4 (0.92). There was no significant correlation between [68Ga]Ga-Pentixafor uptake and pelvic apparent diffusion coefficients or serum parameters.[68Ga]Ga-Pentixafor positron emission tomography/magnetic resonance imaging may possibly be useful for CXCR4-based CLL imaging.