Zhu Hongshan, Heinitz Stephan, Binnemans Koen, Mullens Steven, Cardinaels Thomas
Belgian Nuclear Research Centre (SCK CEN), Institute for Nuclear Materials Science, Boeretang 200, Mol B-2400, Belgium.
KU Leuven, Department of Chemistry, Celestijnenlaan 200F, P.O. 2404, Leuven B-3001, Belgium.
ACS Omega. 2024 Dec 16;9(52):51009-51021. doi: 10.1021/acsomega.4c05457. eCollection 2024 Dec 31.
Separation of high-activity Bi from Ac for targeted alpha therapy is challenging due to the instability of existing sorbents. Surface-modified carbon materials have shown promise for use in inverse Ac/Bi generators. However, previously reported materials with irregular shapes may limit their applications in column separations. In contrast, spherical particles are expected to be more suitable for column chromatography compared to irregular powders as they can ensure uniform flow patterns, lower pressure drop, and effective packing. To address this limitation, a method was developed for the synthesis of spherical carbon beads via the carbonization of cellulose beads. Subsequently, surface modification on the spherical carbon beads was performed via sulfonation or oxidation of the carbon beads. Batch sorption experiments were conducted to assess their selective sorption toward Bi over La (as a surrogate of Ac) by varying the concentrations of HNO and NaNO. It was found that the selective sorption of Bi onto spherical surface-modified carbon beads could be achieved by adjusting the concentrations of HNO and NaNO. Furthermore, the sorption capacity of Bi decreased as the concentration of HCl increased due to the formation of bichloride complexes and the H competition. This implies that Bi can be effectively eluted from the spherical surface-modified carbon beads when using HCl as the eluate. Consequently, spherical surface-modified carbon beads show potential as alternative adsorbents for inverse Ac/Bi generators.
由于现有吸附剂的不稳定性，从锕中分离高活性铋用于靶向α治疗具有挑战性。表面改性的碳材料已显示出在反向锕/铋发生器中使用的潜力。然而，先前报道的形状不规则的材料可能会限制它们在柱分离中的应用。相比之下，球形颗粒预计比不规则粉末更适合柱色谱，因为它们可以确保均匀的流动模式、更低的压降和有效的填充。为了解决这一限制，开发了一种通过纤维素珠碳化合成球形碳珠的方法。随后，通过对碳珠进行磺化或氧化对球形碳珠进行表面改性。通过改变硝酸和亚硝酸钠的浓度进行批量吸附实验，以评估它们对铋相对于镧（作为锕的替代物）的选择性吸附。发现通过调节硝酸和亚硝酸钠的浓度可以实现铋在球形表面改性碳珠上的选择性吸附。此外，由于形成二氯化物络合物和氢离子竞争，随着盐酸浓度的增加，铋的吸附容量降低。这意味着当使用盐酸作为洗脱液时，可以从球形表面改性碳珠上有效地洗脱铋。因此，球形表面改性碳珠显示出作为反向锕/铋发生器替代吸附剂的潜力。
