Production of Endohedral Fullerenes by Ion Implantation

Diener, M.D. ; Alford, J. M. ; Mirzadeh, S.

关键词: ALPHA DECAY;    ATOMS;    BISMUTH 212;    BISMUTH 213;    CAPTURE;    CATABOLISM;    CHEMISTRY;    CONTAINMENT;    ENERGY TRANSFER;    FULLERENES;    ION BEAMS;    ION IMPLANTATION;    LEAD 212;    LUTETIUM 177;    MODIFICATIONS;    NEUTRON REACTIONS;    RADIOIMMUNOTHERAPY;    RADIOI;   

DOI  :  10.2172/940291
RP-ID  :  ORNL01-0624
PID  :  OSTI ID: 940291
Others  :  TRN: US201206%%1

学科分类：材料科学（综合）

美国|英语

来源: SciTech Connect

【 摘 要 】

The empty interior cavity of fullerenes has long been touted for containment of radionuclides during in vivo transport, during radioimmunotherapy (RIT) and radioimaging for example. As the chemistry required to open a hole in fullerene is complex and exceedingly unlikely to occur in vivo, and conformational stability of the fullerene cage is absolute, atoms trapped within fullerenes can only be released during extremely energetic events. Encapsulating radionuclides in fullerenes could therefore potentially eliminate undesired toxicity resulting from leakage and catabolism of radionuclides administered with other techniques. At the start of this project however, methods for production of transition metal and p-electron metal endohedral fullerenes were completely unknown, and only one method for production of endohedral radiofullerenes was known. They therefore investigated three different methods for the production of therapeutically useful endohedral metallofullerenes: (1) implantation of ions using the high intensity ion beam at the Oak Ridge National Laboratory (ORNL) Surface Modification and Characterization Research Center (SMAC) and fullerenes as the target; (2) implantation of ions using the recoil energy following alpha decay; and (3) implantation of ions using the recoil energy following neutron capture, using ORNL's High Flux Isotope Reactor (HFIR) as a thermal neutron source. While they were unable to obtain evidence of successful implantation using the ion beam at SMAC, recoil following alpha decay and neutron capture were both found to be economically viable methods for the production of therapeutically useful radiofullerenes. In this report, the procedures for preparing fullerenes containing the isotopes {sup 212}Pb, {sup 212}Bi, {sup 213}Bi, and {sup 177}Lu are described. None of these endohedral fullerenes had ever previously been prepared, and all of these radioisotopes are actively under investigation for RIT. Additionally, the chemistry for derivatizing the radiofullerenes for water-solubility and a method for removing exohedral radionuclides are reported. The methods and chemistry developed during this CRADA are the crucial first steps for the development of fullerenes as a method superior to existing technologies for in vivo transport of radionuclides.