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Reductive microenvironment responsive gadolinium-based polymers as potential safe MRI contrast agents.

Shiwei Guo1, Xueyang Xiao, Xiaoming Wang

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Area of Science:

  • Biomaterials Science
  • Nanotechnology
  • Radiology and Medical Imaging

Background:

  • Gadolinium-based contrast agents (GBCAs) carry risks of nephrogenic systemic fibrosis and gadolinium deposition due to free Gd(iii) ion release.
  • Existing nano-scale contrast agents can lead to adverse effects, necessitating safer formulations with reduced Gd(iii) retention.
  • Macromolecular MRI contrast agents (Gd-mCAs) offer a potential strategy to mitigate these risks while maintaining diagnostic efficacy.

Purpose of the Study:

  • To develop novel biodegradable Gd-mCAs with reduced Gd(iii) retention and sufficient imaging contrast for tumor diagnosis.
  • To synthesize poly[N-(1,3-dihydroxypropyl)methacrylamide] (pDHPMA) copolymers for conjugating Gd-chelates.
  • To evaluate the safety and efficacy of Gd-mCAs conjugated via sulfide or GSH-sensitive disulfide bonds.

Main Methods:

  • Synthesized biodegradable pDHPMA copolymers using DHPMA monomer and GFLG peptide chain transfer agent.
  • Conjugated small molecular Gd-DOTA to the pDHPMA backbone via sulfide or GSH-sensitive disulfide bonds, creating pDHPMA-Cy5.5-DOTA-Gd and pDHPMA-Cy5.5-SS-DOTA-Gd.
  • Assessed relaxivity and Gd(iii) retention times of the novel Gd-mCAs compared to DTPA-Gd.

Main Results:

  • Novel Gd-mCAs exhibited significantly higher relaxivities (10.49 and 10.24 mM-1 s-1) than DTPA-Gd (3.97 mM-1 s-1).
  • The pDHPMA-Cy5.5-SS-DOTA-Gd showed shorter Gd(iii) retention time compared to pDHPMA-Cy5.5-DOTA-Gd, while maintaining contrast efficacy.
  • Biodegradable pDHPMA copolymers proved effective carriers for Gd-chelates, demonstrating potential for safer MRI contrast agents.

Conclusions:

  • Conjugating Gd-chelates to biodegradable macromolecular carriers via disulfide bonds is an effective strategy for safer MRI contrast agents.
  • The developed Gd-mCAs show promise for reducing adverse effects associated with free Gd(iii) ion release in MRI diagnostics.
  • This formulation approach offers a pathway to improved safety profiles for gadolinium-based MRI contrast agents.