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Title: Nano-gold corking and enzymatic uncorking of carbon nanotube cups

Because of their unique stacked, cup-shaped, hollow compartments, nitrogen-doped carbon nanotube cups (NCNCs) have promising potential as nanoscale containers. Individual NCNCs are isolated from their stacked structure through acid oxidation and subsequent probe-tip sonication. The NCNCs are then effectively corked with gold nanoparticles (GNPs) by sodium citrate reduction with chloroauric acid, forming graphitic nanocapsules with significant surface-enhanced Raman signature. Mechanistically, the growth of the GNP corks starts from the nucleation and welding of gold seeds on the open rims of NCNCs enriched with nitrogen functionalities, as confirmed by density functional theory calculations. A potent oxidizing enzyme of neutrophils, myeloperoxidase (MPO), can effectively open the corked NCNCs through GNP detachment, with subsequent complete enzymatic degradation of the graphitic shells. Lastly, this controlled opening and degradation was further carried out in vitro with human neutrophils. In addition, the GNP-corked NCNCs were demonstrated to function as novel drug delivery carriers, capable of effective (i) delivery of paclitaxel to tumor-associated myeloid-derived suppressor cells (MDSC), (ii) MPO-regulated release, and (iii) blockade of MDSC immunosuppressive potential.
Authors:
 [1] ;  [1] ;  [1] ;  [2] ;  [1] ;  [3] ;  [3] ;  [1] ;  [1]
  1. Univ. of Pittsburgh, Pittsburgh, PA (United States)
  2. National Energy Technology Lab. (NETL), Pittsburgh, PA, (United States)
  3. Univ. of Pittsburgh Medical Center, Pittsburgh, PA (United States)
Publication Date:
OSTI Identifier:
1186638
Report Number(s):
A-UNIV-PUB--122
Journal ID: ISSN 0002-7863
Grant/Contract Number:
0954345; R01CA154369; R01ES019304; NIOSH OH008282; HL114453; U19 AI068021
Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 137; Journal Issue: 2; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Research Org:
National Energy Technology Lab. (NETL), Pittsburgh, PA, (United States)
Sponsoring Org:
USDOE
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 60 APPLIED LIFE SCIENCES; 59 BASIC BIOLOGICAL SCIENCES; 77 NANOSCIENCE AND NANOTECHNOLOGY