Abstract
When nanoparticles interact with cellular or organelle membranes, the coating ligands are known to affect the integrity of the membranes, which regulate cell death and inflammation. However, the molecular mechanisms of this modulation remain unresolved. Here, we use synchrotron X-ray liquid surface scattering and molecular dynamics simulations to study interface structures between phospholipids and gold nanorods (AuNRs) coated by surfactant and polyelectrolyte. These ligands are two types of widely used surface modification with different self-assembled structures and stabilities on the surface of nanoparticles. We reveal distinct mechanisms of the ligand stability in disrupting membrane integrity. We find that the cationic surfactant ligand cetyltrimethylammonium bromide detaches from the AuNRs and inserts into phospholipids, resulting in reduced membrane thickness by compressing the phospholipids to align with the shorter ligand. Conversely, the cationic polyelectrolyte ligand poly(diallyldimethylammonium chloride) is more stable on AuNRs; although it adsorbs onto the membrane, it does not cause much impairment. The distinct coating ligand interactions with phospholipids are further verified by cellular responses including impaired lysosomal membranes and triggered inflammatory effects in macrophages. Together, the quantitative analysis of interface structures elucidates key bio-nano interactions and highlights the importance of surface ligand stability for safety and rational design of nanoparticles.
Original language | English |
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Pages (from-to) | 8680-8693 |
Number of pages | 14 |
Journal | ACS Nano |
Volume | 13 |
Issue number | 8 |
DOIs | |
State | Published - Aug 27 2019 |
Externally published | Yes |
Funding
This work was supported by the Ministry of Science and Technology of China (2016YFA0201600 2016YFA0203200), Key Program for International S&T Cooperation Projects of China (2016YFE0133100), the National Natural Science Foundation of China (91543206, 11435002, 11574224), Science Fund for Creative Research Groups of the National Natural Science Foundation of China (11621505), the National Science Fund for Distinguished Young Scholars (11425520), CAS Key Research Program for Frontier Sciences (QYZDJ-SSW-SLH022) and the CAS Interdisciplinary Innovation Team. We appreciate the assistance by BL07W in NSRL and the Users with Excellence Project of Hefei Science Center CAS (2018HSC-UE004). A part of this work was supported by NSF's ChemMatCARS Sector 15, which is supported by the Divisions of Chemistry (CHE) and Materials Research (DMR), National Science Foundation, under grant number NSF/CHE-1834750. Use of the Advanced Photon Source, an Office of Science User Facility operated for the U.S. Department of Energy (DOE) Office of Science by Argonne National Laboratory, was supported by the U.S. DOE under Contract No. DE-AC02-06CH11357. B.L. acknowledges the support from the University of Chicago MRSEC under grant number NSF/DMR-1420709. R.Z. acknowledges the support from IBM Blue Gene Science Program (W125859, W1464125, and W1464164). This work was supported by the Ministry of Science and Technology of China (2016YFA0201600, 2016YFA0203200), Key Program for International S&T Cooperation Projects of China (2016YFE0133100), the National Natural Science Foundation of China (91543206, 11435002, 11574224), Science Fund for Creative Research Groups of the National Natural Science Foundation of China (11621505), the National Science Fund for Distinguished Young Scholars (11425520), CAS Key Research Program for Frontier Sciences (QYZDJ-SSW-SLH022), and the CAS Interdisciplinary Innovation Team. We appreciate the assistance by BL07W in NSRL and the Users with Excellence Project of Hefei Science Center CAS (2018HSC-UE004). A part of this work was supported by NSF’s ChemMatCARS Sector 15, which is supported by the Divisions of Chemistry (CHE) and Materials Research (DMR), National Science Foundation, under grant number NSF/CHE-1834750. Use of the Advanced Photon Source, an Office of Science User Facility operated for the U.S. Department of Energy (DOE) Office of Science by Argonne National Laboratory, was supported by the U.S. DOE under Contract No. DE-AC02-06CH11357. B.L. acknowledges the support from the University of Chicago MRSEC under grant number NSF/DMR-1420709. R.Z. acknowledges the support from IBM Blue Gene Science Program (W125859, W1464125, and W1464164).
Keywords
- X-ray liquid surface scattering
- gold nanorod
- ligand stability
- membrane integrity
- phospholipid