Protein Binding by Functionalized Multiwalled Carbon Nanotubes Is Governed by the Surface Chemistry of Both Parties and the Nanotube Diameter

The protein binding propensity of nanoparticles determines their in vivo toxicity and their fate to be opsonized and cleared by human defense systems. In this work, protein-binding mechanisms of pristine and functionalized multiwalled carbon nanotubes (f-MWNTs) were investigated by varying f-MWNTs' diameters, nanotube surface chemistry, and proteins using steady-state and time-resolved fluorescence, and circular dichroism (CD) spectroscopies. The f-MWNTs with a larger diameter (∼40 nm) generally exhibited stronger protein binding compared to those with a smaller diameter (∼10 nm), demonstrating that the curvature of nanoparticles plays a key role in determining the protein binding affinity. Negative charges or steric properties on f-MWNTs enhanced binding for some proteins but not others, indicating that the electrostatic and stereochemical nature of both nanotubes and proteins govern nanotube/protein binding. Protein fluorescence lifetime was not altered by the binding while the intensity was quenched in...

[1]  W. D. de Heer,et al.  Carbon Nanotubes--the Route Toward Applications , 2002, Science.

[2]  K. Geckeler,et al.  pH-sensitive dispersion and debundling of single-walled carbon nanotubes: lysozyme as a tool. , 2006, Small.

[3]  B. Jonsson,et al.  Adsorption of Human Carbonic Anhydrase II Variants to Silica Nanoparticles Occur Stepwise: Binding Is Followed by Successive Conformational Changes to a Molten-Globule-like State , 2000 .

[4]  E Gratton,et al.  Multifrequency phase and modulation fluorometry. , 1984, Annual review of biophysics and bioengineering.

[5]  Zhuang Liu,et al.  Functionalization of carbon nanotubes via cleavable disulfide bonds for efficient intracellular delivery of siRNA and potent gene silencing. , 2005, Journal of the American Chemical Society.

[6]  Malcolm L. H. Green,et al.  Directly observed covalent coupling of quantum dots to single-wall carbon nanotubes. , 2002, Chemical communications.

[7]  M. Yumura,et al.  Selectivity of water-soluble proteins in single-walled carbon nanotube dispersions , 2006 .

[8]  L. Drain The Broadening of Magnetic Resonance Lines due to Field Inhomogeneities in Powdered Samples , 1962 .

[9]  Y. Chiang,et al.  Peptides with selective affinity for carbon nanotubes , 2003, Nature materials.

[10]  M. Paoli,et al.  Crystal structure of T state haemoglobin with oxygen bound at all four haems. , 1996, Journal of molecular biology.

[11]  K. Hidajat,et al.  Adsorption of bovine serum albumin on nanosized magnetic particles. , 2004, Journal of colloid and interface science.

[12]  S. Bachilo,et al.  Near-infrared fluorescence microscopy of single-walled carbon nanotubes in phagocytic cells. , 2004, Journal of the American Chemical Society.

[13]  Zhixin Guo,et al.  Carbon Nanotube Delivery of the GFP Gene into Mammalian Cells , 2006, Chembiochem : a European journal of chemical biology.

[14]  P. Baron,et al.  Exposure to Carbon Nanotube Material: Assessment of Nanotube Cytotoxicity using Human Keratinocyte Cells , 2003, Journal of toxicology and environmental health. Part A.

[15]  Todd Emrick,et al.  Control of protein structure and function through surface recognition by tailored nanoparticle scaffolds. , 2004, Journal of the American Chemical Society.

[16]  Zhengding Su,et al.  Conformational selectivity of peptides for single-walled carbon nanotubes. , 2006, The journal of physical chemistry. B.

[17]  T. Ebbesen,et al.  Helical Crystallization of Proteins on Carbon Nanotubes: A First Step towards the Development of New Biosensors. , 1999, Angewandte Chemie.

[18]  Jason J. Davis,et al.  The immobilisation of proteins in carbon nanotubes , 1998 .

[19]  Zhuang Liu,et al.  Carbon nanotubes as intracellular transporters for proteins and DNA: an investigation of the uptake mechanism and pathway. , 2006, Angewandte Chemie.

[20]  M. Karlsson,et al.  Protein adsorption orientation in the light of fluorescent probes: mapping of the interaction between site-directly labeled human carbonic anhydrase II and silica nanoparticles. , 2005, Biophysical journal.

[21]  M. Prato,et al.  Tissue biodistribution and blood clearance rates of intravenously administered carbon nanotube radiotracers. , 2006, Proceedings of the National Academy of Sciences of the United States of America.

[22]  M. Prato,et al.  Translocation of bioactive peptides across cell membranes by carbon nanotubes. , 2004, Chemical communications.

[23]  Chu-Young Kim,et al.  Contribution of Fluorine to Protein−Ligand Affinity in the Binding of Fluoroaromatic Inhibitors to Carbonic Anhydrase II , 2000 .

[24]  Z. Gu,et al.  Biodistribution of carbon single-wall carbon nanotubes in mice. , 2004, Journal of nanoscience and nanotechnology.

[25]  M. Prato,et al.  Functionalized carbon nanotubes for plasmid DNA gene delivery. , 2004, Angewandte Chemie.

[26]  V. Colvin The potential environmental impact of engineered nanomaterials , 2003, Nature Biotechnology.

[27]  Louis E. Brus,et al.  Binding of an Anti-Fullerene IgG Monoclonal Antibody to Single Wall Carbon Nanotubes , 2001 .

[28]  B. Schneider,et al.  Narrowing of proton NMR lines by magic angle rotation , 1970 .

[29]  H. Dai,et al.  Nanotube molecular transporters: internalization of carbon nanotube-protein conjugates into Mammalian cells. , 2004, Journal of the American Chemical Society.

[30]  G. Grüner,et al.  Charge Transfer from Adsorbed Proteins , 2004 .

[31]  J T Yang,et al.  Calculation of protein conformation from circular dichroism. , 1986, Methods in enzymology.

[32]  J. Dordick,et al.  Unfolding of ribonuclease A on silica nanoparticle surfaces. , 2007, Nano letters.

[33]  Jonathan S Dordick,et al.  Silica nanoparticle size influences the structure and enzymatic activity of adsorbed lysozyme. , 2004, Langmuir : the ACS journal of surfaces and colloids.

[34]  Bengt-Harald Jonsson,et al.  Protein adsorption onto silica nanoparticles: conformational changes depend on the particles' curvature and the protein stability. , 2004, Langmuir : the ACS journal of surfaces and colloids.

[35]  Ravi S Kane,et al.  Protein-assisted solubilization of single-walled carbon nanotubes. , 2006, Langmuir : the ACS journal of surfaces and colloids.

[36]  Kimberly Hamad-Schifferli,et al.  Gold nanoparticle-cytochrome C complexes: the effect of nanoparticle ligand charge on protein structure. , 2005, Langmuir : the ACS journal of surfaces and colloids.

[37]  L. Gauckler,et al.  Lysozyme and bovine serum albumin adsorption on uncoated silica and AlOOH-coated silica particles: the influence of positively and negatively charged oxide surface coatings. , 2005, Biomaterials.

[38]  H. Dai,et al.  Carbon nanotubes as multifunctional biological transporters and near-infrared agents for selective cancer cell destruction. , 2005, Proceedings of the National Academy of Sciences of the United States of America.

[39]  Ray H Baughman,et al.  Preparation and characterization of individual peptide-wrapped single-walled carbon nanotubes. , 2004, Journal of the American Chemical Society.

[40]  Hui Xie,et al.  Importance of aromatic content for peptide/single-walled carbon nanotube interactions. , 2005, Journal of the American Chemical Society.

[41]  M. Eftink,et al.  Fluorescence quenching studies with proteins. , 1981, Analytical biochemistry.

[42]  J. James,et al.  A Review of Carbon Nanotube Toxicity and Assessment of Potential Occupational and Environmental Health Risks , 2006, Critical reviews in toxicology.

[43]  Wei Wang,et al.  Advances toward bioapplications of carbon nanotubes , 2004 .

[44]  Laura A. Sowards,et al.  Direct measurements of interactions between polypeptides and carbon nanotubes. , 2006, The journal of physical chemistry. B.

[45]  Vincent M Rotello,et al.  Inhibition of chymotrypsin through surface binding using nanoparticle-based receptors , 2002, Proceedings of the National Academy of Sciences of the United States of America.

[46]  T. Xia,et al.  Toxic Potential of Materials at the Nanolevel , 2006, Science.

[47]  Vincent M Rotello,et al.  Tunable inhibition and denaturation of alpha-chymotrypsin with amino acid-functionalized gold nanoparticles. , 2005, Journal of the American Chemical Society.

[48]  Ravi S Kane,et al.  Structure and function of enzymes adsorbed onto single-walled carbon nanotubes. , 2004, Langmuir : the ACS journal of surfaces and colloids.

[49]  S. Curry,et al.  Structural basis of the drug-binding specificity of human serum albumin. , 2005, Journal of molecular biology.

[50]  H. Dai,et al.  Noncovalent sidewall functionalization of single-walled carbon nanotubes for protein immobilization. , 2001, Journal of the American Chemical Society.

[51]  S Fiorito,et al.  Toxicity and biocompatibility of carbon nanoparticles. , 2006, Journal of nanoscience and nanotechnology.

[52]  H. Dai,et al.  In vivo biodistribution and highly efficient tumour targeting of carbon nanotubes in mice. , 2020, Nature nanotechnology.

[53]  Lawrence F. Allard,et al.  Protein-Affinity of Single-Walled Carbon Nanotubes in Water , 2004 .

[54]  P. Sadler,et al.  Immobilization and Visualization of DNA and Proteins on Carbon Nanotubes , 1998 .

[55]  T. Steitz,et al.  Sequencing a protein by x-ray crystallography. II. Refinement of yeast hexokinase B co-ordinates and sequence at 2.1 A resolution. , 1978, Journal of molecular biology.

[56]  V. Rotello,et al.  Effect of ionic strength on the binding of alpha-chymotrypsin to nanoparticle receptors. , 2004, Langmuir : the ACS journal of surfaces and colloids.

[57]  Malcolm L. H. Green,et al.  Immobilization of Platinated and Iodinated Oligonucleotides on Carbon Nanotubes , 1997 .

[58]  M. Prato,et al.  Applications of carbon nanotubes in drug delivery. , 2005, Current opinion in chemical biology.

[59]  M. Prato,et al.  Functionalized carbon nanotubes as emerging nanovectors for the delivery of therapeutics. , 2006, Biochimica et biophysica acta.

[60]  A G Leslie,et al.  Crystal structure of uncleaved ovalbumin at 1.95 A resolution. , 1991, Journal of molecular biology.