Surface Structure of Aerobically Oxidized Diamond Nanocrystals

doi:10.1021/jp506992c

Title: Surface Structure of Aerobically Oxidized Diamond Nanocrystals

Full Record
Other Related Research

Abstract

Here we investigate the aerobic oxidation of high-pressure, high-temperature nanodiamonds (5–50 nm dimensions) using a combination of carbon and oxygen K-edge X-ray absorption, wavelength-dependent X-ray photoelectron, and vibrational spectroscopies. Oxidation at 575 °C for 2 h eliminates graphitic carbon contamination (>98%) and produces nanocrystals with hydroxyl functionalized surfaces as well as a minor component (<5%) of carboxylic anhydrides. The low graphitic carbon content and the high crystallinity of HPHT are evident from Raman spectra acquired using visible wavelength excitation (λ _excit = 633 nm) as well as carbon K-edge X-ray absorption spectra where the signature of a core–hole exciton is observed. Both spectroscopic features are similar to those of chemical vapor deposited (CVD) diamond but differ significantly from the spectra of detonation nanodiamond. Lastly, we discuss the importance of these findings to the functionalization of nanodiamond surfaces for biological labeling applications.

Authors:

Wolcott, Abraham ^[1]; Schiros, Theanne ^[2]; Trusheim, Matthew E. ^[3]; Chen, Edward H. ^[3]; Nordlund, Dennis ^[4]; Diaz, Rosa E. ^[5]; Gaaton, Ophir ^[6]; Englund, Dirk ^[3]; Owen, Jonathan S. ^[7]

Columbia Univ., New York, NY (United States). Dept. of Chemistry; Columbia Univ., New York, NY (United States). Dept. of Electrical Engineering; Columbia Univ., New York, NY (United States). Dept. of Applied Mathematics and Applied Physics; Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Electrical Engineering and Computer Science; Diamond Nanotechnologies Inc., Boston, MA (United States)
Columbia Univ., New York, NY (United States). Energy Frontier Research Center
Columbia Univ., New York, NY (United States). Dept. of Electrical Engineering; Columbia Univ., New York, NY (United States). Dept. of Applied Mathematics and Applied Physics; Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Electrical Engineering and Computer Science
SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
Columbia Univ., New York, NY (United States). Dept. of Electrical Engineering; Columbia Univ., New York, NY (United States). Dept. of Applied Mathematics and Applied Physics; Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Electrical Engineering and Computer Science; Diamond Nanotechnologies Inc., Boston, MA (United States)
Columbia Univ., New York, NY (United States). Dept. of Chemistry

Publication Date:: 2014-10-27

Research Org.:: Energy Frontier Research Centers (EFRC) (United States). Re-Defining Photovoltaic Efficiency Through Molecule Scale Control (RPEMSC); Brookhaven National Lab. (BNL), Upton, NY (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

OSTI Identifier:: 1229426

Report Number(s):: BNL-111502-2015-JA
Journal ID: ISSN 1932-7447

Grant/Contract Number:: SC00112704; W911NF-12-1-0594; SC0001085; AC02-98CH10886; HDTRA1-11-1-0022; HR0011-14-C-0018; D14PC00121; 1R43MH102942-01

Resource Type:: Accepted Manuscript

Journal Name:: Journal of Physical Chemistry. C

Additional Journal Information:: Journal Volume: 118; Journal Issue: 46; Journal ID: ISSN 1932-7447

Publisher:: American Chemical Society

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE; 77 NANOSCIENCE AND NANOTECHNOLOGY; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats


                    Wolcott, Abraham, Schiros, Theanne, Trusheim, Matthew E., Chen, Edward H., Nordlund, Dennis, Diaz, Rosa E., Gaaton, Ophir, Englund, Dirk, and Owen, Jonathan S. Surface Structure of Aerobically Oxidized Diamond Nanocrystals.  United States: N. p., 2014. 
        Web.  doi:10.1021/jp506992c.

Copy to clipboard


                    Wolcott, Abraham, Schiros, Theanne, Trusheim, Matthew E., Chen, Edward H., Nordlund, Dennis, Diaz, Rosa E., Gaaton, Ophir, Englund, Dirk, & Owen, Jonathan S. Surface Structure of Aerobically Oxidized Diamond Nanocrystals.  United States.  doi:10.1021/jp506992c.

Copy to clipboard


                    Wolcott, Abraham, Schiros, Theanne, Trusheim, Matthew E., Chen, Edward H., Nordlund, Dennis, Diaz, Rosa E., Gaaton, Ophir, Englund, Dirk, and Owen, Jonathan S. Mon .  
        "Surface Structure of Aerobically Oxidized Diamond Nanocrystals".  United States.  doi:10.1021/jp506992c.  https://www.osti.gov/servlets/purl/1229426.

Copy to clipboard


                    
@article{osti_1229426,

  title        = {Surface Structure of Aerobically Oxidized Diamond Nanocrystals},

  author       = {Wolcott, Abraham and Schiros, Theanne and Trusheim, Matthew E. and Chen, Edward H. and Nordlund, Dennis and Diaz, Rosa E. and Gaaton, Ophir and Englund, Dirk and Owen, Jonathan S.},

  abstractNote = {Here we investigate the aerobic oxidation of high-pressure, high-temperature nanodiamonds (5–50 nm dimensions) using a combination of carbon and oxygen K-edge X-ray absorption, wavelength-dependent X-ray photoelectron, and vibrational spectroscopies. Oxidation at 575 °C for 2 h eliminates graphitic carbon contamination (>98%) and produces nanocrystals with hydroxyl functionalized surfaces as well as a minor component (<5%) of carboxylic anhydrides. The low graphitic carbon content and the high crystallinity of HPHT are evident from Raman spectra acquired using visible wavelength excitation (λexcit = 633 nm) as well as carbon K-edge X-ray absorption spectra where the signature of a core–hole exciton is observed. Both spectroscopic features are similar to those of chemical vapor deposited (CVD) diamond but differ significantly from the spectra of detonation nanodiamond. Lastly, we discuss the importance of these findings to the functionalization of nanodiamond surfaces for biological labeling applications.},

  doi          = {10.1021/jp506992c},

  journal      = {Journal of Physical Chemistry. C},

  number       = 46,

  volume       = 118,

  place        = {United States},

  year         = {2014},

  month        = {10}

}

Copy to clipboard

Journal Article:

Free Publicly Available Full Text

Accepted Manuscript (DOE)

Publisher's Version of Record

DOI: 10.1021/jp506992c

Other availability

Search WorldCat to find libraries that may hold this journal

Citation Metrics:

Cited by: 18 works

Citation information provided by
Web of Science

Save / Share:

Export Metadata

Save to My Library

Similar Records in DOE PAGES and OSTI.GOV collections:

Surface Structure of Aerobically Oxidized Diamond Nanocrystals

Journal Article Wolcott, Abraham ; Schiros, Theanne ; Trusheim, Matthew E. ; ... - Journal of Physical Chemistry. C
DOI: 10.1021/jp506992c
Surface Structure Dependence of SO ₂ Interaction with Ceria Nanocrystals with Well-defined Surface Facets

Journal Article Tumuluri, Uma ; Li, Meijun ; Cook, Brandon G. ; ... - Journal of Physical Chemistry. C

The effects of the surface structure of ceria (CeO ₂) on the nature, strength, and amount of species resulting from SO ₂ adsorption were studied using in situ IR and Raman spectroscopies coupled with mass spectrometry, along with first-principles calculations based on density functional theory (DFT). CeO ₂ nanocrystals with different morphologies, namely, rods (representing a defective structure), cubes (100 facet), and octahedra (111 facet), were used to represent different CeO ₂ surface structures. IR and Raman spectroscopic studies showed that the structure and binding strength of adsorbed species from SO ₂ depend on the shape of the CeO ₂more »« less
Cited by 8
DOI: 10.1021/acs.jpcc.5b07946

Full Text Available
The surface structure of silver-coated gold nanocrystals and its influence on shape control

Journal Article Padmos, J. Daniel ; Personick, Michelle L. ; Tang, Qing ; ... - Nature Communications

Understanding the surface structure of metal nanocrystals with specific facet indices is important due to its impact on controlling nanocrystal shape and functionality. However, this is particularly challenging for halide-adsorbed nanocrystals due to the difficulty in analysing interactions between metals and light halides (for example, chloride). Here we uncover the surface structures of chloride-adsorbed, silver-coated gold nanocrystals with {111}, {110}, {310} and {720} indexed facets by X-ray absorption spectroscopy and density functional theory modelling. The silver–chloride, silver–silver and silver–gold bonding structures are markedly different between the nanocrystal surfaces, and are sensitive to their formation mechanism and facet type. A uniquemore »« less
Cited by 17
DOI: 10.1038/ncomms8664

Full Text Available
Surface-structure sensitivity of CeO ₂ nanocrystals in photocatalysis and enhancing the reactivity with nanogold

Journal Article Lei, Wanying ; Zhang, Tingting ; Gu, Lin ; ... - ACS Catalysis

Structure–function correlations are a central theme in heterogeneous (photo)catalysis. In this research, using aberration-corrected scanning transmission electron microscopy (STEM), the atomic surface structures of well-defined one-dimensional (1D) CeO ₂ nanorods (NRs) and 3D nanocubes (NCs) are directly visualized at subangstrom resolution. CeO ₂ NCs predominantly expose the {100} facet, with {110} and {111} as minor cutoff facets at the respective edges and corners. Notably, the outermost surface layer of the {100} facet is nearly O-terminated. Neither surface relaxations nor reconstructions on {100} are observed, indicating unusual polarity compensation, which is primarily mediated by near-surface oxygen vacancies. The surface of CeOmore »« less
Cited by 38
DOI: 10.1021/acscatal.5b00620

Full Text Available
New insights into the growth mechanism and surface structure of palladium nanocrystals

Journal Article Lim, Byungkwon ; Kobayashi, Hirokazu ; Camargo, Pedro H. C. ; ... - Nano Research

Our paper presents a systematic study of the growth mechanism for Pd nanobars synthesized by reducing Na ₂PdCl ₄ with L-ascorbic acid in an aqueous solution in the presence of bromide ions as a capping agent. Transmission electron microscopy (TEM) and high-resolution TEM analyses revealed that the growth at early stages of the synthesis was dominated by particle coalescence, followed by shape focusing via recrystallization and further growth via atomic addition. We investigated the detailed surface structure of the nanobars using aberration-corrected scanning TEM and found that the exposed {100} surfaces contained several types of defects such as an adatommore »« less
DOI: 10.1007/s12274-010-1021-5

Full Text Available

Similar Records