NASA Technical Reports Server (NTRS) 20120001618: Separation medium containing thermally exfoliated graphite oxide

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United States Patent
(12) (lo) Patent No.: US 8,105,976 B2
Prud'homme et al. (45) Date of Patent: *Jan. 31, 2012
(54) SEPARATION MEDIUM CONTAINING 2004/0127621 Al 7/2004 Drzal et al.
THERMALLY EXFOLIATED GRAPHITE 2005/0271574 Al 12/2005 Jang et al.
2006/0121279 Al 6/2006 Petrik
OXIDE
2006/0229404 Al 10/2006 Lechtenboehmer
2007/0142547 Al 6/2007 Vaidya et al.
(75) Inventors: Robert K. Prud'homme, Lawrenceville, 2009/0123752 Al 5/2009 Prud'homme et al.
NJ (US); Ilhan A. Aksay, Princeton, NJ 2009/0233057 Al 9/2009 Aksay et al.
2010/0096595 Al 4/2010 Prud'homme et al.
(US); Margarita Herrera-Alonso, Col.
Valle Tepepan (MX) FOREIGN PATENT DOCUMENTS
JP 2006-225473 8/2006
(73) Assignee: The Trustees of Princeton University,
OTHER PUBLICATIONS
Princeton, NJ (US)
U.S. Appl. No. 12/208,706, filed Sep. 11, 2008, Aksay.
(*) Notice: Subject to any disclaimer, the term of this U.S. Appl. No. 12/208,692, filed Sep. 11, 2008, Korkut, et al.
patent is extended or adjusted under 35 U.S. Appl. No. 12/194,030, filed Aug. 19, 2008, Prud'homme, et al.
U.S.C. 154(b) by 460 days. U.S. Appl. No. 12/194,054, filed Aug. 19, 2008, Prud'homme, et al.
U.S. Appl. No. 12/194,037, filed Aug. 19, 2008, Prud'homme, et al.
This patent is subject to a terminal dis- U.S. Appl. No. 12/194,043, filed Aug. 19, 2008, Prud'homme, et al.
claimer. U.S. Appl. No. 12/194,007, filed Aug. 19, 2008, Prud'homme, et al.
U.S. Appl. No. 12/194,062, filed Aug. 19, 2008, Prud'homme, et al.
U.S. Appl. No. 12/194,016, filed Aug. 19, 2008, Prud'homme, et al.
(21) Appl. No.: 12/208,682
U.S. Appl. No. 12/194,021, filed Aug. 19, 2008, Prud'homme, et al.
L Bautista, et al., "Localizaed N2 Adsorption on Graphites, Graphite
(22) Filed: Sep.11, 2008
Oxides and Exfoliated Graphites", Materials Chemistry and Physics,
vol. 21, No. 4, 1989, pp. 335-343.
(65) Prior Publication Data
P. Ramesh, et al., "Preparation and physicochemical and electro-
US 2009/0123752 Al May 14, 2009 chemical characterization of exfoliated graphite oxide", Journal of
Colloid and Interface Science, vol. 274, 2004, pp. 95-102.
U.S. Appl. No. 12/791,190, filed Jun. 1, 2010, Prund'homme, et al.
Related U.S. Application Data
U.S. Appl. No. 12/866,089, filed Aug. 4, 2010, Crain, et al.
(63) Continuation of application No. 11/249,404, filed on U.S. Appl. No. 12/866,079, filed Aug. 4, 2010, Crain, et al.
Oct. 14, 2005, now Pat. No. 7,658,901. Celzard, et al., "Modelling of Exfoliated Graphite", Progress in
Materials Science (www.elsevier.com/locat/pmatsci), Jan. 1, 2004,
(51) Int. Cl. pp. 1-87.
"Graphite", http://web.archive.org/web/20050827075854/http://en .
C01B 31104 (2006.01)
wikipedia.org/wilci/Graphite, Aug. 20, 2005, 3 pp.
(52) U.S. Cl . ........................................ 502/400; 502/416
U.S. Appl. No. 12/866,306, filed Aug. 5, 2010, Aksay, et al.
(58) Field of Classification Search .................. 423/448; Office Action issued Jul. 26, 2011 in Indian Patent Application No.
502/400, 416 2672/DELNP/2008.
See application file for complete search history. U.S. Appl. No. 12/945,043, filed Nov. 12, 2010, Pan, et al.
U.S. Appl. No. 13/077,070, filed Mar. 31, 2011, Prud'homme, et al.
(56) References Cited
Primary Examiner Stuart Hendrickson
U.S. PATENT DOCUMENTS (74) Attorney, Agent, or Firm Oblon, Spivak,
McClelland, Maier & Neustadt, L.L.P.
4,987,175 A 1/1991 Bunnell, Sr.
5,019,446 A 5/1991 Bunnell, Sr.
5,065,948 A 11/1991 Bunnell, Sr. (57) ABSTRACT
5,876,687 A 3/1999 Hung
A separation medium, such as a chromatography filling or
6,596,396 B2 7/2003 Hirata et al.
6,828,015 B2 12/2004 Hirata et al. packing, containing a modified graphite oxide material,
6,927,250 B2 8/2005 Kaschak et al. which is a thermally exfoliated graphite oxide with a surface
7,071,258 B1 7/2006 Jang et al. area of from about 300 m2/g to 2600 m2/g, wherein the
7,105,108 B2 9/2006 Kaschak et al.
thermally exfoliated graphite oxide has a surface that has
7,658,901 B2 2/2010 Prud'homme et al.
been at least partially functionalized.
7,745,528 B2 6/2010 Prud'homme et al.
7,771,824 B2 8/2010 Herrera-Alonso et al.
2002/0054995 Al 5/2002 Mazurkiewicz 15 Claims, 22 Drawing Sheets
U.S. Patent Jan. 31, 2012 Sheet 1 of 22 US 8,105,976 B2
4, A

17-46 5.84 61" 4A4 3." 2AS
9
3
4)h
413h

96 h
c
120h
240 h

s +o +s xa 26 30
20
1
FIG.
U.S. Patent Jan. 31, 2012 Sheet 2 of 22 US 8,105,976 B2
U.S. Patent
Jan. 31, 2012 Sheet 3 of 22 US 8,105,976 B2
x---8 a-.'8 ....I
tea..
CO P oc
E
d^^ta4m ^^C°t4
i
C 0 COOS
xp. _.p^...(_.t.:l.Y ) .Y........ Y -------- ------l' ------ .t.... .... -Y F
200 150 100 50
FIG,
U.S. Patent Jan. 31, 2012 Sheet 4 of 22 US 8,105,976 B2
Q
LO
CO
C9
to
C4
W7
U.S. Patent Jan. 31, 2012 Sheet 5 of 22 US 8,105,976 B2
U.S. Patent
Jan. 31, 2012 Sheet 6 of 22 US 8,105,976 B2
vco
c^U
200 400 600 800 3000
(C)
Exfoliation temperature
FIG. 6
U.S. Patent Jan. 31, 2012 Sheet 7 of 22 US 8,105,976 B2
U.S. Patent Jan. 31, 2012 Sheet 8 of 22 US 8,105,976 B2
U.S. Patent ,Tan. 31, 2012 Sheet 9 of 22 US 8,105,976 B2
C-C
5000
4000
3000
5 2000 C-0 or C 0-C
dCW
1000
r
r
0
280 284 288 292
B. E. (eV)
FIG. 9