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(12) United States Patent (10) Patent No.: US 7,618,725 B2 Masel Et Al

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(12) United States Patent (10) Patent No.: US 7,618,725 B2 Masel Et Al US007618725B2 (12) United States Patent (10) Patent No.: US 7,618,725 B2 Masel et al. (45) Date of Patent: Nov. 17, 2009 (54) LOW CONTAMINANT FORMIC ACID FUEL 3,983,010 A * 9, 1976 Rauch et al. .................. 203/15 FOR DIRECT LIQUID FUEL CELL 4,126,748 A 11, 1978 Scholz 4,262,140 A 4, 1981. Bott (75) Inventors: Richard I. Masel, Champaign, IL (US); 5,294,740 A * 3/1994 Kiefer et al. ................ 562/609 5,393,922 A 2, 1995 Sen Yimin Zhu, Urbana, IL (US); Zakia 5,599.979 A 2/1997 Berg Kahn, Palatine, IL (US); Malcolm Man, 5,633,402 A 5/1997 Berg Vancouver (CA) 5,763,662 A 6/1998 Ikariya 5,869,739 A 2/1999 Ikariya (73) Assignee: The Board of Trustees of the 5,879,915 A 3, 1999 Loubiere University of Illinois, Urbana, IL (US) 5,904,740 A * 5/1999 Davis .......................... 44,385 2003/0050506 A1 3/2003 Auer et al. (*) Notice: Subject to any disclaimer, the term of this 2003/0198852 A1 10, 2003 Masel et al. .................. 429/30 patent is extended or adjusted under 35 U.S.C. 154(b) by 550 days. OTHER PUBLICATIONS Yiminet al., High power density direct formic acid fuel cells, Journal (21) Appl. No.: 11/079,893 of Power Sources 130 (2004) 8-14.* (22) Filed: Mar. 14, 2005 (Continued) (65) Prior Publication Data Primary Examiner Patrick Ryan Assistant Examiner Thomas H. Parsons US 2006/OO597.69 A1 Mar. 23, 2006 (74) Attorney, Agent, or Firm Greer, Burns & Crain, Ltd. Related U.S. Application Data (57) ABSTRACT (60) Provisional application No. 60/611,906, filed on Sep. A low contaminant formic acid fuel is especially Suited 21, 2004. toward use in a direct organic liquid fuel cell. A fuel of the invention provides high power output that is maintained for a (51) Int. Cl. substantial time and the fuel is substantially non-flammable. HIM S/ (2006.01) Specific contaminants and contaminant levels have been C06B 33/00 (2006.01) identified as being deleterious to the performance of a formic CIOL I/30 (2006.01) acid fuel in a fuel cell, and embodiments of the invention (52) U.S. Cl. .............................. 429/12: 44/251; 44/358 provide low contaminant fuels that have improved perfor (58) Field of Classification Search ................... 429/12: mance compared to known commercial bulk grade and com 44/251, 358 mercial purified grade formic acid fuels. Preferred embodi See application file for complete search history. ment fuels (and fuel cells containing Such fuels) including (56) References Cited low levels of a combination of key contaminants, including acetic acid, methyl formate, and methanol. U.S. PATENT DOCUMENTS 2,407,157 A 9/1946 Hyde 8 Claims, 5 Drawing Sheets US 7,618,725 B2 Page 2 OTHER PUBLICATIONS BASF 90%. Formic Acid, Unknown. Orbiter WABE 18-2 Formic Acid, Unknown. Rice et al., Direct formic acid fuel cells, Journal of Power Sources Reidel Puriss Grade Formic Acid, Unknown. 111 (2002) 83-89.* BASF Corporation Formic Acid 88% Technical Data Sheet, Jan. GFS Double Distiller Formic Acid, Unknown. 2006. Aldrich ACS Grade Formic Acid, Unknown. * cited by examiner U.S. Patent Nov. 17, 2009 Sheet 2 of 5 US 7,618,725 B2 N 3 U.S. Patent Nov. 17, 2009 Sheet 3 of 5 US 7,618,725 B2 a)SÐ, wow --i- U.S. Patent Nov. 17, 2009 Sheet 4 of 5 US 7,618,725 B2 0"| | uo Wu Ov (D (W) e6elow U.S. Patent Nov. 17, 2009 Sheet 5 of 5 US 7,618,725 B2 V+pe?lejeud{ |---- |---- | ----------------+---------- (OldH)WH||…)THoew*spoorGiaº* (sunou)ºu?L A CSO (D (uo w) Al-Isued Jueluno US 7,618,725 B2 1. 2 LOW CONTAMINANT FORMIC ACID FUEL While fuel cells will have different configurations for dif FOR DIRECT LIQUID FUEL CELL ferent applications, the compact fuel cells will be suitable for replacement in Small portable electronics, e.g., cellular hand PRIORITY CLAIM sets and personal digital assistants (PDAs). As an example, 5 cellular handsets typically require a certain amount of power This application claims priority under 35 U.S.C. S 119 of (usually 3 watts) which should fit within a cavity of approxi application Ser. No. 60/611,906 filed Sep. 21, 2004. mately 10 cc to 30 cc. In order for a fuel cell technology to accomplish this, it must have the capability of operating at a STATEMENT OF GOVERNMENT INTEREST high power density. Direct formic acid fuel cells in accor 10 dance with embodiments of the 852 publication and the 518 This invention was made with Government assistance publication have been demonstrated as suitable to deliver under Department of Energy Grant No. DEGF-02 such power in the small form factor suited to small portable 99ER14993. The Government has certain rights in the inven electronics. tion. Commercial bulk grades of formic acid are made by a FIELD OF THE INVENTION 15 number of processes. Processes for making formic acid are disclosed in U.S. Pat. Nos. 5,879,915, 5,869,739, 5,763,662, The field of the invention is liquid organic fuels. A fuel of 5,633,402, 5,599,979, 5,393,922, 4,262,140, 4,126,748 and the invention is applicable, for example, to direct liquid feed 2,407,157. Commercial bulk grades of formic acid are used in electrochemical fuel cells. a variety of industries and processes. It is used, for example in animal feed additives, to dye clothing, and in the manufacture BACKGROUND of vinyl resin plastics. It is also used to manufacture aspar tame. There are also commercial purified grades of formic Fuel cells are electrochemical cells in which a free energy acid. The commercial purified grades have a smaller market. change resulting from a fuel oxidation reaction is converted The commercial purified grades are used, for example, as a into electrical energy. End uses for fuel cells include battery 25 Solvent in high performance liquid chromatography (HPLC) replacement, mini- and microelectronics, automotive engines and as solvents for other measurement techniques. and other transportation power generators, power plants, and many others. One advantage of fuel cells is that they are SUMMARY OF THE INVENTION substantially pollution-free. In hydrogen/oxygen fuel cells, hydrogen gas is oxidized to 30 A low contaminant formic acid fuel is especially Suited form water, with a useful electrical current produced as a toward use in a direct organic liquid fuel cell. A fuel of the byproduct of the oxidation reaction. A solid polymer mem invention provides high power output that is maintained for a brane electrolyte layer can be employed to separate the hydro substantial time and the fuel is substantially non-flammable. gen fuel from the oxygen. The anode and cathode are Specific contaminants and contaminant levels have been arranged on opposite faces of the membrane. Electron flow 35 identified as being deleterious to the performance of a formic along the electrical connection between the anode and the acid fuel in a fuel cell, and embodiments of the invention cathode provides electrical power to load(s) interposed in provide low contaminant fuels that have improved perfor circuit with the electrical connection between the anode and mance compared to known commercial bulk grade and com the cathode. Hydrogen fuel cells are impractical for many mercial purified grade formic acid fuels. Preferred embodi applications, however, because of difficulties related to stor 40 ment fuels (and fuel cells containing Such fuels) including ing and handling hydrogen gas. low levels of a combination of key contaminants, including Organic fuel cells may prove useful in many applications as acetic acid and methyl formate. an alternative to hydrogen fuel cells. In an organic fuel cell, an organic fuel Such as methanol is oxidized to carbon dioxide at BRIEF DESCRIPTION OF THE DRAWINGS an anode, while air or oxygen is simultaneously reduced to 45 water at a cathode. One advantage over hydrogen fuel cells is FIG. 1 is an exploded view of an exemplary embodiment that organic/air fuel cells can be operated with a liquid organic fuel cell; fuel. This diminishes or eliminates problems associated with FIG. 2 is a view of a portion of the fuel cell of FIG. 1; hydrogen gas handling and storage. Some organic fuel cells FIG. 3 is a view of a portion of the fuel cell of FIG. 1; require initial conversion of the organic fuel to hydrogen gas 50 FIG. 4 is a partial view of another exemplary embodiment by a reformer. These are referred to as indirect fuel cells. fuel cell; The presence of a reformer increases cell size, cost, com FIG. 5 plots the current density over time for an exemplary plexity and start up time. Other types of organic fuel cells, embodiment fuel and various commercial purified grade called direct fuel cells, avoid these disadvantages by directly samples: oxidizing the organic fuel without conversion to hydrogen 55 FIG. 6 plots the voltage over time for an exemplary gas. Until recently, methanol and other alcohols were the fuel embodiment fuel and a commercial purified grade sample: of choice in the development of direct fuel cells, and most and research focused on the use of these fuels. FIG. 7 plots the current density over time for an exemplary An advance in the art is presented in U.S. Patent Applica embodiment fuel and a commercial purified grade sample tion Publication No. 2003/0198852 (“the 852 publication”) 60 with varying levels of methanol added. and 2004/0115518 (“the 518 publication”). Embodiments described in these applications disclose formic acid fuel cells DETAILED DESCRIPTION OF THE PREFERRED with high power densities and current output.
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