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  Paramagnetic additive method of optimizing cell electrohydrodynamicsUSPTO Application #: 20060180471Title: Paramagnetic additive method of optimizing cell electrohydrodynamics Abstract: Magnetoelectrolysis cells known to operate successfully without utilizing a non-electrogenerated paramagnetic additive added to an aqueous electrolyte solution of such a cell may in some instances be further enhanced by utilizing such an additive. However, excessive amounts of additive are impracticable and formerly proposed transition metal salts used as paramagnetic additives were never demonstrated as effective except when used in large amounts. Now it is disclosed that small amounts of a salt of a paramagnetic lanthanide solve the problem, if methodically applied to enhancing the magnetoelectrolysis cell in accordance with the specified steps of the invention. (end of abstract) Agent: Robert Neville O'brien - Victoria, BC, CA Inventor: Robert Neville O'Brien USPTO Applicaton #: 20060180471 - Class: 205043000 (USPTO) Related Patent Categories: Electrolysis: Processes, Compositions Used Therein, And Methods Of Preparing The Compositions, Electrolytic Process Involving Actinide Series Elements Or Compound (at. No. 89+) (product, Process, Composition, And Method Of Preparing Composition) The Patent Description & Claims data below is from USPTO Patent Application 20060180471. Brief Patent Description - Full Patent Description - Patent Application Claims
BACKGROUND OF THE INVENTION [0001] 1. Technical Field [0002] This invention relates, in general, to utilizing selected chemical additives in fluid electrolyte solutions of electrochemical cells exemplified by types described hereinafter, for the purpose, primarily, though not necessarily exclusively, of initiating and/or increasing a measurable extent of beneficial fluid convection. [0003] More particularly, what is taught and claimed below as new is an improved method of utilizing non-electrogenerated paramagnetic species of inorganic solutes as solution-improving additives added to aqueous electrolyte solutions of electrochemical cells, preexistently designed to operate more effectively, than otherwise, when a suitably strong external magnetic field of permanent magnet or electromagnet origin projects within a volume containing an aqueous electrolyte solution between an anode and a cathode. [0004] Known from background art are several cells made to utilize magnetic phenomena, including both electrolysis cells supplied dc electricity to enact useful non-spontaneous chemical changes, and voltaic cells that produce dc electricity. Magnetically enhanced cells of all kinds are subjects of development in an area of electrochemistry which T. Z. Fahidy, at the University of Waterloo in Canada, suggested in "Magnetoelectrolysis", J. Appl. Electrochem., v13 (1983) 553, may be called "magnetoelectrolysis". The same label aptly identifies the technical field to which the present invention most closely pertains. [0005] 2. Background Art [0006] The fact that Dr. Fahidy's suggested label acquired in-use currency is shown by: "Applications of Magnetoelectrolysis"; Tacken, R. A. and Jansen, L. J. J.; J. Appl. Electrochem., v25 (1995) 1, in which recognition is present respecting innovative use of special laser interferometry set-ups, introduced at the University of Victoria in Canada by R. N. O'Brien (the present inventor) and colleagues, to obtain visualized evidence of convection adjacent-electrodes in small magnetoelectrolysis cells made into Fabry-Perot interferometers. [0007] Using the investigative tool of interferometry to examine one particular cell led to discovery in the O'Brien laboratory of an occurrence of convection where density layering would normally have made the electrolyte solution stagnant. The cell was configured with a cathode-over-anode (C/A) horizontal plane parallel electrodes orientation, with the direction of the imposed magnetic field parallel with the electrodes. No convective transport of species between the electrodes, to possibly supplement migration and diffusion, could be expected to result from magnetohydrodynamic (MHD) effects commonly explained by invoking the well-known "Lorentz force". A new postulate became needed, because clearly something differentiable from an MHD force was driving the unexpected convection in the C/A-configured CU/CUSO.sub.4/CU cell immersed in a 0.512 T magnetic field. Whatever the "something" force was, it did not occur for a similarly configured Zn/ZnSO.sub.4/Zn cell studied in similar magnetic field immersion. The new postulate invoked an internally generated gradient force involving inhomogeneity of volume magnetic susceptibility and a nonuniform induced magnetic field. The applicable underlying principle is that which states free-to-move paramagnetic substances tend to move into a region of higher magnetic field, whereas diamagnetic substances move away therefrom. [0008] The O'Brien laboratory's discovery and new postulate has become of such evident pertinence, in the background of the present invention, as to warrant incorporating the following publications by reference herewith: "Electrochemical hydrodynamics in magnetic fields with laser interferometry: Influence of paramagnetic ions ; O'Brien, R. N. and Santhanam, K. S. V.; J. Appl. Electrochem., v20 (1990) 427; and, "Magnetic field assisted convection in an electrolyte of nonuniform magnetic susceptibility"; O'Brien, R. N. and Santhanam, K. S. V.; J. Appl. Electrochem., v27 (1997) 573. These publications are of key relevance to delineating with permissible hindsight the below-claimed advance over instances of previous inventions for which, respectively, patent applications were filed within the time limits appropriate to the two articles' publication dates. The background art inventions are discussed further below. [0009] The postulate and explanation conveyed in the abovecited two key references gained currency, ie., recognition, in the art, as these articles ultimately became subjects of footnotes 25 and 26 in a more recent publication of others, namely: "Electrochemically Generated Magnetic Forces. Enhanced Transport of a Paramagnetic Redox Species in Large, Nonuniform Magnetic Fields"; Ragsdale, S. R.; Grant, K. M.; and White, H. S.; J. Am. Chem. Soc., v120 (1998) 13461. By 1998 these University of Utah chemists had advanced into an area of the art of magnetoelectrolysis perceived as existing but then not well understood, back in 1990 when Dr. O'Brien and Dr. Santhanam wrote: "There is a clearly demonstrated paramagnetic effect interacting in a way, as yet unknown in detail, with the magnetohydrodynamic effect". (From the Summary in "Electrochemical hydrodynamics . . . influence of paramagnetic ions".) [0010] Dr. White and Univ. of Utah colleagues published isolation of the paramagnetic effect. [0011] Drs. O'Brien and Santhanam, even as late as 1997, did not have a suitable investigatory tool to assure studying the paramagnetic effect in definite isolation from any possible intermingling of MHD effect, whereas Dr. White and Univ. of Utah colleagues lately found how to do it, with introduction of using modified NMR (nuclear magnetic resonance) tubes for experimental magnetoelectrolysis cells having electrolyte solutions containing highly concentrated organic species such as the nitrobenzene radical anion. A well polished platinum microdisk electrode was found ideal for studying how an inhomogeneous susceptibilities-related gradient force, "without interference from the masking effects of Fmhd", by itself "may result in a significant enhancement in electrochemical current." (Abovecited J. Am. Chem. Soc. article, Ragsdale et al., 1998) Older Magnetoelectrolysis Patents [0012] An early patent disclosing a purpose-built magnetic field enhanced cell, although without proposing a paramagnetic additive to optimize its electrolyte solution, is U.S. Pat. No. 1,658,872 issued to YEAGER (February, 1928) for a then unique "ELECTROLYTIC APPARATUS". The simpler-constructed of two versions devised for electrodeposition of a metal under the influence of a magnetic field was shown in a drawing figure, the significant righthand portion of which is reproduced herewith as "PRIOR ART" FIG. 2a. Including this figure materially assists understanding the present invention, and reviewing the YEAGER invention in detail further below helps equip interested artisans with enabling know-how for "retrofitting" the present invention to pre-existent apparatus. Such retrofits are here conceived as actions of skilled artisans applying the method of the present invention according to its best mode of use, and should prove helpful to delineate the advance made by this invention. [0013] Another leading example of a patented invention featuring magnetic field assisted stirring of an electrolyte solution, again without proposing a paramagnetic additive to increase stirring, is an "ELECTROLYTIC CELL COMPRISING MEANS FOR CREATING A MAGNETIC FIELD WITHIN THE CELL" for which U.S. Pat. No. 3,597,278 (August, 1971) issued to VON BRIMER. To enable retrofitting the present invention to the modified lead-acid battery of VON BRIMER, one of its figures of drawing is reproduced herewith as "PRIOR ART" FIG. 3a. [0014] Another cell designed for magnetic field enhancement was disclosed by KAWAKAMI ET AL in U.S. Pat. No. 5,728,182 issued March, 1998 for a "SECONDARY BATTERY AND METHOD FOR MANUFACTURING THE SAME." A figure illustrating a coin-shaped embodiment is reproduced herewith as "PRIOR ART" FIG. 4a, also useful for a "retrofit" of the present invention. Nearer Related Patents [0015] In part more closely related to the present invention than are the three abovecited patents, are three forming a group, the first of which issued September 1991 to O'BRIEN ET AL for a "SPACER FOR AN ELECTROCHEMICAL APPARATUS", U.S. Pat. No. 5,051,157. The 1990 published J. Appl. Electrochem. article partly entitled "influence of paramagnetic ions", cited above, was one of four "OTHER PUBLICATIONS" identified as relevant. Manganous and chromic ions were the only specifically named examples of "suitable" paramagnetic ions whose addition to electrolyte solutions was proposed "to further increase the stirring and to lower internal resistance (concentration polarization)", and it is no coincidence that these were the ions used in the O'Brien laboratory's interferometric investigations. [0016] The second nearer art patent in the group of three is U.S. Pat. No. 6,194,093 B1 issued February, 2001 to O'BRIEN for "MAGNETIZED CURRENT COLLECTORS COMBINED WITH MAGNETIC SHIELDING MEANS". This patent too incorporates the proposal that advantage can be gained by adding, to the peculiarly constructed various cells' electrolyte solutions, indifferent paramagnetic ions again exemplified by manganous and chromic ions. [0017] The third nearer art patent is U.S. Pat. No. 6,556,424 issued April, 2003 to O'BRIEN for a "SUPERCAPACITOR HAVING MAGNETIZED PARTS", wherein again appeared the proposal of an electrolyte solution changed by adding indifferent paramagnetic ions, eg., the manganous and chromic ones of the original influence of paramagnetic ions article by this time (2003) dating back thirteen years. [0018] From none of these three closely related patents, nor from them all cumulatively, did a presented reason emerge for specifically always naming manganous and chromic ions. An informed artisan could, however, from attending to "OTHER PUBLICATIONS" cited, find and read the only explicitly stated reason where it once was published, viz., in the 1990-dated "influence of paramagnetic ions" article. Out of a truly vast number of all potentially usable paramagnetic ions, the reason for selecting manganous and chromic ions was capability on their part to satisfy "thermodynamic considerations" related to those of the otherwise stagnant Zn/ZnSO.sub.4/Zn cell modified. See the criterion set forth at about the middle of the second column of text in the article's Introduction. [0019] In the O'BRIEN ET AL patent, first in the nearer art group of three, the prospect that additive paramagnetic ions may lose potency for the method via undesired coordination with certain ligands was left unconsidered. [0020] Moreover, although not a specifically claimed aspect of teachings, a teaching in the only paragraph teaching the paramagnetic additive method suggested to the artisans that even ions which are not indifferent", and even which may be included in "the deposition", may be used--qualifying this aspect of the teaching with the phrase: "as long as the deposition on an electrode does not cause detrimental effect, e.g. pressure discharge, loss of active material, etc." With candid permissible hindsight of an artisan today, reviewing that single paragraph of paramagnetic additive method teaching, particularly in view of its "etc.", more likely than not elicits an impression of an invitation to experiment, at indefinite length, to discover whatever the actual practicable scope encompassed by the method might be. [0021] The second and third already identified nearer art patents substantially re-instituted the aforesaid teaching from O'BRIEN ET AL, with the one exception of including a caution regarding possible "corrosive shuttle mechanisms". What was there intended to be conveyed concerns the fact that many ions are capable of changing in solution from one valency to another, if not by chemical reaction with other solute species, then possibly by being brought by diffusion or convection into contact with an oxidizing or reducing electrode. Such undesired electrodes-discharging "shuttles" or "redox couples" are described by H. Bode, page 321, Lead-Acid Batteries, Wiley-Interscience (1977). Electrolyte solution "impurities" named as likely to create the problem in a lead-acid battery include chromium, manganese, and chlorine. These, it happens, are constituents of the compounds which, for reason of "thermodynamics considerations", were selected to supply paramagnetic ions to add to the electrolyte solution of the Zn/ZnSO.sub.4/Zn cell featured in the background art's "influence of paramagnetic ions" reference--not very like the lead-acid cell which was one of three illustrated embodiments in U.S. Pat. No. 5,051,157. Continue reading... Full patent description for Paramagnetic additive method of optimizing cell electrohydrodynamics Brief Patent Description - Full Patent Description - Patent Application Claims Click on the above for other options relating to this Paramagnetic additive method of optimizing cell electrohydrodynamics patent application. ###  How KEYWORD MONITOR works... a FREE service from FreshPatents1. Sign up (takes 30 seconds). 2. Fill in the keywords to be monitored. 3. Each week you receive an email with patent applications related to your keywords. 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