Radioactive Artifacts: Historical Sources of Modern Radium Contamination☆☆☆

Journal of Medical Imaging and Radiation Sciences

Journal of Medical Imaging and Radiation Sciences 50 (2019) S3-S17

Journal de l’imagerie médicale et des sciences de la radiation

www.elsevier.com/locate/jmir

Historical Vistas

Radioactive Artifacts: Historical Sources of Modern Radium Contamination M. Donald Blaufox* From the Department of Nuclear Medicine, Montefiore Hospital and Medical Center, Albert Einstein College of Medicine, New York

Radium has been distributed in a wide variety of devices during the early part of this century. Antique objects containing significant amounts of radium turn up at flea markets, antique shows, and antique dealers, in a variety of locations. These objects include radium in devices which were used by legitimate medical practitioners for legitimate medical purposes such as therapy, as well as a wide variety of ‘‘quack cures.’’ These devices may contain anywhere from a few nanocuries to as much as several hundred microcuries of radium. In addition to medical sources, a large variety of scientific instruments utilize radium in luminous dials. These instruments include compasses, azimuth indicators, and virtually any object which might require some form of calibration. In addition, the consumer market utilized a large amount of radium in the production of wrist watches, pocket watches, and clocks with luminous dials. Some of these watches contained as much as 4.5 mCi of radium, and between 1913 and 1920 about 70 gm was produced for the manufacture of luminous compounds. In addition to the large amount of radium produced for scientific and consumer utilization, there were a number of materials produced which were claimed to contain radium but in fact did not, further adding to the confusion in this area. The wide availability of radium is a result of the public’s great fascination with radioactivity during the early part of this century and a belief in its curative properties. A number

This article was originally published in Seminars in Nuclear Medicine, Vol XVIII, No 1 (January), 1988: pp 46-64 RADIUM, which was used in a wide variety of objects during the early part of this century, is a source of radioactive environmental contamination which frequently is overlooked. Radium may be derived from a number of sources, not the least of which is material which was originally dedicated to * Corresponding author. M. Donald Blaufox, MD, PhD, Professor and Chairman, Department of Nuclear Medicine Albert Einstein College of Medicine, 1300 Morris Park Ave, Bronx, NY 10461. ** This article is a reprint of a previously published article. For citation purposes, please use the original publication details; Journal of Medical Imaging and Radiation Sciences, 18(1), pp. 46-64. ** DOI of original item: https://doi.org/10.1016/S0001-2998(88) 80019-9

of objects were produced in order to trap the emanations of radium in water for persons to drink in order to benefit from their healing effects. Since the late 20s and early 30s the public’s attitude towards radiation has shifted 180 and it is now considered an extremely dangerous and harmful material. However, even as late as the 1950s, there were still some items produced containing radioactivity which today would be unthinkable. The ‘‘Buck Rogers Mystery Ring’’ of the 1950s was activated with polonium. With the shift in public attitudes towards radioactivity, and increasing problems in disposal of radioactive materials, the disposal of radium presents a particularly perplexing problem. The radium which was produced in the early part of the century is still around in various forms and is extremely difficult to dispose of. All objects discovered claiming to contain radium should be taken seriously and should be properly surveyed. They then should either be stored in some area where the environment is protected from the radioactivity or if a very small amount of radium is present, they may be disposed of through one of several commercial sources. Any significant amount of radium is extraordinarily difficult and expensive to dispose of and there are only limited sites which will accept these materials. No clear cut, uniform mechanism for the handling of radioactive materials which turn up outside of the usual institutional sources, is currently in place.

a legitimate medical purpose. In a most entertaining volume published in 1937, Dr Robert B. Taft writes about ‘‘Radium Lost and Found.’’1 The introduction to this book describes the existence at that time of a group of people who were called ‘‘Radium Hounds’’ and who were charged with the responsibility of finding lost radium. This was particularly difficult in 1937 due to the lack of sophistication of equipment available to detect the radioactive sources During the early part of the century, the major reason for seeking lost radium was not necessarily the potential health hazard, but rather the intrinsic value of the material. A 100 mg specimen is characterized in Taft’s book as being the average amount of radium owned by a physician. This amount of radium has a mass about equal to a quarter inch of graphite from a lead pencil, and at one time cost as much as $12,000. The preparation of 100 mg of radium by

1939-8654/$ - see front matter Ó 2019 Published by Elsevier Inc. on behalf of Canadian Association of Medical Radiation Technologists. https://doi.org/10.1016/j.jmir.2019.11.004

an analytic chemist working with a physicist, took 1 month and required raw materials consisting of ten tons of ore, three tons of hydrochloric acid, five tons of carbonate of soda, one ton of sulphuric acid, and ten tons of coal. All of this was processed in an electric furnace. A particularly illuminating statement is made in the introduction to this volume, where Dr George Pfahler states ‘‘The loss of radium not only involves money, but, as indicated above it involves danger to the finder, for if he picks this up and holds it in his hand or puts it in his pocket, or leaves it about where a child could pick it up and swallow it, it may result in a serious damage or even death.’’ It is noteworthy that the health danger is mentioned in a context secondary to the monetary value of the material. Not only was there remarkably little concern of the danger of radium, but there was an almost religious belief in its curative properties. Dr Taft himself recalls in the preface that the stimulus for his book was produced by an event several years prior to its publication in which 75 mg of radium was lost from his office. The material was found the next day in the trash. He also writes about finding 25 mg serendipitously in a trash dump in North Carolina. As a result of these experiences, Dr Taft embarked on an effort to collate materials relating to radium loss and the results of his efforts are shown in Table I adapted from his volume,1 which cites the owner, city, amount, avenue of loss, whether or not the materials were found, and the instruments and searcher used. It is remarkable that as of 1937, a total of more than 1 gram of radium was completely lost and unaccounted for in this incomplete and casual survey. Where or when this missing radioactivity did or will turn up is anyone’s guess. Recently in New Jersey, a large amount of contaminated radioactive earth was discovered at homesites built on the grounds of what was thought to be an old watch factory. A satisfactory solution to the disposal of this material has only recently been found, after causing major environmental problems. Similarly, in recent years alerts have been put out for radioactive gold, which was waste material and had been utilized in the manufacture of rings. The ring story is a particularly alarming one. Spent radon seeds made of 24 K gold, which was contaminated with lead 210 and bismuth 210 (radon daughters), were used to make and repair jewelry as a cheap source of gold. According to the FDA drug bulletin2 as of January 1981, 12 cases of dermatitis and other problems had been reported in the state of New York. Forty-seven radioactive rings were located in New York and Pennsylvania, and at least two squamous cell carcinomas of the finger were reported. Thirty to 40-radon generators were in operation in the United States at one time and the problem may be widespread. Radiation dose rates from this jewelry ranged from 2 to 900 mR/hr, and problems may persist for 20 years or more after exposure. These large quantities of radioactive material left over from various manufacturing processes, were not even considered by Dr Taft I have recently encountered a most unusual descendent of medical radium, which was brought to my attention in 1983. Around that time, a New York antique dealer received a letter S4

from an individual in Massachusetts which stated the following: ‘‘I have an antique small metal box containing some radioactive radium and medical instruments used by a famous physician in Vienna around the turn of the century for treatment of cancers. The radium is supposed to have been refined by the Curie’s, kindly let me know if you are interested.’’ I followed up this offering by speaking to the person involved and asking him to send me some snapshots of the box. The materials included some paper, which contained a powder in a package of very friable paper about the size of a dollar bill, and what appeared to be molding wax for therapy with radium and a small metal container. The nature of the box and its contents were identified for me by an elderly radiotherapist. He remarked, "We used to store those under the hospital steps." The box and its contents were the property of a great uncle of the individual in Massachusetts, who was "a respected physician in Vienna around the turn of the century." Upon this individual’s death, the sister came into possession of materials and had learned that it apparently had been received directly from Madame Curie. Believing it to be quite valuable, because of its historic origin, she placed the packet which contained powered radium in a safe deposit box in a bank, where it remained for 20 or 30 years. Fortunately, the individual who came in possession of it after his mother died, had some familiarity with radioactivity and was able to store this at his place of work. He measured it with a survey meter and reported obtaining a reading of 3R per hour, with the B Shield opened, and. 1R per hour with it closed. These readings were at a distance of a couple of feet. I advised the person in question to contact the proper authorities in Massachusetts to arrange for disposal of the materials. He apparently was unable to obtain any help and, according to my last contact with him, was storing the materials at his place of work. I have tried to follow-up on this several times, but have been unable to obtain a reply. It appears that the safe deposit box was not surveyed for possible contamination. Other sources of "legitimate" radioactive materials which are to be found within the environment, are summarized nicely in the National Council on Radiation Protection and Measurements (NCRP) Report 56,3 "Radiation Exposure from Consumer Products and Miscellaneous Sources," published in August 1977. In that publication, it is stated that among the 45 million wrist watches sold in the United States between 1971 and 1972, nine million had luminous hands or dials. Until about 1963, radium-226 was used as the activating agent in most of the luminous watches sold in this country. At that time, they estimated that as many as ten million watches containing radium were still in use in the United States and that clocks containing radium were still being distributed. Estimates for radiation dose equivalent rates range from .5 to 3.3 millirem (mrem) per year per device and individual dose equivalent rates as high as 310 mrem per year were given for a wearer of a wrist watch containing 4.5 mCi of radium. Pocket watches provided an even higher radiation dose equivalent rate of about 60 mrem per year per mCi of radium. The annual absorbed dose of the skin direcly under the face of a pocket watch could be as high as 165 rad and it

M.D. Blaufox/Journal of Medical Imaging and Radiation Sciences 50 (2019) S3-S17

Table 1 A Listing of Lost Radium Owner

City

Mg

Avenue of Loss

Found

Instruments

Searcher

– – – – Dr J.T. Murphy Dr J.T. Murphy University of Michigan University of Michigan University of Michigan University of Iowa University of Iowa University of Iowa Dr L.J. Menville Dr L.J. Menville Dr L.J. Menville Dr W.H. Van Allen Dr W.H. Van Allen Baker Sanatorium Drs Martin & Martin Drs Martin & Martin – – – Dr F.A. Coughlin Morrisania Hospital Kings County Hospital Dr W.W. Watkins – Moe Hospital Sheboygan Clinic Radium & X-Ray Institute Huron Road Hospital Keith & Keith Keith & Keith Keith & Keith Keith & Keith Local Infirmary Dr Wright Clarkson Dr Lomax Gwathmey Dr H.W. Grimm Dr C.C. Phillips Dr F.P. Boswell Dr Norman Titus – – Dr Harold Swanberg – Norton Infirmary Dr W.G. Herrman Dr Albert Cole Dr Dewell Gann, Jr – – – Dr C.D. Cleghorn Dr C.D. Cleghorn – – – – –

MO Kansas City, KN Pittsburg, KN Pittsburg or Windfield Toledo Toledo Ann Arbor, Ml Ann Arbor, Ml Ann Arbor, Ml Iowa City Iowa City Iowa City New Orleans New Orleans New Orleans Springfield, MA Springfield, MA Lumberton, NC Dallas, TX Dallas, TX – – – Providence, RI New York New York Phoenix Scranton, PA Sioux Falls, SD Sheboygan, Wl Calgary, Alberta Cleveland Louisville Louisville Louisville Louisville Louisville Petersburg, VA Norfolk, VA Pittsburg Charlotte, NC Montgomery, AL – Detroit Detroit Quincy, IL – Louisville Asbury Park, N J Indianapolis Little Rock, AR MO MO MO Macon, GA Miami, FL Rochester, NY Philadelphia Oklahoma City Richmond, VA –

– 6 3 5 30 – – – 10 – – – 50 15 20 – – – .6 6.4 50 20 50 50 – 30 5 50 25 50 50 10 10 50 50 10 50 50 10 5 – 50 – 10 – .66 100 50 50 100 – 50 25 5 50 50 50 25 50 – 50

Sewer – Sewer – Sewer Stolen (?) Floor Broken needle – Dump Trash basket Trash container – – – Patient Floor Wax Mould Thrown away – Garbage Garbage Sewer Incinerator Incinerator Drain pipe Floor Hospital Pig Laundry Sewer Rubbish Drain Sewer Sewer Floor Furnace Stove Office Office Office Stolen Closet Mirror Frame Trash barrel Ashes Stolen (?) Furnace Theft (?) Ashes Sewer Sewer Sewer Exploded Sewer Furnace Furnace Dressing Garbage Furnace Sewer

Yes No No No No No Yes Part No Yes Yes Yes Yes No No Yes Yes Yes No No 75% Yes No Yes Yes Yes No Yes Yes Yes Yes Yes Yes No No Yes 35 mg Yes Yes No No Part Yes Yes Yes Yes No Yes No No No No No Part No No Yes Yes Yes 70% No

– – Electroscope – – – Electroscope – – Electroscope Electroscope – – – – Electroscope Electroscope – – Electroscope Electroscope Electroscope – Spinthariscope Electrometer Counter – Electroscope Electroscope Counter Counter Counter Taft Counter – – – – Taft Counter Counter Counter Counter – Willemite Victoreen Victoreen Counter Counter – Electroscope Electroscope – – – – Electroscope – Electroscope Electroscope Electroscope Electroscope Electroscope

Owner Owner Owner Owner Owner – – – – Lapp Lapp – Elliott – – Van Allen Van Allen Murphy – Owner Knowlton Knowlton – – Braestrup Braestrup – Weatherwax Buchta Rovner McGuffin Beasley Owner – – Owner – Owner Taft Taft Taft – Owner Corrigan Corrigan Owner Swanberg Keith – – – Owner Owner Owner – – Miller Miller Miller Miller Miller (continued)

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Table 1 (continued ) Owner

City

Mg

Avenue of Loss

Found

Instruments

Searcher

– – – Roper Hospital University of Pennsylvania Dr Sanford Withers Dr Sanford Withers Dr Sanford Withers Dr Sanford Withers University of Pennsylvania University of Pennsylvania University of Pennsylvania University of Pennsylvania The Clinic University of Iowa Harper Hospital Municipal – Dr R.B. Taft Dr Robert Drane Dr Robert Drane Dr Curtis Burnam Dr Albert Soiland Dr Albert Soiland Howard Kelly Hospital Cleveland Clinic Cleveland Clinic People-s Hospital Drs Hill & Thomas – Gallinger Hospital Dr G.E. Pfahler Vanderbilt Uni. Hospital Dr S.S. Marchbanks Dr S.S. Marchbanks Drs Newell & Newell Drs Newell & Newell Newell Sanatorium Newell Sanatorium –

– – – Charleston, SC Philadelphia Denver Denver Denver Denver Philadelphia Philadelphia Philadelphia Philadelphia Lewis ton. ID Iowa City Detroit Monroe. NC – Charleston. SC Savannah, GA Savannah, GA Baltimore Los Angeles Los Angeles Baltimore Cleveland Cleveland Akron, OH Cleveland – Washington, DC Philadelphia Nashville, TN Chattanooga, TN Chattanooga, TN Chattanooga. TN Chattanooga, TN Chattanooga. TN Chattanooga, TN Philadelphia Philadelphia Philadelphia Philadelphia Philadelphia Philadelphia Nanicoke, PA

25 25 – 10 1 – – 200 – 50 25 10 – 25 10 5 25 20? 75 50 – 50 75 3 600MC – – 5 – 50 25 100 50 50 35 35 5 45 5 50 50 200 10 10 10 40

Toilet Furnace Wash tub Hospital Rubbish Cuff Trousers Roof Sewer Exploded Street Floor Trash Bed Floor Exploded Floor Dump Dump (?l Trash Sewer Dental mould Dump Toilet Waste basket Furnace Furnace Floor – Furnace Incinerator Trash Dump Trash barrel Sewer Sewer Dump Dump Furnace – Ashpile Ashpile Dump Floor Floor – Drain

No 80% No Yes Yes Yes Yes Yes Part Yes Part yes Part Yes Part No Yes No Yes No Yes Yes Yes Yes Yes Yes Yes Yes Yes Yes Yes Yes Yes No No No No Yes – Yes Yes Yes Yes No No Yes

Electroscope Electroscope Electroscope None Counter Electroscope – Electroscope – – Fluor scope Electroscope – Electroscope Counter – Electroscope Electroscope Electroscope – None Electroscope Electroscope None Electroscope Electroscope Electroscope Victoreen Electroscope Counter Curtıas Det. Electroscope Victoreen Electroscope Electroscope Electroscope Electroscope – – Electroscope Electroscope Electroscope Counter Electroscope Electroscope Counter

Miller Miller Miller Rudisill Locher – – – – Pancoast Pancoast Pendergrass – Johnson Kerr Witwer Taft Taft Owner Owner Owner Owner Owner Owner Glasser Glasser Glasser Classer Glasser Glasser – Weatherwax Omberg – Insurance company Insurance company Insurance company Allen – Weatherwax Weatherwax Weatherwax Weatherwax Weatherwax Weatherwax Weatherwax

– – – – – Data from Taft.1

was estimated that 20,000 people in the United States carried these watches, each of which contains approximately .1 mCi of radium. Antique pocket watches and clocks, as well as wrist watches, have become major collectables and are being auctioned and sold at antique markets continually. Another source of potential radiation exposure is luminous clock faces. Radium also was commonly used for instrument panel illumination in airplanes, as check sources in survey meters, and more recently in smoke detectors in homes. Another source of information about these sources of contamination is in the publication "Radioactivity in Consumer Products. ’’4 Dr Holm (p 118) points out in this report that radioluminosity was the most important phenomenon associated S6

with consumer products and radium. Alpha particles were counted using zinc sulphide screens which were incorporated into spinthariscopes, which are discussed later. Between 1913 and 1920 about 70 g of radium were produced by refineries in Pittsburgh and a considerable amount of this was used to make luminous compounds. Luminous dials were vital to early aviation when electrical systems were not present on aircraft. Even in the 1920s many homes lacked electricity and luminous dials were essential. Early luminous dials contained as much as 100 mg of radium per gram of phosphor. Luminous chains for switches, luminous rings to attach to chamber pots, and luminous paints were commonplace. California orange fiesta dinnerware (1920 to 1930) used uranium

M.D. Blaufox/Journal of Medical Imaging and Radiation Sciences 50 (2019) S3-S17

Table 2 Survey of Packing Material Wrist Compasses Containing Radium Location

Measurement

Surface of wooden crate Surface of "tar paper" sealed package Interior surfaces of sealed wrapper Outer surfaces of waxed waterproof wrapper Outer surface inner carton Inside surface of carton Surface of individual compass boxes Wrapping of individual compass

5 mr/h–beta-gamma 8 mr/h–beta-gamma 4.5 nCi 2.2 nCi 4.5 nCi 13.5 nCi 4 nCi 4.5 nCi

Wipe Tests of Wrist Compasses Containing Radium Dry Wipes

Wet Wipes

Compass No.

Beta (pCi)

Alpha (pCi)

Beta (pCi)

Alpha (pCi)

1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 Average:

25 35 45 36 27 60 46 27 46 52 36 45 72 51 46 46 47 64 43 51 25 45 34 33 43  12

17 25 23 28 14 35 25 19 27 28 18 28 57 29 35 25 26 43 26 35 21 32 25 10 28  9

150 128 89 119 102 154 150 99 107 113 128 132 156 163 93 119 172 95 133 134 143 269 63 149 132  40

48 26 37 30 26 34 40 24 24 24 33 37 49 47 21 25 68 18 39 34 36 136 20 90 40  26

Data from Moghissi et al (p 298).4

oxide to achieve its color (20,000 dpm of alpha activity per set). The Buck Rogers Mystery Ring of the 1950s contained polonium. Lightening rods containing radium were manufactured in quantity. Military uses of radium were as widespread as were the commercial products for the luminescent light sources. Herman4 (p 294) reports on two objects tested in the 1960s. An azimuth indicator scale which was used in the turret of an armored vehicle was examined by a variety of techniques. The beta-gamma dose rate at one foot from the center of the scale was calculated to be 6 mrem/h. The dose rate on contact with the scale was estimated to be 100 mrem/h. After one week 13.6 nCi of radon were leaked from the scale (see the articles by Hendee and Doege). Herman also describes the storage of 38,000 wrist compasses with luminous dials purchased by the military in 1953. One of the cartons containing 100 compasses contained 267 nCi of radon gas (see Table 2) when tested.

Radioactivity in commercial scientific instruments and particularly in old scientific instruments, provides another interesting and often unsuspected source of radioactivity. Antique scientific instruments with luminous dials are of particular concern because they are frequently polished down with buffing wheels to expose the brass surface which is attractive and saleable. In this process, the paint on the instrument is removed, exposing the buffer to inhalation or ingestion of the associated radium-226. This particular threat was recently reviewed in an article by Anthony R. Constable.5 w In his review, he points out that if all the radium in one single World War II Army compass were ingested by a single person (unlikely though it may be), it could exceed the maximum permissable body burden by 50 times. Among the more common scientific instruments, the Crook’s spinthari scope contains a small amount of radium, probably in harmless amounts, and is a most interesting device.6 I will return to this later. The entire area of scientific instruments encompasses within it a smaller and fascinating source of radioactive materials which are likely to be encountered in the environment, namely, radioactive materials which were sold to be used as medical cures. A large number of radioactive sources are available in the form of devices which were thought to be curative in their properties because of radioactivity they contain. I have encountered a large number of these items in my medical antique collecting which deserve some mention and which represent varying degrees of hazard. In 1983, a person who fortunately was associated with a Radiology Department and was clearly aware of what he had, offered me (and I subsequently purchased it) an early American stoneware jug which had the label on it "Revigator Radium Ore, Patented 7/16/12, Trademark The Radium Ore Revigator Company, 260 California Street, San Francisco, California. ’’7 The instructions on the jar were "fill jar every night, use hydrant or any good water, drink freely when thirsty upon arising, and retiring, average 6 or more glasses daily, scrub with stiff brush and scald monthly." The radiation reading inside of this stoneware jug was 5.2 mR per hour and outside the reading was about 1 to 2 mR per hour. The Revigator originally contained a cone of radioactive ore which was placed in the crock. The water then would sit with it, presumably absorb the emitted radon, and was to be drunk on a regular basis (Fig 1). In 1984, I came across a much more dangerous example of a device with the same basic purpose. An antique dealer located in a busy area of New York City, offered me an instrument which was labeled "Radiumator, the standard radium emanator, guaranteed to contain real radium," manufactured by the North American Radium Company. This device 7 was examined by me with Drs L. Rao Chervu and Paul Goodwin, and was estimated to contain somewhere between 100 to 300 mCi of radium. It originally functioned as a source through which air was pumped in order to absorb the radon emanating from the radium and force it into a glass of water. The radioactive water was to be drunk. To the best of my

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Fig 1. (A and B) The revigator, patented July 16, 1912, is shown above. The device is a large pottery crock about 12" high and 10" in diameter at the base. The instructions are written on the side and water is introduced through the top, which has a removable cap. The glass is filled with the simple faucet on the jug. Originally a small cone of radioactive material was contained in the crock. An open gas flow counter yielded 4,400 cpm at the top and 10,000 cpm at the side of the vessel. Inside the counts reached 175,000 cpm. The ionization rates were 5.2 mR/hr inside and 1 mR/hr at the surface. A custom-made acrylic case houses the entire crock for display and safe viewing in the nuclear medicine conference room (no detectable radioactivity at the surface of the case).

Fig 2. (A and B) These are two views of the radiumator. A second, curved metal tube similar to the one shown at top, has been lost. The device is considerably more complex than the revigator and contains a great deal more radium. The tube below the glass housing was probably used to discharge gas into a glass of water. The gas was pumped out using the tubes on top. The radium is contained in a small vessel within the glass cylinder which makes up the instrument. This was examined away from the laboratory so the amounts of radium thought to be contained in it are crude estimates.

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M.D. Blaufox/Journal of Medical Imaging and Radiation Sciences 50 (2019) S3-S17

Fig 3. (A and B) This is the Radiorem. Note the directions in the lid of the simple wooden box. It is interesting that the device was distributed by Schieffiin and Co in New York, a legitimate pharmaceutical company founded in 1881. The brown material at the bottom of the embossed jar probably contains radium. The fluid in the jars appears to be tap water. The count rate at the bottom of the bottle is 43,000 cpm with the gas flow counter and at the surface of the box it is 7,000 cpm. The exposed bottle gives a reading of about 0.1 mR/hr at the surface.

knowledge, this relatively large amount of radium currently is still residing in the shop of the antique dealer with whom I consulted (Fig. 2). It is particularly disturbing to note that in seeking out the proper agency responsible for supervising the disposal of this material, there was no clearcut line of responsibility and, in fact, the dealer, since he was not licensed, was not under the jurisdiction of the Office of Radiation Control. The latest source, to which I believe the problem had been referred, was the Occupational Safety and Health Unit of the Department of Labor of New York State. Letters from me to that office have remained unanswered. Another potentially large source of radioactivity was brought to my attention in the form of a device in the possession of another antique dealer in Westchester County in New York. That source was shown to me last summer and I

promised to return sometime during the year to survey it. About April I received a hysterical phone call from the owner telling me that a friend had brought over a makeshift radiation detector and that he had measured a dose rate of "100 rad per hour," a couple of feet from the source. I assured the owner that this could not be a correct reading and that the units were not even correct but that I would come up and check it out. The device is called a "Radiorem Outfit" and originally consisted of eight bottles in a simple box, of which five are still present. The bottles contain a brown solid material in the bottom, which is radioactive, and they are filled with water. The stoppers are frozen and we have been unable to check the contents directly without danger of breaking the bottles. The directions read "Stand the 8 bottles in a row, with the ring marker on the first one. Put one rod in

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Fig 4. The top of a radium salve pot is shown. The lid and jar contain no radioactivity, but there is no trace of the original contents left. This is most interesting for the claims made by its manufacturer. It is not certain whether this ever contained any significant amount of radioactivity.

each bottle. Fill them all to the brim with water and press in the stoppers so that air is excluded. Drink 2 bottles every day, one during or after each morning and evening meal, drink slowly from the bottle to avoid shaking. Refill and replace it in line and put the ring on the next bottle each time. After four days the eighth bottle will be reached and thereafter each one in turn will contain a charge of radium emanation equal to that of the stronger natural radioactive springs. Made by the Radium Therapy Corporation." The radiation from the box and its contents (Fig 3) was almost immeasurable at a few inches. The outfit was marketed by Schiefflin and Company, New York. This legitimate pharmaceutical firm was founded about 1880. A number of other less potent but definitely radiumcontaining "cure" devices have either been acquired by me or brought to my attention during the past several years. Dr Ronald Berger from Baltimore, sent me a photocopy of the directions for "Use of Radium Stone." They read that you should "place the radium stone in a 3 gallon water receptacle, preferably an earthen jar and fill with any water. Allow it to stand 12 hours before using and then fill water container every night. This insures a supply for the next day. Drink at least one or two glasses before breakfast and drink freely during the day, never drink less than 12-15 glasses a day." The brochure goes on to say how radioactivity is good for your health and will cause the following, all of which are signs of its curative operations: "One, noticeable increase in the amount of urine, and the frequency of urination; Two, temporary disturbance of the bowel action inclining towards looseness in some cases, and toward temporary constipation in others, depending upon the systematic condition of the individual; Three, discoloration of the tongue caused by excess elimination of poisons from the liver, also manifested by discoloration of the stool; Four, temporary nausea and temporary sick headache and gas S10

pains in the stomach caused by excess elimination of poisons from the mucous covering of the stomach and intestines; Five, temporary itching of the skin, sometimes slight eruptions of rash caused by excess elimination of poisons from the blood stream and excess metabolic action from the skin; Six, aching joints, due to increased elimination activity of toxic poisons (this is especially noticeable at the beginning in rheumatism, arthritis and gout); Seven, temporary depressed feeling of increased nervousness caused by reactions of regulation of metabolism in the entire body economy." It was manufacured by the Hogan Radium Water Company. Another device with curative powers which may have contained radium was Dr Showers’ radium salve (Fig 4), made by the Cardinal Manufacturing Company. This salve was recommended for lupus, scrofular, and cancerous growths, and for all kinds of ulceration and diseases of the skin. Since all of the containers which 1 have are empty, it is impossible to estimate how much radium they contained. Another interesting item is ‘‘Spa-radium’’ or radium sparklets. This emanator was made available in 1912 by the Sparklets Company (Fig 5). They state ‘‘A Spa-radium is a sparklet containing a quill impregnated with a measured quantity of an active radium salt. This salt is continually giving off countless minute electrical discharges producing emanations which, when dissolved in water by means of the well known Sparklet apparatus, produce a palatable radioactive drinking water of a curative strength far exceeding that obtainable at any Continental or British spa. (Many of the spas of Europe and the United States advertised their waters as being naturally radioactive, which was thought to enhance their curative properties.) This radioactive water expels poisonous elements from and adds a new wealth of energy to the system, enabling anyone who drinks it to battle against disease. To quote the words of Dr Howard Kelly, the celebrated American radiologist, it is ‘‘a gift of God, curing practically all nervous orders." Benefits claimed for the use of spa radium sparklets include: "It relieves the pain of gout, it eliminates uric acid from the system thus preventing its deposit in the joints, lowers the blood pressure, is a general all-around stimulant and increases the appetite, it will often cure obstinate neuralgia, its use is not comparable with that of a drug as it does not in any way interfere either with the diet or daily routine. It increases the red count and stimulates phagocytic action of the leukocytes. It is a tonic to a system lowered by anxiety or illness. Hay fever, catarrah in the head and colds have been allayed in many cases by the use of radioactive water as a nasal douche. No harmful effects have ever been known to be produced by the use of radioactive water." The brochure goes on to indicate "during an influenza epidemic, the miners at the radium ore mines at Colorado were found to be immune from this disease. After research, the conclusion arrived at was that their immunity was due to the fact they were drinking water charged with radium emanations from the mine. The amount of radium contained in these sparklets was described as an amount capable of discharging one electrostatic unit.

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Another remarkable facet of the story of radium is that there were a large number of ‘‘radium cures" which were distributed in the 1920s and 1930s which, in fact, had no radium at all. These artifacts when encountered appear to pose the potential threat of containing radioactivity but in reality they were hoaxes perpertrated on an unsuspecting public. Since it is impossible to differentiate between the numerous "cures" which did or did not contain radium, they all must be treated with respect and surveyed. The ironic thing about many of these particular items is that judgments were handed down by the court against the various promulgators of the "cures" on the basis of the fact that they did not contain radium. The quack doctors were not prosecuted for exposing the public to a dangerous substance, but rather for advertising fraudulent contents. James M. Harris from Tulsa, OK, marketed a cancer cure called "Radium Oil. ’’8 A $10,000 award was judged against him in 1927 because he treated a woman with a probably operable case of cancer of the breast and allowed the matter to progress until it became inoperable. The woman received $7,500 in actual damages, and $2,500 in exemplary damages although she had died of cancer in 1925.

Another company produced a metal device with a straight cylinder which fit into the ear canal and a curved portion of the outer ear.8 Its chief attraction was a claim that it was radioactive. It was said to be charged with "Hearium," an alleged radioactive substance with curative powers. It was produced by an individual who made his living dealing in fake radium. Ultimately the "Hearium" ingredient was abandoned and a very small amount of real radium was substituted. The radium was provided by an advertising quack from the Pacific Coast. J. Bernard King sold earth as a cure for illness under the claim that it was a radium salt.8 In 1918 "Dr" King sent a full size sample of his tuberculosis cure to a representative from the American Medical Association (AMA). The material consisted of soil in a quilted pad. King declared that it was new radium and reported that, although it was quite radioactive, it was harmless. He charged $50 for these pads but offered the AMA investigator a free one in exchange for a testimonial. King ultimately was prosecuted in Cincinnati for the illegal practice of medicine, fined $100 and sent to jail for 30 days. He used trade names such as International Radium Company and Radium Products Company. The

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Fig 5. (A, B, C, and D) A photo of the advertising brochure for "SPA-Radium" radium sparklets is shown. Figures A and B show the apparatus and (continued on page 57).

material in one form of his pads cost King 5 1/3¢ for a pad and he sold it for $15. Other materials were "sold under money back guarantee for $2.50 (half price) to prove the power of radium as a cure for all diseases’’. In 1915, an individual named White, who espoused a wide variety of quack cures, provided a testimonial for the Radiumacti Company of California, that put out a line of fake radioactive preparations.8 Medical advisers recommend their patients to visit a Continental Spa suth as Baden Baden, Franzensbad, Marienbad, Rastenberg or Wiesbaden, where many sufferers go yearly for treatment by, the waters, and where many cures have been effected, and to-day it is not questioned that these cures are due to tile emanations of radium derived from the radioactive properties of the waters. From their source these waters traverse rocks, and absorb emanations of radiam from radioactive matter deep down in the centre of the earth, and these emanations, when absorbed in tile system, produce remarkable curative results. Yet another material was radium healing balm, shipped by J.H. Frank Smokey, who traded as the Uranium Mining S12

Company of Denver.9 Colorado was an important early source of radium. This material was a soap with the odor of sassafrass containing 9.3% washing soda, 4.6% baking soda, 1.1% sand, and 56.4% water. He was convicted of fraudulent advertising and fined $10 and costs in 1918. The Radio-Sulpho Company was incorporated in Denver for one million dollars, with E.H. Griffith, MD, as its consulting physician and Philip Schuch, Jr, as the President.10 These individuals claimed that the vaccine used in vaccination was the cause of cancer and that cancer germs could be cultured directly from the vaccine. The cures they recommended included Radio-Sulpho, Radio-Sulpho Brew, and Limburger cheese (Yes, Limburger cheese). The method of application was to wash the cancer with radio-sulpho solution and then apply a cheese poultice. The radio-sulpho itself consisted of a strongly alkaline solution of sodium sulphide with a little sodium carbonate and the distinct odor of hydrogen sulphide. Beside all the other unpleasant aspects of this particular quack cure, the statement is made in their advertising booklet "I treat personally the white race only." Radio Sulpho Brew was found to be nothing more than a solution of epsom salts.

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Fig 6. The advertising card for radium described in the text is shown. Thousands of these must have been circulated. The card, which is a modification of the concept of the spinthariscope, yielded 2,300 cpm within the circled area which was claimed to contain radium.

Both the Radio-Sulpho Brew and Radio-Sulpho were declared misbranded by the American courts on the grounds that they did not possess the therapeutic virtues claimed for them, neither did they possess radium or radioactive properties, as their name would indicate. BENEFITS CLAIMED FOR THE USE OF "SPA-RADIUM" (RADIUM SPARKLETS). It relieves the pain of gout. It eliminates uric acid from the system, thus preventing its deposit in the joints. Lowers the blood pressure. Is a general all-round stimulant and increases the appetite. It will often cure obstinate neuralgia. Its use is not comparable with that of a drug, as it does not in any way interfere either with the diet or daily routine. It increases the red count and stimulates the phagocytic action of the leucocytes. It is a tonic to a system lowered by anxiety or illness. Hay fever, catarrh in the head and colds have been allayed in many cases by the use of radioactive water as a nasal douche. No harmful effects have ever been known to be produced by the use of radioactive water. During an influenza epidemic the miners at the radium ore mines of Colorado were found to be immune from this disease. After research the conclusion arrived at was that their immunity was due to the fact that they were drinking water charged with radium emanations from the mines.

Fig 5. (Cont’d.) C and D provide some insight into the manufacturers claims. This is a British device and it is patented. I have not encountered an example. Yet another substance was called Radol, marketed with the claim "I can cure cancer." This company was ultimately put out of business by issuance of a post office fraud order.10 Radol was claimed to be a "radioactive and radium impregnated fluid which was sold for the cure of cancer." Analysis showed that Radol was, in fact, a weakly acid watery solution of quinine sulphate with about 7% alcohol. It was neither radioactive nor did it contain radium, and the label failed to state the presence of alcohol; all these misrepresentations lead to the prosecution of the nostrum in the US courts under the Food and Drug Act for misbranding. A plea of guilty to indictment was entered and fines of $100 and $50 were assessed for the issues of misbranding and alcohol content, respectively. Returning to truly radioactive materials, it is interesting to review a variant of the spinthariscope which was mentioned earlier and is available in several forms, all of which contain some radium incorporated into a small advertising brochure. One trade card which I have recently acquired through Dr Jim Conway, has radium in a photoluminescent material deposited on it, and has the following caption. "Observe the radium on this card only in total darkness of night and remain in darkness until eyes are accustomed. Use a magnifying glass. If not previously exposed to any light, thousands of alpha rays may be seen like vivid sparks." And then on the back of the card is a story about the wonders of radium, recommending that you send for the story of a quarter

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Fig 7. The Radiothor brochure is shown closed (A) and with the cover opened (B). The cover effectively screens the radioactive source and acts as a lens for the spintbariscope. With the cover open, the luminous spot has a count rate of 15,000 cpm. A few other pages are shown for interest (C, D, and E). Publisher’s note: Figure & B and C were missing from the original article

century of radium research, written up in "The Sleeping Servant," the story of radium and cosmic rays, by Luther H. Gable (Fig 6). Another advertising booklet is "Radiothor Perpetual Sunshine." This also operates like a spinthariscope and has a spot on the first page which contains radium (Fig 7). Under the spot is printed: "Millions of radium rays arise from this little spot constantly. You can actually see the rays S14

on the cover." This, too, is to be seen in the darkness and claims to treat a huge number of conditions with the material advertised by the booklet. During a recent trip to England, I encountered a spinthariscope, which consisted of an individual eye piece and polonium screen, which was being shown as a Victorian device (Fig 8). It obviously was not Victorian and it probably

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Fig 8. (A and B) A spinthariscope from England with an eyepiece and separate polonium screen is shown (A). There is a slot in the box for a second screen. An American spinthariscope used as a teaching device from the Radium Chemical Company which is still in existence, is also shown (B).

Fig 9. The figure for a department of transportation specification 2R containment vessel is shown. A type A package is simply a containment vessel such as the routinely encountered steel drum. The 2R vessel is a much more sophisticated container which is intended to prevent any possible contamination with radioactive material, but not necessarily to shield from radioactivity. (Modified from ref.11) M.D. Blaufox/Journal of Medical Imaging and Radiation Sciences 50 (2019) S3-S17

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Table 3 An Example of the Radium Packaging Instructions Followed by the Albert Einstein College of Medicine Procedure for Packaging Radium Sources

1. 2. 3. 4. 5. 6. 7. 8.

9. 10. 11. 12.

13.

14. 15. 16. 17. 18. 19.

It is important that you read and understand the entire procedure before attempting to package actual radium sources. For assistance with specific questions contact: Bill Dornsife Pa. Bureau of Radiation Protection 717-787-2163 Estimate the number of sources, based on physical size and activity that will fit into the disposal capsule and shielded overpack. (Use attachment A as a guide.) Write a letter to the Nevada Department of Human Resources, Radiological Health Section, describing in detail what is desired to be disposed of. Include as a minimum: description of the sources, proposed packaging, quality control (who will witness packaging) and expected date of arrival. Contact U.S. Ecology (702-553-2203) to obtain appropriate shipping papers and site license conditions. The site should be contacted again prior to shipping to insure compliance with all license conditions. Request disposal capsules and transportation overpacks from the Conference as appropriate. Obtain CERROBEND* or equivalent alloy and epoxy sealant. Arrange for State Inspector to witness packaging of the source(s). Leak test source(s) (Hale method is preferred) within one week prior to packaging. If source is leaking, all packaging steps should be performed in a controlled environment, such as a glove box or hot cell. As an alternative, if the current source container is deemed adequate, it could be sealed in the disposal capsule without removing the leaking source. If the source is not leaking, all packaging steps should be performed in a filtered vent hood. Note: Steps 9, 10, 11, 12, and 13 should be performed several times with a simulated source or until it can be assured that personnel are familiar with the procedure. Place disposal capsule and source container in the controlled enclosure. Melt sufficient low melting point alloy (CERROBEND* or equivalent lead-bismuth alloy) to fill disposal capsule. Fill disposal capsule about half full of melted alloy. When a thin crust forms on the surface of the alloy, using appropriate tools, place source(s) in the alloy such that they can subsequently be completely covered by additional alloy. (Sources should be free standing in the alloy at this point and not in direct contact with the capsule inner surface.) Allow the container to cool for several minutes in air. Note: At this point corrective action can be taken if the sources have been misplaced. The alloy can be remelted by placing the entire capsule in a shallow pool of boiling water. This should be done only if using simulated sources for training or if the sources are not in the proper position after the alloy cools. The source(s) or simulated source(s) can then be removed and steps 9 through 13 repeated. Fill the remainder of the capsule with liquid alloy to completely cover source(s). Take care not to overfill capsule so as to prevent the complete insertion of the screw cap. After the alloy has cooled, insert the screw cap with the copper 0-ring and tighten securely. Use the slot at the bottom of the disposal capsule to hold the capsule steady while torquing. Seal the cap with an epoxy substance. Perform a leak test on the disposal capsule. Place the disposal capsule in the shielded cavity of the shipping container and insert the shielded plug. Hand tighten the screw cover of the inner 2R container. Place cover on the outer container and properly seal the container. Conduct appropriate radiation surveys and complete shipping papers and manifest. Lable the container as appropriate. *Trademark for bismuth/lead alloy that melts at 158 F. Manufactured by: CERROMETAL Products Box 388 Bellefonte, PA 16823

was a variant of the parlor variety device or perhaps a teaching aid. There undoubtedly are numerous other sources of radium that were used in legitimate medical endeavors which have been misplaced during their use, or used as quack cures and survive to this day in some form. It is important to keep in mind that most of these devices may contain a certain amount of radium. This ranges from an exceedingly small amount, to the very large amounts noted in the Radiumator and the left over radium therapy device which was stored in a bank for several decades. All of these artifacts should be treated with caution and with respect for their potential danger. The amount of radiation should be assayed in order to define proper handling procedures and storage. Although it is S16

unlikely that any individual would ingest all of the radium in any one of these examples, they remain a potential hazard. For instance, the radium bottles were stored next to the work bench of the owner and had been there for 20 some odd years. Had this contained a significant amount of radiation, some significant and highly undesirable exposure might have resulted; even worse is the possibility of the materials being in an area where they can be reached by children and possibly ingested. The biggest problem which one encounters when discovering materials such as these in the environment is their proper disposal. The obvious necessity to remove them to the safety of a laboratory which is capable of dealing with radioactivity, is the easiest part of their care. It appears that

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there is not a clear or logical line of responsibility for their disposal by governmental agencies. Regular licensing agencies generally are concerned with professional or business categories of use and are responsible only for supervision of licenses. Therefore, the ironic situation arises that the layman, having acquired a measurable source of radioactivity and not having a license, is technically in violation of some law but at the same time is not directly subject to monitoring by many of the agencies which most often are responsible for checking on radiation safety. In some states nonlicensed possession falls under the purview of occupational health and in others it may be the responsibility of the Environmental Protection Agency. There does not appear to be a unified approach and certainly in New York and Massachusetts, those states with which I am most familiar, it is exceedingly difficult to find a proper governmental agency to dispose of the material. Given then the possibility of having the Nuclear Medicine Department dispose of it, you are faced with a cost which may be insurmountable. At the present time both Nevada and Washington are accepting radium for disposal at their sites under very strict guidelines. The State of Washington allows the disposal of up to 10nCi of radium per gram of material without prior approval, and for amounts of 11 to 100 nCi specific approval is required. Amounts greater than 100 nCi are not accepted for disposal at these sites. These small amounts can be shipped in a standard container. Nevada is more demanding and requires certification of shipments as to proper container, proper handling and proper surface exposure levels. The permit fee for radium shipment is $3,100, although a proposal for a low volume generator fee of $100 to $500 is pending at this time. The radium is not specifically limited to quantity but must be in a sealed container (Fig 9). The directions for radium packaging for shipment to Nevada used in our institution are shown in Table 3

Obviously the problem with encountering radium from these many possible sources noted above does not stop with its identification. Identification may be the beginning of the problem. The simplest solutions would appear to be either to lock it in a safe for radioactivity, or perhaps send it to me. ACKNOWLEDGMENT The author wishes to thank Harold Marcus and Jeffrey Brown for their kind help in surveying the devices described here and for providing a number of valuable reference sources. REFERENCES [1] Taft, R. B. (1938). Radium Lost and Found. Charleston, SC: JNO. J. Furlong. [2] Skin lesions and radioactivity in jewelry. FDA Drug Bull 11, 3–4. [3] Radiation Exposure from Consumer Products and Miscellaneous Sources, NCRP National Council on Radiation Protection and Measurements: Washington, DC, Nov 1, 1977, Report No. 56 [4] Moghissi, A. A., Pasas, P., & Carter, M. W., et al. (Eds.). (1978). Radioactivity in Consumer Products. US Nuclear Regulatory Commission. NUREG/CP-0001. [5] Constable, A. R. (1987). Radioactivity in Scientific Instruments. Bull Scientific Inst Soc 12, 9–10. [6] Blaufox, M. D. (1983). Antique Hazards: "A Latter Day Encounter with Radium. J Nucl Med 24, 79–82. [7] Eisenbud, M. (1973). Environmental Radioactivity. San Diego: Academic. [8] Cramp, A. J. (1936)Nostrums and Quackery and Pseudo-Medicine 3. Chicago: Press of the American Medical Association. [9] Cramp, A. J. (1921)Nostrums and Quackery 2. Chicago: Press of the American Medical Association. [10] Nostrums and Quackery 11911. Chicago: Press of the American Medical Association. [11] A Review of the Department of Transportation (DOT) Regulations for Transportation of Radioactive Materials (1977). Washington, DC: US Department of Transportation, Materials Transportation Bureau, Office of Hazardous Materials Operations.

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