Kaj Eli Roholm. Fluorine Intoxication. Copenhagen 1937

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To date, probably the best, most comprehensive documentation of fluoride interactions with living organisms.


FLUORINE INTOXICATION
A Clinical-Hygienic Study
With A Review Of The Litterature And Some Experimental Investigations.
By Dr. Kaj Eli Roholm

Published by NYT NORDISK FORLAG, Arnold Busck, Copenhagen 1937
Published by H.K. LEWIS & CO. LTD. 136 Gower Street, London 1937

Read Online Web.Archive.org
Download from Canadians Opposed to Fluoridation (COF-COF) (Large File - 413 Pages - 51 MB)
Download from Web.Archive.org (Large File - 413 Pages - 16 MB)

(Read below a quotation from a "White Paper: The Anti-Fluoridationist Threat to Public Health" which is the official response to public concern about fluoride's role in everyday life, from the medical profession, published by Institute for Science in Medicine (ISM) April 2012)

• Table of Content: see below
• Illustrations: see below
• Tables: see below
• Preface: read below
• Introduction: coming soon
• Sammenfatning (in Danish): read below

[Mod]

FLUORINE INTOXICATION
A Clinical-Hygienic Study
With A Review Of The Litterature And Some Experimental Investigations.
By Dr. Kaj Eli Roholm



Published by NYT NORDISK FORLAG, Arnold Busck, Copenhagen 1937
Published by H.K. LEWIS & CO. LTD. 136 Gower Street, London 1937

Table of Contents

TABLE OF CONTENTS

Preface (see below) V-VII
Introduction (coming soon) - 1

• The Chemistry of Fluorine Compounds
• History
• Own Investigations

PART I
A Review of the role played by fluorine in biology

Chapter I - IX (see: 1 - 9)

1. Fluorine intoxication in man - 9

1. Local Effect
2. Acute Poisoning
   a. Frequency and Form
   b. Clinical Symptoms
   c. Morbis Anatomy
   d. Toxic and Lethal Dose
3. Chronic Poisoning
   a. Sporadic Cases
   b. Poisoning with Cryolite
   c. Mottled Enamel

2. Intoxication of plants and animals - 36

1. Injuries to Plants
2. Acute Poisoning of Animals
3. Chronic Poisoning of Animals
   a. Enzootics round Factories
   b. Darmous
   c. Domestic Animal Disease in Iceland after Volcanic Eruption
   d. Feeding on Fluoric Forage

3. Occurrence of fluorine in inanimate nature - 46

1. Minerals and Rocks
2. Soil
3. Water
4. Volcanoes

4. Distribution of fluorine in animate nature - 52

1. Plants
2. Bones and Teeth
   a. Presence of Fluorine
   b. Quantity
   c. Origin
   d. Form
3. Other Animal Tissues

5. Effects of fluorine on protoplasm and enzymes - 60

1. Protoplasm. Lower Organisms
2. Effect on Blood in vitro
3. Effect on Various Enzymatic Processes

6. Experimental investigations into the effects of gascous fluorine compounds - 64

1. Effects on Plants
2. Effects on Animals

7. Experimental acute and subacute fluorine intoxication - 67

1. Experiments on Man
2. Intoxication Symptoms in Animals
3. Morbid Anatomy
4. Effects on Various Tissues or Functions
   - The Blood
   - The Circulatory System
   - Musculature
   - The Central Nervous System
   - Glands
   - Renal Functions. N-Metabolism
   - Sugar Metabolism
   - Mineral Metabolism
   - Total Metabolism
   - Dental Tissue

8. Chronic experimental fluorine intoxication - 76

1. Growth. General Condition. Reproduction
2. Gastro-Intestinal Tract
3. Urinary System
4. Blood and Bone Marrow. Spleen
5. Nervous System and Musculature
6. Endocrine Glands
   a. Thyroid Gland
   b. Parathyroid Gland
   c. Other Glands
7. Various Functions
   a. Inorganic Components of the Blood
   b. Calcium and Phosphorus Metabolism
   c. Other Functions
8. Dental Tissue
   a. Gross Changes
   b. Treshold Values for rats
   c. Other Animals
   d. Histopathology
   e. Chemical Compositions
9. Bone Tissue
   a. Gross Changes
   b. X-Ray Picture
   c. Histopathology
   d. Strength and Chemical Composition

9. Absorption, storage and excretion - 103

1. Absorption
2. Storage
3. Excretion
4. Maternal Transfer

PART II
Techniques employed in own investigations

Chapter X (see: 10)

10. Technique - 111

1. Determining the Dust Quantity
2. Analytical Technique
   a. Preparation of Organic Material
   b. Qualitative Test for Fluorine
   c. Quantitative Determination of Fluorine
3. Histological Technique
4. Haematological Technique
5. Fluorine Compounds Used

PART III
Investigations into spontaneous cryolite poisoning

Chapter XI - XX (see: 11 - 20)

11. Cryolite and its manufacture - 121

1. Occurence and Mining
2. The Properties of Cryolite
3. Processes in Cryolite Manufacturing

12. Number and employment-period of workers - 130

1. Lenght of Employment-Period
2. Extent of Investigation
   - Medical History
   - Physical Examination

13. Complaints of workers - 136

1. Acute or Subacute Gastric Symptoms
2. Intestinal Symptoms
3. Symptoms from Circulation and Respiration
4. Symptoms from Bones, Joints and Muscles
5. Symptoms of Nervous Character
6. Skin Symptoms
7. Other Symptoms

14. Examination of osseous system - 141

1. Röntgen Examination
   - 1st Phase
   - 2nd Phase
   - 3rd Phase
2. Clinical Examination

15. Other results of physical examination - 148

1. General Condition
2. Teeth
3. Respiratory System
4. Circulatory System
5. The Blood
6. Nervous System
7. Endocrine Glands
8. The Skin
9. Urine
10. Sundry Examination

16. Examination of former cryolite workers - 162

1. Questionnaire on Discomfort of Work
2. Result of Röntgen Examination
3. Workers from the Cryolite Mine at Ivigtut

17. Morbidity and mortality - 169

1. Morbidity
2. The Various Affections
3. Mortality and Causes of Death

18. Post-mortem examination of two cryolite workers - 180

1. Cryolite Worker No. 55
   - Medical History
   - Clinical Examination
   - X-Ray Examination
   - Necropsy
   - Macroscopic Examination of Bones
   - Microscopic Examination of Bones
2. Cryolite Worker No. 200
   - Medical History
   - Clinical Examination
   - Bones
3. Analyses

19. Examination of children of female cryolite workers - 195

1. The mother is a former worker No. 100
2. The mother is a former worker No. 98 at the factory
3. The mother is a former worker born 1870

20. Survey of spontaneous cryolite intoxication - 200

1. Agent and Dose
2. Subjective Symptoms
3. Physical Findings
4. Pathological Anatomy
5. Biochemistry
6. Pathogenesis
7. Diagnosis
8. Prognosis

PART IV
Own experimental investigations

Chapter XXI - XXIV (see: 21 - 24)

21. Experiments on rats - 213

1. Technique
2. Subchronic Intoxication
3. Chronic Intoxication
   - Growth and Mortality
   - Attitude and Gait
   - Symptoms from Alimentary Canal
   - Skin and Eye Symptoms
   - Teeth
   - Form and position anomalies
   - Organs
   - Bones
   - Microscopic Examination
4. Summary

22. Experiments on pigs - 225

1. Technique
2. Course of Experiment. Symptoms
3. Organs
4. Bones
5. Teeth
6. Analyses
7. Summary

23. Experiments on calves - 234

1. Technique
2. Course and Experiment. Symptoms
3. Blood and Organs
4. Bones
5. Teeth
6. Analyses
7. Summary

24. Experiments on dogs - 244

1. Technique
2. Course of Experiment. Symptoms
3. Blood and Organs
4. Bones
5. Teeth
6. Analyses
7. Summary

PART V
Discussion and general conklusions

Chapter XXV - XXX (see: 25 - 30)

25. The normal fluorine content of organic material - 257

1. The Analytical Problem
2. Vegetable Tissue
3. Bones
4. Teeth
5. Other Animal Tissues

26. Acute fluorine intoxication - 262

1. Clinical Symptoms
2. Morbid Anatomy
3. The Dose
4. Pathogenesis
5. Diagnosis
6. Prognosis and Therapy

27. Chronic fluorine intoxication - 269

1. Clinical Symptoms
2. Morbid Anatomy
   - Gastro-Intestinal Tract
   - The Kidney
   - The Teeth
   - Bone Marrow. Spleen
   - Other Organs
3. Biochemistry
   - Absorption and Excrection
   - Composition of the Blood
   - The Organs
   - The Bones
   - Metabolism
4. The Question of the Dose
5. Pathogenesis
6. Diagnosis
   - The Dental Anomaly
   - Osteosclerosis
   - The Osteomalacic Condition
7. Prognosis and Therapy
   - Dental Anomaly
   - Osteosclerosis
   - Osteomalacia

28. Posibilities of intoxication - 292

1. Occurrence of Fluorine
   - Drinking Water
   - Food
   - Volcanoes
2. Extraction of Fluoric Minerals
3. Industrial Use of Fluorine Materials
4. Various Uses of Fluorine Compounds in Technical Processes
5. Use of Superphosphate
6. Fluorine Compounds as a Poison for Noxious Animals and Plants
7. Employment of Fluorine Compounds in the Food Industry
   - Wine
   - Fruit Juice
   - Other Food
8. Use of Fluorine in Therapy
   - Pulmonary Tuberculosis
   - Bones. Teeth.
   - Hyperthyroidism
   - Disinfection
   - Other Uses

29. Prophylactic problems - 307

1. Trade in Fluorine Compounds
2. Use as Preservative in Food
3. Use as Insecticide
4. Undustrial Problems
5. Other Prophylactic Problems

30. The physiological role of fluorine - 312

1. The Necessity of Fluorine
2. Stimulating Effect of Small Quantities of Fluorine
3. The Action of Fluorine in Physiological Doses

PART VI

Summary - 316

- Occurrence of Fluorine in Nature
- Effect of Enzymatic Processes and Protoplasm
- Fluorine Compounds
- Acute Intoxication
- Chronic Intoxication
- Mode of Action of Fluorine
- Possibilities of Intoxication
- Prophylaxis

Sammenfatning (in Danish read below) - 322

- Fluors forekomst i naturen
- Virkning paa enzymatiske processer og protoplasma
- Fluorforbindelser
- Akut forgiftning
- Kronisk forgiftning
- Fluors virkemaade
- Forgiftningsmuligheder
- Profylakse

Bibliography - 328

- 36 Pages
- 893 References

ILLUSTRATIONS (see below)

TABLES (see below)

[Mod]

FLUORINE INTOXICATION
A Clinical-Hygienic Study
With A Review Of The Litterature And Some Experimental Investigations.
By Dr. Kaj Eli Roholm



Published by NYT NORDISK FORLAG, Arnold Busck, Copenhagen 1937
Published by H.K. LEWIS & CO. LTD. 136 Gower Street, London 1937

Illustrations

ILLUSTRATIONS
(Placed on or opposite page)

• Mottled teeth in man - figure 1 - page 32
• Spontaneus intoxication in sheep - figure 2-9 - page 42
• Apparatus for determination of dust - figure 10 - page 111
• Processes in cryolite manufacturing - figure 11-15 - page 124
• Radiographs of cryolite workers - figure 16-31 - page 144
• Diagram illustrating occurence of osteoscrelosis - figure 32 - page 145
• Picture of cryolite worker - figure 33 - page 145
• Necropsy findings in cryolite workers - figure 34-46 - page 184
• Mottled teeth in children of cryolite workers - figure 47 - page 184
• Weight curves for rats - figure 48-51 - page 216
• Weight curves for rats - figure 52 - page 223
• Intoxication in rats - figure 53-60 - page 224
• Weight curves for pigs - figure 61 - page 226
• Intoxication in pigs - figure 62-76 - page 232
• Weight curves for calves - figure 77 - page 336
• Intoxication in calves - figure 78-90 - page 240
• Intoxication in dogs - figure 91-96 - page 248

TABLES (see below)

[Mod]

FLUORINE INTOXICATION
A Clinical-Hygienic Study
With A Review Of The Litterature And Some Experimental Investigations.
By Dr. Kaj Eli Roholm



Published by NYT NORDISK FORLAG, Arnold Busck, Copenhagen 1937
Published by H.K. LEWIS & CO. LTD. 136 Gower Street, London 1937

Tables

TABLES

1. The water Solubility of Some Fluorine Compounds - Page 2
2. Acute, Fatal Fluorine Intoxications 1873-1935 - Pages 12-23
3. Acute, Non-fatal Fluorine Poisoning 1873-1935 - Pages 24-25
4. Frequency of Each Symptom in 34 Cases of Acute Fatal Fluorine Poisoning - Page 27
5. Pathologico-Anatomical Changes in 32 Cases of Acute Fluorine Intoxication - Page 28
6. Approximate Toxic and Lethal Dose in Acute Fluorine Poisoning in Man - Page 30
7. Fluorine Content in Natural Water - Page 48
8. Volcanoes Emitting Fluorine - Pages 50-51
9. Analyses of Normal Fluorine Content in Bones and Teeth - Pages 55-56
10. Fluorine Content of Normal Organs Page 58
11. Dosis minima letalis of various Fluorine Compounds - Page 69
12. Experimental Fluorine Intoxication - Pages 78-83
13. Deposition of Fluorine in a Dog which received Sodium Fluoride perorally - Page 104
14. Storage of Ingested Fluorine in Bones and Teeth - Pages 104-105
15. Determination of Error of Willard and Winther's Method of Fluorine Analysis - Page 114
16. Double Analyses of Fluorine Content in Bone Ash, Willard and Winter's Method - Page 115
17. Gravimetric Determination of Dust Content in the Air at Various Working Places - Page 128
18. Grain Size in Dust Samples from Factory - Page 129
19. Employment Period of Discharged Male and Female Cryolite Workers - Page 131
20. Age Distribution of Examined Cryolite Workers - Page 132
21. Period of Employment of Examined Cryolite Workers - Page 133
22. Frequency of Various Complaints by Cryolite Workers - Page 137
23. Frequency of Complaints Arranged in Groups - Page 138
24. Frequency of Osteosclerosis and its Relations to Period of Employment, Exposure to Dust etc. - Page 144
25. Relationship between Osteosclerosis and Restriction of Motility in Columna - Page 147
26. Condition of Teeth in 66 Cryolite Workers - Page 149
27. Grequency of Pulmonary Found by X-ray Examination - Page 150
28. Relation between Period og Enployment and Occurrence of Pulmonary Fibrosis - Page 151
29. Relation between Changes in Lungs and Bones in Cryolite Workers - Page 152
30. Average of Blood Composition in Cryolite Workers - Page 155
31. Relation between Osteosclerosis and Blood Picture - Page 156
32. Serum Calcium of Cryolite Workers - Page 159
33. Fluorine Content in Teeth of Cryolite Workers Compared with Normal Teeth - Page 160
34. Frequency of Various Complaints of Former and Present Cryolite Workers - Page 163
35. Relation between Lenght of Employment and Frequency of Certain Complaints among Cryolite Workers - Page 163
36. Frequency of Osteosclerosis and Pulmonary Fobrosis among Former Cryolite Workers - Page 164
37. Results of Röntgen Examination of 9 Male Workers from the Cryolite Mine at Ivigtut, Greenland - Page 167
38. Morbidity of Cryolite Workers in the Period January 1st, 1923 til January 4th, 1933, recorded by the Factory - Page 169
39. Morbidity before, during and after Employment at the Cryolite Factory, Recorded by Sick-Clubs - Page 170-171
40. Distribution of Sick-Days over Individual Diseases or Disease-Groups - Page 174-175
41. Cause of Death and Post-mortem Examination of Former Cryolite Workers - Page 176-177
42. Fluorine Content in Organs of Cryolite Workers - Page 192
43. Fluorine Content of Bones in Cryolite Workers - Page 193
44. Fluorine Content in Costae (Rib/red.) of Normal Individuals - Page 193
45. Data concerning Rats 1-25 - Page 214
46. Data from Experiment on Pigs, Concerning Stabling of Animals, Fluorine Compounds Used, Weight - Page 226
47. Change of Form of Corpus Mandibule in Pigs - Page 229
48. Fluorine Content of Organs in Pigs - Page 231
49. Fluorine Content of Bones and Teeth in Pigs - Page 232
50. Intoxication Symptoms in Calves - Page 235
51. Blood Picture in Calves - Page 238
52. Fluorine Content of Bones and Teeth in Calves - Page 242
53. Summary of Doses of Fluorine Compounds used in Experiments with Dogs - Page 246
54. Blood Picture in Dogs after Fluorine Ingestion - Page 247
55. Fluorine Content in Bones and Teeth of Dogs - Page 251
56. Fluorine Content of Bones and Teeth of Normal Animals - Page 259
57. Various Uses of Fluorine Compounds in Technical Processes - Page 299

[Mod]

FLUORINE INTOXICATION
A Clinical-Hygienic Study
With A Review Of The Litterature And Some Experimental Investigations.
By Dr. Kaj Eli Roholm



Published by NYT NORDISK FORLAG, Arnold Busck, Copenhagen 1937
Published by H.K. LEWIS & CO. LTD. 136 Gower Street, London 1937

Preface V-VII

PREFACE

Cryolite intoxication, a hitherto unknown disease among the workers at the Øresund Chemical Works, Copenhagen, was found in November, 1932, as a result of a profitable collaboration between the Industrial-hygienic Researches of the Inspectorate of Factories and Workshops and the X-ray Department of the Rigshospital. Professor P. Flemming Møller, the leader of that department, interested me in the disease and suggested that I should go more deeply into the problems of fluorine intoxication.

Through the medium of an appointment at private expense as Assistant Physician under the Inspectorate of Factories and Workshops, I was enabled to complete the principal part of the investigations which form the foundation of the present work. The material from the first investigation was placed at my disposal, including the blocks for the illustrations Figg. 16, 19—26, 28 and 29.

I wish to thank Professor Flemming Møller for inducing me to embark on the subject, for kind permission to examine my material by X-ray at the Rigshospital, for passing judgment on the radiographs of cryolite workers’ lungs, and for unflagging interest in my efforts.

To the Director of the Inspectorate of Factories and Workshops, Mr. E. Dreyer, and its Chief Physician, Dr. Sk. V. Gudjonsson, I tender my best thanks for their confiding the task to me and allowing me a free hand to complete it as well as for their interest and support. By his energetic labours for industrial hygiene in Denmark Dr. Gudjonsson laid the foundation on which this work was started.

A great deal of the work was done at the Copenhagen University Institute of Hygiene and the Budde Laboratory, to whose Director, Professor L. S. Fridericia, I am greatly indebted for hospitality, the best of facilities, and friendly interest. I am obliged to the staff of workers at the Institute for help and encouragement in the daily work. Miss Kirsten Becker and Miss Lotte Holm assisted me in tending the experimental animals and with the preparation of microscopic slides. Preparations were photographed in collaboration with Mr. Henrik Jensen and Mr. E. D. Lange. Some of the microphotographs are the work of Miss Margrete Falck, of the Copenhagen University Institute of Pathological Anatomy.

It would not have been possible to carry on the work without help and kindness from many quarters. Dr. O. Brinch discussed problems of bone pathology with me and gave me valuable guidance. Dr. J. Engelbreth-Holm assisted me in judging the microscopic organ changes. Mr. R. Bogvad, M. Sc, examined bone slides in the polarization microscope. Mr. H. Buchwald, the Chief Chemist, analyzed fluorine preparations for me and helped with the analytical part. Mr. C. J. Howitz, of Viborggaard Farm, Herlufmagle, and Mr. S. Hjortlund, the Veterinary Surgeon, Copenhagen, assisted me to tend and slaughter the large experimental animals.

Materials of many kinds, comprising case-records, radiographs, autopsy material and statistics, were entrusted to me by Professors H. M. Hou-Jensen, Poul Møller, K. Sand, Erik Warburg, and J. Collin, all in the Copenhagen University; Professor J. J. Hoist, School of Dental Surgery; Dr. M. Degerbal, Zoological Museum; the Chief Chemist H. H. Stevenius-Nielsen, of the Danish Fertilizer Company, Ltd.; Chief Physician G. Biering, Kommunehospitalet; Chief Physician Chr. I. Baastrup, Bispebjerg Hospital, and the Cryolite Mining and Trading Co. Ltd., Copenhagen.

The sending out of an international questionnaire was made possible through the kind assistance of Dr. Johs. Frandsen, Director of the Danish National Health Service, and the Ministry of Foreign Affairs.

With financial assistance from the Dano-Icelandic Union-Foundation I was able to undertake a journey to Iceland in the autumn of 1935 to investigate conditions connected with the sheep disease gaddur. When collecting literature I was given excellent help by many Danish and foreign libraries, but especially by the University Library in Copenhagen, where the officials were indefatigable in their readiness to assist. By means of a grant from the Budde Foundation I was able to make library studies in Berlin in the summer of 1934.

A number of investigators abroad very kindly placed materials of various descriptions at my disposal: Professor E. W. Baader, Berlin; Dr. M. Bonjean, Rabat; Professor J. Casares Gil, Madrid; Dr. Juan Chaneles, Buenos Aires; Air. H. T. Dean, D. S., Washington; Professor Niels Dungal, Reykjavik; Dr. Leon Goldemberg, Buenos Aires; Dr. F. S. McKay, New York; Professor L. Slagsvold, Oslo; Dr. Margaret C. Smith, Tucson, Arizona; Dr. H. Velu, Casablanca.

It was possible to accomplish the work in its present form through considerable financial support from the Øresund Chemical Works, Copenhagen. Mr. H. Tuxen, the Manager, Dr. A. Westergaard, the Secretary, as well as the employees and officials have displayed great interest in it and helped me in the course of my daily collaboration with them. So did Mr. C. F. Jarl, C. B. E., the Proprietor of the Works, who induced me to extend my investigations as far as possible in order to find out available prophylactic measures. The translation of the book is the work of Mr. W. E. Calvert, Copenhagen.

I tender my most cordial thanks to all who in any way have aided me in my work.

Kaj Roholm

Blegdamshospitalet, Copenhagen N.

February 1937

[Mod]

FLUORINE INTOXICATION
A Clinical-Hygienic Study
With A Review Of The Litterature And Some Experimental Investigations.
By Dr. Kaj Eli Roholm



Published by NYT NORDISK FORLAG, Arnold Busck, Copenhagen 1937
Published by H.K. LEWIS & CO. LTD. 136 Gower Street, London 1937

Introduction

INTRODUCTION (coming soon)