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506 LCGC VOLUME 19 NUMBER 5 MAY 2001 www.chromatographyonline.

com

The Birth of Partition


Chromatography
in
Milestones Chromatogra
in
I
n June of 1941, almost exactly 60
When still in high school, Martin
became fascinated by fractional
distillation and even built in the
basement of his house some

phy years ago, the (British)

Milestones Biochemical Society held its


214th meeting in London, at
At this meeting, A.J.P. Martin and R.L.M. graduated in 1932 and Synge in 1936.
Synge, two young chemists (Martin was 31 long distillation columns from empty coffee
and Synge 26) presented a paper on the cans, soldered together. He originally
separation and determination of the mono planned to be a chemical engineer, but at
amino monocarboxylic acids present in wool Cambridge he changed to biochemistry upon
using a new method (1). This lecture and its the influence of Professor J.B.S. Hal dane. As
subsequent detailed publication rep resent a teenager, Synge had already become
the birth of partition chromatography (2). fascinated by how living things functioned
On the occasion of the 60-year Exactly 10 years later, Martin and another and, thus, he also majored in biochemistry at
anniversary of the invention of young scientist, 29-year-old A.T. James, Cambridge.
submitted the manuscript of a major paper After graduation, both Martin and Synge
partition chromatography and the
that described an extension of parti tion remained at Cambridge as graduate stu
50-year anniversary of the chromatography in which the mobile phase dents, although their paths had not yet
introduction of gas–liquid partition was a gas (3). This publication repre sents crossed. Martin joined the Dunn Nutri tional
the birth of gas–liquid partition chro Laboratory and was involved in research on
chromatography, this installment of
matography (GLPC). vitamin E. He started separating carotenes
“Milestones in On the occasion of these two anniver saries, by distribution between two sol vents using
Chromatography” we shall discuss in this “Milestones in separating funnels. Being always interested in
Chromatography” column these milestones, engineering, he eventually built a very
discusses the
probably the most important in the long complicated laboratory machine, consisting
circumstances that led to these evolution of chromatography since its dis of 45 5-foot-long tubes con nected to one
developments and outlines the work covery by M.S. Tswett almost 100 years ago. another and serving as the extraction
Without these inventions, this magazine funnels: 90 ball valves rattling loudly on their
of A.J.P. Martin, R.L.M. Synge, A.T.
would not exist and most of our readers seats prevented the liquid from dropping
James and their co would have some other job, maybe titrating back to the previous tube. In this machine
workers, which opened new chapters or trying to isolate chlorophyll from some (details of which have never been published
hundreds of kilograms of dried stinging net but were only included in his doctoral thesis)
in
tle, as done in Willstätter’s laboratory 96 Martin could carry out very efficient
chromatography. years ago (4). countercurrent extraction.
The invention of partition chromatogra phy Meanwhile, Synge was active at the uni
and the development of GLPC are fas versity’s biochemical laboratory, and in 1938
cinating stories. Fortunately, they are he was offered an unusually generous schol
recorded fairly well in the Nobel Lectures of arship by the International Wool Secretariat
Martin (5) and Synge (6) and in the per sonal (IWS). Interestingly, both Martin and Synge
recollections of the principal players (7–10). had seen demonstrations of the potential of
I also had the honor of personally knowing adsorption chromatography during this time.
them, discussing with them a number of Martin participated in a lecture by Dr.
times the background of their pioneering Winterstein of Kuhn’s laboratory (in Heidel
work. This column is based on these berg, Germany) showing a chromatographic
publications and personal informa tion. separation on a short CaCO3 column.
Although Martin immediately recognized the
The Start at Cambridge University Both similarity between the chromatographic
Leslie S. Ettre Martin and Synge were students at technique and the theory of distillation, he
Milestones in Chromatography Editor
Cambridge University in England — Mar tin did not further pursue this subject at the
the National Institute for Medical Research.
time. However, he evidently stored this time, Synge also saw a demonstration of the According to his recollections, “Everybody
observation in his memory. About the same chromatography of sea urchin pigments.
www.chromatographyonline.com MAY 2001 LCGC VOLUME 19 NUMBER 5 507
and water. Encouraged by the distinct but problems always remained. Thus,
stood around and goggled at the pretty col
differences although their work on the separation of
ors but no explanation was forthcoming
found, the next logical step would have the monoamino monocarboxylic acids
from anyone present for how the
been to try to carry out separation by present in wool using countercurrent
undoubted separations had come about.”
liquid–liquid extraction. At that time it was extraction was published (11), it really
Thus, it remained just a curiosity to him,
suggested to Synge to contact Martin, who could not be termed as satisfactory.
inspiring no further interest in the
obviously had a lot of experience in the In 1940, Martin had a radically different
technique.
extraction process and whose unorthodox kind of idea: to pack a glass tube with a
large glass machine for countercurrent dis mixture of wool and cotton, with the fibers
Beginning of the Cooperation Between
tribution was well known in the chemistry parallel to the axis of the tube, and to have
Martin and Synge The IWS was
and biochemistry circles of Cambridge. the chloroform flow above, and the water
maintained by the wool growers of With this step, their five-year and very suc flow below, the packing. The idea was that
Australia, New Zealand, and South Africa. cessful cooperation started. the fibers would separate the two flows,
Among other things, its aim was to fund but the amino acids would distribute
research on various aspects of wool. It was The Birth of differen tially between the two solvent
proposed to Synge to study in detail the Partition Chromatography Because flows. How ever, it really did not work as
amino acid composition of wool, and also Martin’s existing apparatus was not hoped. Martin realized that the problem
to try improving the methods of amino suitable for use with a chloroform– water was related to cre ating equilibria in two
acid analysis, which were still done on a system, he designed a completely dif ferent liquids moving con tinuously in the
fairly primitive basis. This suggestion fit machine, now for continuous-flow, opposite direction. Then, suddenly he
well his research activities at that time in liquid–liquid countercurrent extraction. found the solution: it was not necessary to
the field of glycoproteins. One of the Meanwhile, he moved to the laboratories move both liquids, but only one, keeping
meth ods used was to acetylate digested of the [British] Wool Industries Research the other stationary in the tube. This was
egg albu min and remove the N-acetyl Asso ciation in Leeds, United Kingdom. the birth of partition chro matography.
amino acids and peptides from the Synge joined him there, bringing with him Martin and Synge decided that water
carbohydrate moiety by exhaustive the IWS scholarship. This new machine should serve as the stationary phase and
was set up there. As Martin mentioned, “It chloroform as the moving phase. They
extraction with chloroform.
was a fiendish piece of apparatus,” with 39 impregnated silica gel (used otherwise as
Beginning his activities under the aus
theo retical plates. The two operators had the drying agent in a balance case) with
pices of the IWS, Synge first measured water, packed the column with it, added
to watch it in 4-h shifts, continually battling
the partition coefficients of acetyl amino the
drowsiness due to chloroform vapor. The
acids between two phases: chloroform
machine was redesigned a number of times
508 LCGC VOLUME 19 NUMBER 5 MAY 2001 www.chromatographyonline.com
for publication; it was finally received on by Martin and Synge was that it could not
acetylamino acid mixture onto the top,
19 November by the editor of Biochemical be used for the analysis of dicarboxylic
and poured chloroform down the column.
Journal. However, its publication was acids: the silica packing materials intended
Addition of methyl orange indicator to the
almost instantaneous: it was already to serve only as a support for water
water permitted it to follow the amino
included in the December 1941 issue of adsorbed them. Thus, another material
acids passing through the column as red
the journal (2). This paper, entitled “A had to be found. The first thought was to
bands. In the first experiment they sepa
New Form of Chromatogram Employing use filter paper. As mentioned by Martin,
rated acetylproline and acetylleucine, and
Two Liquid Phases,” consisted of two he had seen “paper chromatograms” used
collected the respective fractions.
parts. The first presented the theory of by
This sounds very simple. However, it
chromatogra phy, and the second reported dyestuff chemists to check the purity of
took Martin and Synge months of hard
on the deter mination of the higher dyes (they did not call it a chromatogram).
work to reproduce the conditions and
monoamino acids present in proteins. Martin and Synge tried the technique, plac
obtain satisfactory results. The main prob
It may be interesting to mention ing a drop of the solution of two amino
lems were associated with questions that
that at that time Martin and Synge pre acids in the center of the paper, which was
today sound trivial: the preparation of the
ferred to speak of this new technique as impregnated with water (the stationary
proper silica gel, the use of the proper chlo
liquid–liquid chromatography — the phase). Butanol (the mobile phase) moved
roform, and how to apply the indicator
phrase partition chromatography was men up the paper by capillary action and even
and initiate the fraction collection. During
tioned only once in the paper, between tually reached its edge, moving the two
this time, Martin also developed the theory
quotation marks. However, in subsequent amino acids at different speeds.
of chromatography, applying the
years this expression became more and Meanwhile, A.H. Gordon, a new addition
theoretical plate concept from distillation
more used, and the citation of Martin to their team, was searching for a suitable
(which he already learned while in high
and Synge’s 1952 Nobel Prize in color reaction that could reveal the amino
school).
Chemistry specifically mentions their acids on the paper, and he found a
As mentioned in the introduction, Mar
fundamental work resulting in the description in Beilstein’s Handbuch der
tin and Synge presented the first report Organischen Chemie of the ninhydrin reaction
“invention of parti tion
on their work in June 1941, at the that was adapted for this purpose.
chromatography.”
meeting of the [British] Biochemical Subsequently they devel oped a more
Society. They convenient setup that involved the use of
Paper Chromatography
were slow with finishing the manuscript paper strips placed in a closed container in
An essential problem of the column used
which the air was saturated with water and classic article represents the start of paper Amino acids, which were formerly sep
the tops of the strips were dipped into chromatography. arated by laborious techniques of
troughs containing the mobile phase. Although liquid–liquid partition chro organic chemistry and where large
After this initial success, many different matography carried out in a column had quantities of protein hydrolysates were
solvents were tried and the possibility of only relatively few followers, the use of needed, could now be separated in
separating increasingly complex mixtures paper chromatography advanced very microgram amounts and visualized . . .
was investigated. However, no single sol rapidly. This mainly was due to the remark [Paper chromatography] would allow
vent was able to resolve a mixture of all able simplicity of the method. At that one within the space of a week to
common amino acids. Therefore, they time, filter papers of standardized quality carry out first a test for homogeneity
successfully tried what we now call two were commercially available and the and then a structural analysis of an
dimensional chromatography. After develop necessary setup was within the reach of oligosac charide, which until then
ing the chromatogram on the paper strip every labora tory. Naturally, this had not could very well have occupied the
in one dimension, they turned the paper always been so, and Martin’s group had three years of a Ph.D. dissertation
90° and used a different solvent to further had many difficul ties at the beginning. using Haworth’s technique of
sepa rate the spots formed in the first The situation was amply characterized by exhaustive methylation, hydrolysis, and
develop ment. Today, as electrophoresis Consden, in the preface he wrote 10 years identification of the methylated
enjoys its renaissance, it may be interesting later to the Eng lish edition of F. Cramer’s monosaccharides.”
to men tion that in the very first textbook on paper chromatography (16): As mentioned earlier, Synge left the
experiment of two-dimensional “Like other established methods, paper team before the completion of the
chromatography, the first development chromatogra phy was not brought into the development of paper chromatography.
was done by electrophoresis. However, world with out considerable birthpangs, However, he remained in contact with his
they did not pursue this tech nique at that and much could be written about these former col leagues. Synge’s interest at that
time. early adven turous days.” time turned to the investigation of the
Synge participated in the initial work Using paper chromatography, amino acid com position of the antibiotics
(12,13), but he left Leeds in 1943 to join separation required only a relatively short tyrocidin (18) and gramicidin S (19–21).
the Lister Institute of Preventive time and surpassed any techniques known The latter work was particularly important:
Medicine at that time. A good characterization of Synge was the first who was able to
in London, thus ending his participation the impact of paper chromatography was elucidate the amino acid sequence in a
in the final development of the technique. given by W.J. Whelan of the department of polypeptide, and for this he used mainly
Three scientists authored the main report biochemistry and molecular biology of the paper chromatography. This work
on paper chromatography: Martin, Gor University of Miami who, from 1945 to represented the basis of the more
don, and R. Consden, a young chemist 1948, was a graduate student at the elaborate investigations of F. Sanger,
who meanwhile joined the team. This University of Birm ingham with Professor which determined the entire peptide
report was first presented on 25 March N. Haworth, the winner of the 1937 sequence of insulin and for which he
1944 at the Annual Meeting of the Nobel Prize in Chem istry (17): received the 1958
Biochemical Society (14) and then pub “The technological advance the tech
lished in the society’s journal (15). This nique represented was astonishing.
www.chromatographyonline.com MAY 2001 LCGC VOLUME 19 NUMBER 5 509
possible by treating kieselguhr — a ment: “The mobile phase need not be a liq
Nobel Prize in Chemistry. An excellent
diatomaceous earth–based product — by uid but may be a vapour . . . Very refined
summary of these investigations was
dichlorodimethylsilane vapor, rendering it separations of volatile substances should
given in Synge’s Nobel Lecture (6).
unwettable by the strongly polar solvents. therefore be possible in a column in which
Using such columns and systems, reversed permanent gas is made to flow over gel
Reversed-Phase Chromatography In
phase LC was introduced in 1949 and impregnated with a nonvolatile solvent.”
1948, Martin joined the staff of the first used for the separation of lauric However, gas–liquid partition
Medical Research Council, first at the chromatogra phy (GLPC) had to wait 10
Lister Institute and shortly thereafter at (C12) to stearic (C18) acids (22).
For more than two decades the wide years until it finally became reality.
the National Institute for Medical We often find remarks in the chroma
Research in London. At the Lister spread use of reversed-phase LC was hin
dered by the lack of suitable stationary tography literature questioning the reasons
Institute, the prob lem of separating for the 10-year delay in picking up this
longer-chain fatty acids by liquid phases and an understanding of the under
lying physicochemical phenomena. In very clear and unequivocal suggestion.
chromatography (LC) arose. However, the However, this can be easily explained. Let
existing system of having a polar fact, a 1972 publication by the IUPAC
(23) indicated that reversed-phase LC is us not for get that in 1941, World War II
stationary phase and a less-polar mobile was raging and the United Kingdom was in
phase was unsatisfactory for this purpose: “a tech nique of only historical interest.”
However, the situation changed in the her most difficult period. British journals
the partition coefficients of such could be received in only a few countries,
substances favored too much the first part of the 1970s, and today
reversed-phase LC is the foremost liquid and the whole of continental Europe was
less-polar phase. Therefore, Martin started under German domination. In fact, even
to investi gate the possibility of having a chromatographic technique.
after the war, the 1941–1945 issues of
two-phase system in which the less-polar many jour nals were missing from libraries.
phase is sta tionary. Various attempts were Gas–Liquid
When communication was finally restored,
tried, but these were not satisfactory: the Partition Chromatography The
paper chromatography was the most
problem was to find a hydrophobic introduction of the 1941 publication of
exciting new technique, and most people
support material for the less-polar Martin and Synge on liquid–liquid chro
did not (or could not) go back to the basic
stationary phase. Finally, this became matography (2) contained the famous state
1941 publi cation.
There also was another reason why the chemists (mainly in Germany) that longitu promi nent German scientist, best
analogy to gas-phase separation did not dinal diffusion in a gas stream was so articulated this belief in a lecture during
become obvious. At that time there was a rapid that it would prohibit the existence the meeting of the German State Office
general belief among prominent physico of any small, discrete, and separate zones for Economic Devel-
with dif ferent compositions. E. Wicke, a
510 LCGC VOLUME 19 NUMBER 5 MAY 2001 www.chromatographyonline.com
processes in petroleum refining and in the
opment, held on 5 April 1940. The subject
petrochemical industries required
of his lecture was a summary of the
improved analytical controls that were no
possible chemical separation methods.
longer pos sible by the old laboratory
Among these, he mentioned
techniques. GC provided the ideal way to
chromatography; how ever, he stated that
solve these prob
the use of a chromato graphic method
with a gas as the means of elution seemed
nearly without prospect, owing to the
mixing in the direction of flow (24).
Thus, it was up to Martin to finally
prove the validity of their original predic
tion. When in 1950 he moved to the
National Institute for Medical Research, he
invited A.T. James, a young scientist he
met at the Lister Institute, to join him
there. Martin’s original idea was to develop
a countercurrent column procedure using A.J.P. Martin receiving the 1952 Nobel Prize in
crystallization as the basic distribution sys Chemistry from King Gustav VI Adolphus of
tem. However, after a few months of inten Sweden. (Courtesy of the Nobel Foundation,
sive work, no results were obtained, and Stockholm, Sweden.)
James became very discouraged. solution, and the amounts of the eluted
Therefore, “to improve James’ morale” (as compounds were determined by titration,
said in Mar tin’s personal recollections), first manually; however, soon Martin con
R.L.M. Synge receiving the 1952 Nobel Prize in
Martin sug gested that they go back to the structed a very elegant automatic titration
Chemistry from King Gustav VI Adolphus of
1941 pre diction and try using a gas as the machine for this purpose. It was also real Sweden. (Courtesy of the Nobel Foundation,
mobile phase in chromatography. The ized that for higher-boiling compounds Stockholm, Sweden.)
impetus to this was actually given by an the column must be heated: therefore, a lems; within a couple of years, however, it
inquiry from one of Martin’s colleagues, steam jacket was used for the column. was used for the analysis of almost every
looking for a more refined method than Parallel to these investigations, Martin type of organic compound. Martin person
paper chromato graphy to separate fatty also expanded the theory of partition ally facilitated the rapid spread of the tech
acids. chromatography by considering the nique. He had early contact (even before
In the unsuccessful crystallization compressibility of the gas used as the the publication of their seminal paper)
experi ments, long columns packed with mobile phase. with scientists from major industrial
Celite were used. Celite lso was used for Their preliminary report on “liquid–gas organiza tions and not only demonstrated
the gas chromatography (GC) columns, partition chromatography” was presented the tech nique but also advised them on
with a sili cone oil used as the stationary at the 20 October 1950, meeting of the how to simplify it by, for example, using
phase to coat the Celite particles. They Bio chemical Society (25). At that time, syringe injection and a thermal
first tried the lower fatty acids, but these manual titration was still used for conductivity detector.
gave consider able trouble due to detection; the automated titrator was
dimerization on the col umn. To prevent developed by Mar tin in the subsequent The 1952 Nobel Prize in Chemistry The
this, 10% of a nonvolatile acid (stearic months, and its description was included invention of partition chromatography
acid) was added to the station ary phase. in their final paper also discussing the earned Martin and Synge the 1952 Nobel
The column’s end was dipped into a test theory and the separation of C1–C12 acids. Prize in Chemistry, a richly deserved recog
tube containing an indicator The manu script of this paper was nition. The announcement of this award
submitted on 5 June 1951 to the editor of in Nature concluded with the statement:
Biochemical Jour nal; it is, however, “The methods evolved by Martin
interesting that while the 1941 paper by and Synge are probably unique by
Martin and Synge was pub lished within virtue of simplicity and elegance of
one month after receiving the manuscript, conception and execution, and also by
now it took almost 10 months. Then a few the wide scope of their application. It
months later, two additional papers were is likely that their invention will be con
published demonstrating the use of GLPC sidered by future generations as one
for the separation of ammo nia, aliphatic of the more important milestones in
amines, and pyridine homo logues (26,27). the development of chemical
The impact of GLPC on analytical sciences” (28). In fact, the impact of
chemistry was tremendous and almost partition chro
instantaneous. It was the right method matography has not been restricted to
introduced just at the right time, when the the chemical sciences. It also laid the
founda tion for the explosion of our On the occasion of the centenary of the Royal
Institute of Chemistry, the British Postal Service
knowledge in
issued four stamps on 2 March 1977 honoring
biochemistry and biology, which is still British achievements in chemistry. This stamp
continuing with no slowdown in sight. honored the 1952 Nobel Prize of Martin and
All these developments are living proof Synge. The text on the stamp incorrectly men
tions “starch chromatography.”
of the genius of the inventors of partition
chro matography, particularly that of
A.J.P. Martin.
At a symposium held in 1969, Yale Uni
versity Medical School Professor S.R. Lip
sky, himself a pioneer in extending the
use of GLPC into biochemistry, finished
his
512 LCGC VOLUME 19 NUMBER 5 MAY 2001 www.chromatographyonline.com
Biochem. J. Proc. 38, ix (1944).
lecture titled “Gas Chromatography: (15) R. Consden, A.H. Gordon, and A.J.P. Martin,
The Anatomy of a Scientific Revolution” Biochem. J. 38, 224–232 (1944).
(29) with the following words of tribute (16) F. Cramer, Paper Chromatography (Macmillan,
to Dr. Martin: London, 1954).
“He has twice made outstanding (17) W.J. Whelan, FASEB J. 9, 287–288 (1995). (18)
A.H. Gordon, A.J.P. Martin, and R.L.M. Synge,
contributions to this field — in his dis Biochem. J. 37, 313–318 (1943). (19) A.H. Gordon,
covery of partition chromatography A.J.P. Martin, and R.L.M. Synge, Biochem. J. 37,
and in his pioneering work on gas 86–92 (1943).
chromatography. He has thus altered, (20) R.L.M. Synge, Biochem. J. 39, 363–367 (1945).
for the better, the lives of many of us. (21) R. Consden, A.H. Martin, A.J.P. Martin, and
We, his scientific colleagues, thank R.L.M. Synge, Biochem. J. 41, 596–602 (1947). (22)
G.A. Howard and A.J.P. Martin, Biochem. J. 46,
him for allowing us to share with him
532–538 (1950).
this wonderful adventure.” (23) Recommendations on Nomenclature for Chro
There is nothing I could add to this matography (IUPAC Secretariat, Oxford, United
tribute. Kingdom, February 1972).
(24) E. Wicke, lecture presented at the session of
References the German Reichsamt für
(1) A.J.P. Martin and R.L.M. Synge, Biochem. J. 35, Wirtsachaftsausbau, Berlin, Germany, 5 April
91 (1941). 1940.
(2) A.J.P. Martin and R.L.M. Synge, Biochem. J. 35, (25) A.T. James and A.J.P. Martin, Biochem. J. Proc.
1358–1368 (1941). 48(1), vii (1951).
(3) A.T. James and A.J.P. Martin, Biochem. J. 50, (26) A.T. James, A.J.P. Martin, and G.M. Smith,
679–690 (1952). Biochem. J. 52, 238–242 (1952).
(4) R. Willstätter, Aus meinem Leben: Von Arbeit, (27) A.T. James, Biochem. J. 52, 242–247 (1952).
Musse und Freunden (Verlag Chemie, Wein heim, (28) Nature (London) 170, 826 (1952).
Germany, 2nd ed., 1973), p.156. (29) S.R. Lipsky, in Gas Chromatography in Biology and
(5) A.J.P. Martin, in Nobel Lectures — Chemistry Medicine — A CIBA Foundation Symposium
1942–1962 (Elsevier, Amsterdam, 1964), pp. (February 5–6, 1969), R. Porter, Ed. (J&A
355–371. Churchill Ltd., London, 1969), pp. 11–16.
(6) R.L.M. Synge, in Nobel Lectures — Chemistry
1942–1962 (Elsevier, Amsterdam, 1964), pp.
372–387.
Leslie S. Ettre
“Milestones in Chro
(7) A.J.P. Martin, in Gas Chromatography in Biology
and Medicine — A CIBA Foundation Symposium matography” editor
(February 5–6, 1969), R. Porter, Ed. (J&A Leslie S. Ettre is a
Churchill Ltd., London, 1969), pp. 2–10. research affiliate of
(8) A.J.P. Martin, in 75 Years of Chromatography — A the chemical engi
Historical Dialogue, L.S. Ettre and A. Zlatkis, neering department
Eds. (Elsevier, Amsterdam, 1979), pp. of Yale University
285–296. and a member of
(9) R.L.M. Synge, in 75 Years of Chromatography — LCGC’s editorial advi
A Historical Dialogue, L.S. Ettre and A. Zlatkis, sory board. Direct
Eds. (Elsevier, Amsterdam, 1979), pp. correspondence about this column to “Mile
447–457. stones in Chromatography,” LCGC, 859
(10) A.T. James, in 75 Years of Chromatography — A Willamette Street, Eugene, OR 97401, e-mail
Historical Dialogue, L.S. Ettre and A. Zlatkis, lcgcedit@lcgcmag.com.
Eds. (Elsevier, Amsterdam, 1979), pp.
167–172.
(11) A.J.P. Martin and R.L.M. Synge, Biochem. J. 35,
91–121 (1941).
(12) A.H. Gordon, A.J.P. Martin, and R.L.M.
Synge, Biochem. J. Proc. 37, xiii–xiv (1943). (13) A.H.
Gordon, A.J.P. Martin, and R.L.M. Synge, Biochem.
J. 37, 79–86 (1943).
(14) R. Consden, A.H. Gordon, and A.J.P. Martin,

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