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History of Cryogenics: A Cryo Central resource from the CSA

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History of Cryogenics
From the Fall 1999 issue of Cold Facts magazine

April 18, 2008

Millennium Breakthroughs
A variety of CSA members give different perspectives on the past millennium: What were the most significant breakthroughs in cryogenics during the past millennium? 1. Prof. R.G. Scurlock, Kryos Technology, scurlock@soton.ac.uk (Breakthrough = way through obstacles Oxford English Dictionary) 1. Introduction My first response to this question was to suggest that the invention of Dewars dewar in 1892 should be on the list. Thinking a little more about the history of cryogenics, the technology for producing and using cold, the latter half of the 20th Century has seen a tremendous surge in the number and range of applications of cryogenics. Pinpointing the key technical achievements the breakthroughs which have enabled these applications to develop and go ahead on a commercial scale, is controversial because everyone will have his own list. I shall exclude achievements in low temperature physics, like the discoveries of superconductivity (low Tc in 1911, high Tc in 1986) or the identification of superfluidity in helium in 1938 or the first liquefaction of particular gases like oxygen in 1877, hydrogen in 1898, or helium in 1908. The history of breakthroughs in cryogenics and their consequences and impact on the world make fascinating reading. This article has developed into a long contribution; yet it is all too brief in its coverage. Over the first 840 years of the millennium, cryogenics was mainly concerned with the collection, storage and use of ice. There were no breakthroughs in a long established practice because at the beginning of preceding millennium, the Romans and others had collected ice for food preservation and snow for fruit sorbets. They were not the first, either, because the Chinese were using ice in food around 2000 BC. 2. Shipborne refrigeration: the first breakthrough, 1877, UK From about 1840 the technology of refrigeration started to develop using hazardous fluids like ethyl ether, ammonia and sulfur dioxide. The invention of the Bell-Coleman steam driven air-cycle refrigerator in 1877 was the breakthrough which enabled ship-borne refrigeration to develop (on sailing clippers! and steam ship) for transporting frozen meat from Australia, New Zealand and South America to Europe. The Bell-Coleman machine was a British (Scottish) invention and led directly to the domination of the frozen meat trade by British ships for the next 100 years or more. 3. Storage and transport breakthroughs 1. Dewars dewar, 1892, London UK When the young James Dewar was appointed Fullerian Professor of Chemistry at the Royal Institution, London, in 1877, he set about tackling the two obstacles to progress in cryogenics at that time. The first was the complete lack of understanding of heat transfer processes and of how to achieve thermal insulation; the second was the lack of basic data on the properties of fluids for producing low temperatures. For fifteen years progress

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History of Cryogenics: A Cryo Central resource from the CSA

was slow until, in 1892, he was able to employ his invention of the silvered, double walled, glass vacuum vessel to contain cryogenic liquids for the first time, for relatively long periods, before they evaporated. The idea of vacuum insulation had been used by Dewar and others as early as 1873 and he went on to show how he could obtain significant reduction (up to 6 times) in heat influx by introducing into the vacuum space powders such as charcoal, lamp black, silica, alumina and bismuth oxide the first vacuum insulated powder insulations. He also found that three turns of aluminum sheet was not as good as silvered surfaces. Had he gone on to apply further turns of aluminum, he would have discovered the principle of multi-layer insulation, which is superior to silvering. Nevertheless, his discovery of silvering as an effective means of reducing the radiated heat flux component was a breakthrough. From 1802, the glass dewar flask quickly became the standard container for cryogenic liquids, leading to the successful liquefaction of hydrogen and helium in later years. Dewar had considerable difficulty in finding competent glass blowers willing to undertake the construction of his doublewalled vessels, and was forced to get them made in Germany. By 1898, a ready supply became available. The discovery by German glassblower Muller of Coburn that a silvered vacuum flask could also be used for keeping milk hot overnight for feeding his baby, led to a major commercial development, the Thermos Flasche, for keeping liquids hot. The manufacture of Thermos flasks rapidly developed into an important industry, first in Germany and then in the UK and USA. Dewar never patented his silvered vacuum flask and never benefited financially from his invention. Following Dewars invention in 1892, the design of dewars for containing cryogenic liquids did not change for over 60 years, until the growing availability of helium in the 1950s gave rise to its use in open cryostats without liquid hydrogen shielding. 2. Vapor-cooled radiation shields, 1969, Southampton, UK One improvement on Dewars dewar was achieved by the discovery at Southampton, UK, of the vapor-cooled radiation shield, in 1969. This simple device enables the majority of ambient temperature radiation funneling down the neck to be absorbed by heating the cold vapor rather than by evaporating the liquid, thereby reducing the evaporation rate in a liquid helium cryostat or dewar by a factor of three or more. This device is also applicable to the large-scale storage of cryogenic liquids, for example via the use of a suspended deck in LNG storage tanks. 3. Vapor-cooled necks, 1975 USA and UK Further study of the convection in dewar necks led to the discovery of boundary layer flows with high heat transfer capability to the neck wall, together with reverse flow in the core of the vapor column. Quantifying these studies led to design criteria for the geometry of vapor-cooled neck walls to achieve minimum helium evaporation rate. These criteria are now in standard use for the design of containers for all cryogenic liquids. 4. Multilayer insulations, 1950s USA The evacuated multi layer insulation MLI technique another improvement on Dewars dewar was not developed until the requirement arose in the 1950s for lightweight insulation of cryogenic propellants for space rockets. Since then, MLI has become the standard insulation in most cryogenic liquid storage vessels and tanks. 5. Effect of improvements on Dewars dewar 1955-2000 One way of highlighting the improvements made on Dewars dewar is to consider how containment times of liquid helium systems have changed over 45 years. 1892-1995 Dewars dewar 4 hours 1965 +Vapor-cooled radiation shields 12 hours 1970 +Vapor-cooled necks 100 hours 1975 +MLI 100 days 1983 IRAS 300 days 2000 Space probes 1000 days In other words, in less than 30 years, the insulation performance has been improved 1000-fold over that of Dewars dewar, another breakthrough. It is this improvement that has led to the advent of todays miniature cryocoolers, capable of absorbing the residual heat flow through insulation in the absence of any cryogenic liquid.

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History of Cryogenics: A Cryo Central resource from the CSA

6. LNG tankers; 1960 trials by UK team While the improvement in performance of insulations has led to many applications, the scale of operation has increased dramatically, particularly with liquid hydrocarbons. The breakthrough in LNG technology came in 1960 with the conversion in the U.K. of a small crude oil tanker to a 5000m 3 LNG tanker, the Methane Pioneer, which was then used to carry the first trans-Atlantic trial shipments from the Gulf of Mexico to Canvey Island, UK. These led directly to the development of the 125,000m 3 LNG tankers operating around the world today. 4. Refrigeration breakthroughs Cold engines are the enablers of low temperatures, and there have been many breakthroughs including: 1. Freons, 1930 The development of halogenated hydrocarbons in 1930 led to the tremendous expansion in refrigeration and airconditioning from the 1940s onward. 2. Collins helium liquefier 1946, U.S.A. The Collins machine enabled many laboratories around the world to have liquid helium on tap for the first time. 3. MCR cycles 1958, Russia The use of multi-component refrigerants (MCR) cycles and their refinement by computational techniques to produce large natural gas liquefaction plants from 1964. The MCR cycle was first suggested by Kleemenko in 1958. More recently, from 1996, mixed hydrocarbon refrigerants have replaced the environmentally discredited Freons in the domestic refrigerator and air-conditioning markets, and have provided lower temperatures down to 70K in low-cost cryocoolers such as the Cryotiger series. 4. 2-stage 4K cryocoolers, 1996, Japan These 4K cryocoolers follow the development of rare earth magnetic alloys with large heat capacities in the 4 10K range. 5. Large-scale gas separation and production 1. Double column air distillation, 1910, Germany One of the first key developments toward the large-scale rectification of liquid air was the double column distillation system of Linde. This simplifying feature was a breakthrough which has been adopted in the majority of air separation plants, and was driven by the growing demand for industrial gases and the invention of oxyacetylene welding in Europe in 1905. 2. Turbine expanders, 1939, Russia The second breakthrough toward low-cost air separation plants came in 1939 with the construction of the first air liquefier with an expansion turbine by Kapitza in Moscow. However, it was not until after WW2 in 1948 that the first industrial air separation plants incorporated turbine expanders. 3. Space rocketry, 1961, USA Although LOX was first used in rockets from 1926 by Goddard and in the German V2 rockets of 1944, the combination of liquid hydrogen and liquid oxygen was first used in the U.S. rocket Atlas Centaur in 1961. This achievement represents the breakthrough in space rocketry which led to the large-scale production of liquid hydrogen and the Saturn series from 1963, the ESA Ariane series from 1975, the NASA Space Shuttles from 1983 and others. 6. Materials 1. Ductile-brittle transformation, 1940s, USA Understanding the nature and dependence on plate thickness of the ductile-brittle transformation at low temperatures in bcc materials (such as carbon steels), and its absence in the fcc materials (such as nickel and copper) came about in the USA in the 1940s. This understanding became the breakthrough for the choice of materials with adequate strength at low temperatures, to meet both impact and slow-loading conditions. Before this breakthrough, structural failures on protoype plants turned away commercial interest in cryogenic systems. 7. Medicine 1. Cryoprotectants, 1946 and 1959, UK The discovery of cryoprotectants, such as glycerol, in 1946, by Polge and Smith, and dimethylsulfoxide (DMSO)

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History of Cryogenics: A Cryo Central resource from the CSA

in 1959 by Lovelock and Bishop, for ensuring the survival of cryopreserved cells and tissues, provided the breakthrough for the development of the cryopreservation of spermatazoa, embryos, ovaries, blood and other tissues, which is taken for granted today. 2. Cryosurgery, 1961, USA, 1967 South Africa The destruction of diseased tissue by slow freezing was able to develop from the breakthroughs in the design of practicable cryoprobes, by Cooper in the USA using liquid nitrogen, in 1961 and by Amoils, in South Africa, using nitrous oxide, in 1967. 3. Magnetic Resonance Imaging , 1983, UK The bringing together in the early 1980s of cryogenics, superconductivity, proton nuclear magnetic resonance and computer processing by Nottingham and Oxford Universities and Oxford Magnet Technology UK, has led to a breakthrough in medical diagnostics. Now the majority of hospitals have at least one MRI system which is in constant use. 8. Instrumentation Two breakthroughs have revolutionized cryogenic instrumentation. 1. Cold electronics, 1980s The discovery at Southampton and elsewhere that CMOS silicon chips with no bipolar elements will operate at low temperatures enables previously unattainable precision levels of measurement (to less than one part in 10,000) to be made routinely in cryogenic systems. 2. SQUIDs, 1967, USA The development of the Superconducting Quantum Interference Detector (SQUID) by Zimmerman and others in 1967 represents a breakthrough in sensitivity for the detection of small electrical, magnetic or electromagnetic signals; for example in the multi-SQUID magneto-encephalograph. 9. Superconductors 1. Stabilization of LT superconductors, 1960s, UK The discovery of Type 2 superconductors in 1961 with exceptional, thin, high magnetic field performance was tainted with frustration when their current-carrying capabilities at liquid helium temperatures turned out to be severely limited by what we now know to be flux jumping, which caused local heating above the transition temperature. The development of stabilized composite conductors with superconducting wires enclosed in a copper matrix by the Rutherford Laboratory group and others in the late 60s provided the breakthrough for the application of LT superconductors. 2. HTS no breakthroughs yet The need for stabilization of high temperature superconductors, HTS, operating at liquid nitrogen temperature is relatively important owing to their very much higher heat capacities. The obstacles to progress with HTS relate to the conflicting demands of processing hard ceramic powder particles inside or outside a relatively soft metal tube whilst in a controlled oxygen atmosphere. A systematic approach towards manufacturing kilometer lengths of HTS composite wire or tape has been established. This is achieving results, enabling power engineering prototypes for transformers, cables and fault current limiters to be tested. The present HTS applications for RF filters (for better mobile phone networks) and current leads (for LHC magnets) represent small markets in comparison with power engineering requirements in the new millennium. This list of breakthroughs is bound to be incomplete in the eyes of many readers if so please add your suggestions to the list, together with their provenance and consequences. I, myself, have concentrated on those enabling technological achievements which have led to significant commercial applications. 2. Ray Szara, former CSA Chairman, President, and Cold Facts columnist (deceased), sent these thoughts: Millennium of progress in cryogenics (not necessarily in the order of importance): Invention of the helium liquefier which could be manufactured commercially (Sam Collins). Discovery of superconductivity by Kamerlingh Onnes (mercury) in about 1908. HTSC MRI SMES (Roger Boom)

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History of Cryogenics: A Cryo Central resource from the CSA

Cryogenic food freezing using liquid nitrogen and cryogenic carbon dioxide. Commercial use of products of air (oxygen, nitrogen, argon). Basic oxygen furnace for steel making. Space flight using liquid hydrogen and liquid oxygen propellants. Cryopreservation of blood and body parts. Deep space communication using cryoelectronics. Superconductivity theory (John Bardeen). Infrared imaging (using cryogenic cooling) 3. Dr. Randall F. Barron , Professor Emeritus, Mechanical Engineering, Louisiana Tech University, sent these thoughts: 1877 Cailletet and Pictet liquefied oxygen. This was really the beginning of cryogenics as an area separate from refrigeration. 1884 Wroblewski (Kracow University, Poland) first liquefied hydrogen as a mist. 1892 Sir James Dewar (England) developed the vacuum-insulated vessel for storage of cryogenic fluids 1895 Heike Kamerlingh Onnes (Holland) established the Leiden Cryogenic Lab, and Karl von Linde (Germany) obtained a basic patent for air liquefaction 1898 James Dewar produced liquid hydrogen in bulk at the Royal Institute of London 1902 Georges Claude developed the first air-liquefaction system using an expansion engine 1908 H.K. Onnes first liquefied heliumthe last of the so-called permanent gases to be liquefied 1911 H.K. Onnes discovered superconductivity 1916 First commercial American-made air liquefaction plant completed 1922 First commercial production of neon in the United States 1926 Robert Goddard conducted the worlds first successful flight of a rocket powered by cryogenic (liquid) oxygen and noncryogenic gasoline propellant 1933 Magnetic cooling used to reach temperatures below 1K 1934 Peter Kapitza built the first expansion engine for a helium liquefier 1939 First vacuum-insulated railway tank car built for transport of liquid oxygen 1947 The Collins cryostat developed for liquefaction of helium 1952 1952 National Bureau of Standards Cryogenic Engineering Laboratory established in Boulder, Colorado 1957 Atlas ICBM powered by LOX/RP-1 was test fired. Fundamental theory (Bardeen-Cooper-Schrieffer or BCS theory) of superconductivity presented 1958 Multilayer insulation (MLI) developed 1961 Saturn launch vehicle, powered by liquid oxygen and liquid hydrogen, was test-fired 1966 He3/He4 dilution refrigerator developed 1969 3250-hp dc superconducting motor constructed for ship drive application 1986 Georg Bednorz and Alex Muller discover high-transition-temperature ceramic superconductor with a Tc of about 30K 1987 Paul Chu (Univ. of Houston) and Maw-Kuen Wu (Univ. of Alabama at Huntsville) develop the 1-2-3 yttrium based highTc superconductor with a Tc of about 90K 4. From John Urbin, Linde Cryogenics: In helium cryogenics, I think the Collins Helium Cryostat, developed in 1946 and commercialized in 1947 by ADL, was an important breakthrough technology. Liquid helium became available to a wide range of researchers leading to developments in many areas of science. 5. Robert E. Bernert, Sr., Thermax, Inc., saw as a significant breakthrough the extruded aluminum ambient vaporizers introduced in 1958, now the workhorse energy-saving cryogenic vaporizing process of choice after nearly 50 years of continuous improvement in both design and application. 6. Mark Haberbusch , Principal Engineer, Sierra Lobo, Inc., mentioned first flight of aircraft using liquid hydrogen, which led to the use of hydrogen on the Centaur and Saturn rockets. 7. Stanislaw Augustynowicz , CSA Director for International Affairs, singled out the development of High Temperature Superconductivity (HTS) that opened the highway to use cryogens and cryogenic equipment for transformers, motors, transport energy cables, etc. 8. Vincent Arp, Cryodata, Inc., singled out the liquefaction of helium, leading to the discovery of superconductivity and superfluidity.

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History of Cryogenics: A Cryo Central resource from the CSA

Most Influential People in Cryogenics in the Past Millennium One individual who deserves to be recognized as one of the greatest contributors to cryogenics in the past millennium is Dr. Abe Silverstein. Under his direct supervision as Chief of Research at the National Advisory Committee for Aeronautics (NACA) Lewis Flight Propulsion Laboratory in Cleveland, the highly energetic and difficult-to-handle liquid hydrogen was harnessed and shown for the first time to be a feasible propellant for aerospace vehicles. The basic research conducted in investigating hydrogen as a potential propellant, combined with the engineering experience gained in conducting the first flight demonstration, formed a solid foundation and experience base that would be invaluable to the country. Armed with this liquid hydrogen experience base, Silverstein led the young and newly formed National Aeronautics and Space Administration (NASA) in the successful development of the workhorse Centaur hydrogen/oxygenpowered upper-stage which demonstrated that hydrogen propulsion technology was mature enough to power the upper stages of the Saturn V rocket that successfully took humans to the moon for the first time. This saga began in the Lewis Laboratory rocket research group in 1945. The research group began by studying potential rocket fuels at a time when rocketry was taboo within NACA. One fuel in particular, hydrogen, intrigued Silverstein, who followed the rocket groups research. He was interested in helping the Air Force increase the range of their aircraft by using hydrogen fuel. The Air Force eventually sponsored a research program called Program Bee at Lewis Labs that would demonstrate liquid hydrogen powered flight. Silverstein personally directed the project and put the project office under his office in the basement of the Administration Building. A B-57B bomber with two Curtiss Wright J-65 engines was modified so that one of the engines could run on either jet fuel or hydrogen. The project culminated in a successful hydrogen-powered flight demonstration over Lake Erie the first time out. Experience was gained for the first time on the storage, pumped transfer and vaporization of liquid hydrogen for use in a flight propulsion system. Silverstein was called to Washington to head the Office of Space Flight for the newly formed NASA. He had full responsibility for the Mercury and unmanned satellite programs. He named the Apollo program and formed the Saturn Evaluation committee whose primary mission was to focus on determining the upper stage configuration that would fly on top of Wernher von Brauns Saturn V booster. Silverstein knew that liquid hydrogen could provide a 40% increase in payload capability over other propellant combinations, and that this extra payload would be needed to accomplish Apollos mission goals. Von Braun, although skeptical about using liquid hydrogen, initially agreed with the committees recommendation to use it. This would change later. Almost simultaneously, von Braun had been working with General Dynamics Krafft Ehricke in developing a liquid hydrogen/oxygen upper-stage called Centaur but was having significant problems in getting it to work. After considerable difficulty von Braun strongly recommended to NASA HQ to cancel the Centaur program because of concerns with the tank design which consisted of pressurestabilized propellant tanks and a common bulkhead separating the hydrogen and the oxygen. NASA HQ asked Silverstein, who had since left NASA HQ in 1961 to become the director of the NASA Lewis Research Center, if he was interested in taking over the Centaur development program and trying to make it work. He eagerly accepted the challenge and led his hand-picked teams in successfully making the Centaur a flying success. The Centaur was coined Abes Baby. The first mission Centaur performed was the successful delivery of the Surveyor moon probe that provided critical data for the planned manned moon landings. The success of Centaur was a proof test that paved the way for using hydrogen on the manned Saturn rocket. Silverstein was later quoted as saying, I believe the decision to go with hydrogen and oxygen in the upper stages of the Saturn V was the significant technical decision that enabled the US to achieve the first manned lunar landing. As with the other legends of cryogenics mentioned in this issue, the ground-breaking technical accomplishment made by Abe Silverstein and his talented staff has touched many lives over the last half of this Century. Tens of thousands of engineers and technicians make a living by continuing to launch hydrogen-powered rockets into space. A significant number of communications and weather satellites that all of us depend on have been put into orbit using hydrogen powered rockets. The space shuttle powered by three liquid hydrogen engines continues to provide the boost into space that inspires others to continually look up towards the final frontier. Abes cryogenic accomplishments are truly out-of-this world. Background information for this article came from a NASA Special Publication in the NASA History Series, Engines and Innovation: Lewis Laboratory and American Propulsion Technology, NASA SP-4306, 1991, written by Virginia Dawson.

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History of Cryogenics: A Cryo Central resource from the CSA

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