Kinetics and Selectivity of the Fischer–Tropsch Synthesis: A Literature Review

A critical review of the kinetics and selectivity of the Fischer–Tropsch synthesis (FTS) is given. The focus is on reaction mechanisms and kinetics of the water–gas shift and Fischer–Tropsch (FT) reactions. New developments in the product selectivity as well as the overall kinetics are reviewed. It is concluded that the development of rate equations for the FTS should be based on realistic mechanistic schemes. Qualitatively, there is agreement that the product distribution is affected by the occurrence of secondary reactions (hydrogenation, isomerization, reinsertion, and hydrogenolysis). At high CO and H2O pressures, the most important secondary reaction is readsorption of olefins, resulting in initiation of chain growth processes. Secondary hydrogenation of α-olefins may occur and depends on the catalytic system and the process conditions. The rates of the secondary reactions increase exponentially with chain length. Much controversy exists about whether these chain-length dependencies stem from differe...

[1]  A. Kiennemann,et al.  Study on a cobalt silica catalyst during reduction and Fischer–Tropsch reaction: In situ EXAFS compared to XPS and XRD , 1998 .

[2]  B. Davis Fischer-Tropsch conversion of gas to liquid , 1997 .

[3]  G. Beitel,et al.  A COMBINED IN-SITU PM-RAIRS AND KINETIC STUDY OF SINGLE-CRYSTAL COBALT CATALYSTS UNDER SYNTHESIS GAS AT PRESSURES UP TO 300 MBAR , 1997 .

[4]  C. Bianchi,et al.  Experimental evidence of α-Olefin readsorption in Fischer-Tropsch synthesis on ruthenium-supported ETS-10 titanium silicate catalysts , 1997 .

[5]  Gabor A. Somorjai,et al.  Reproducibility of Turnover Rates in Heterogeneous Metal Catalysis: Compilation of Data and Guidelines for Data Analysis , 1997 .

[6]  R. Everson,et al.  Cobalt as an alternative Fischer-Tropsch catalyst to iron for the production of middle distillates , 1997 .

[7]  Fischer-tropsch synthesis on cobalt catalysts: Structural requirements and reaction pathways , 1997 .

[8]  Gilbert F. Froment,et al.  A Steady-State Kinetic Model for Methanol Synthesis and the Water Gas Shift Reaction on a Commercial Cu/ZnO/Al2O3 Catalyst , 1996 .

[9]  Snehal A. Patel,et al.  Activation studies with an iron fischer‐tropsch catalyst in fixed bed and stirred tank slurry reactors , 1996 .

[10]  B. Davis,et al.  Mössbauer Study of Iron Fischer−Tropsch Catalysts during Activation and Synthesis , 1996 .

[11]  Adesoji A. Adesina,et al.  Hydrocarbon synthesis via Fischer-Tropsch reaction: travails and triumphs , 1996 .

[12]  M. Dry,et al.  Practical and theoretical aspects of the catalytic Fischer-Tropsch process , 1996 .

[13]  Ib Chorkendorff,et al.  A Microkinetic Analysis of the Water–Gas Shift Reaction under Industrial Conditions , 1996 .

[14]  J. H. Wilson,et al.  Non-ASF product distributions due to secondary reactions during Fischer-Tropsch synthesis , 1996 .

[15]  R. O'brien,et al.  Mössbauer spectroscopy study of iron-based catalysts used in Fischer-Tropsch synthesis , 1995 .

[16]  R. A. Santen,et al.  Concepts in Theoretical Heterogeneous Catalytic Reactivity , 1995 .

[17]  Abhaya K. Datye,et al.  Activation of Precipitated Iron Fischer-Tropsch Synthesis Catalysts , 1995 .

[18]  D. Bukur,et al.  Activation studies with a precipitated iron catalyst for Fischer-Tropsch synthesis. I. Characterization studies , 1995 .

[19]  Lech Nowicki,et al.  Activation studies with a precipitated iron catalyst for Fischer-Tropsch synthesis. II. Reaction studies , 1995 .

[20]  B. B. Breman,et al.  Kinetics of the gas-slurry methanol-higher alcohol synthesis from CO/CO2/H2 over a CsCu/ZnO/Al2O3 catalyst, including simultaneous formation of methyl esters and hydrocarbons , 1995 .

[21]  Gerald P. Huffman,et al.  Pretreatment effect studies with a precipitated iron Fischer-Tropsch catalyst , 1995 .

[22]  R. Nieminen,et al.  Monte Carlo study of CO hydrogenation on cobalt model catalysts , 1995 .

[23]  John L. Falconer,et al.  Spillover in Heterogeneous Catalysis , 1995 .

[24]  S. C. Saxena,et al.  Bubble column reactors and Fischer-Tropsch synthesis , 1995 .

[25]  H. Schulz,et al.  Specific inhibition as the kinetic principle of the Fischer-Tropsch synthesis , 1995 .

[26]  H. Oosterbeek,et al.  Chain Length Dependence of α-Olefin Readsorption in Fischer-Tropsch Synthesis , 1995 .

[27]  A. Kiennemann,et al.  Higher alcohol and paraffin synthesis on cobalt based catalysts: Comparison of mechanistic aspects , 1995 .

[28]  Motoyuki Suzuki,et al.  Solvent effect on adsorption phenomena in reversed‐phase liquid chromatography , 1995 .

[29]  Motoyuki Suzuki,et al.  Chromatographic study on liquid‐phase adsorption on octadecylsilyl‐Silica Gel , 1995 .

[30]  B. Jager,et al.  Advances in low temperature Fischer-Tropsch synthesis , 1995 .

[31]  J. G. Goodwin,et al.  In-Situ XAFS Investigation of K-Promoted Co Catalysts , 1995 .

[32]  R. O'brien,et al.  Effect of pre-heat treatment on a Fischer-Tropsch iron catalyst , 1994 .

[33]  Frank E. Huggins,et al.  The role of magnetite in Fischer-Tropsch synthesis , 1994 .

[34]  D. Bukur,et al.  Mössbauer study of CO-precipitated Fischer-Tropsch iron catalysts , 1994 .

[35]  Enrique Iglesia,et al.  Hydrogen and CO Intrapellet Diffusion Effects in Ruthenium-Catalyzed Hydrocarbon Synthesis , 1994 .

[36]  B. B. Breman,et al.  GAS-LIQUID SOLUBILITIES OF CARBON-MONOXIDE, CARBON-DIOXIDE, HYDROGEN, WATER, 1-ALCOHOLS (1-LESS-THAN-OR-EQUAL-TO-N-LESS-THAN-OR-EQUAL-TO-6), AND N-PARAFFINS (2-LESS-THAN-OR-EQUAL-TO-N-LESS-THAN-OR-EQUAL-TO-6) IN HEXADECANE, OCTACOSANE, 1-HEXADECANOL, PHENANTHRENE, AND TETRAETHYLENE GLYCOL AT PRESSUR , 1994 .

[37]  Alexis T. Bell,et al.  Estimates of rate coefficients for elementary processes occurring during Fischer-Tropsch synthesis over RuTiO2 , 1994 .

[38]  G. Kliger,et al.  The molecular weight distribution of the products of the Fischer-Tropsch synthesis , 1994 .

[39]  J. Nicholas,et al.  Molecular modeling of the enthalpies of adsorption of hydrocarbons on smectite clay , 1994 .

[40]  U. Landman,et al.  Molecular Dynamics of Adsorption and Segregation from an Alkane Mixture , 1993, Science.

[41]  J. Fox,et al.  The Different Catalytic Routes for Methane Valorization: An Assessment of Processes for Liquid Fuels , 1993 .

[42]  B. B. Breman,et al.  On-line single column capillary gas chromatographic analysis of all reactants and products in the synthesis of fuel methanol from hydrogen and oxides of carbon , 1993 .

[43]  E. Iglesia,et al.  The Importance of Olefin Readsorption and H2/CO Reactant Ratio for Hydrocarbon Chain Growth on Ruthenium Catalysts , 1993 .

[44]  A. Kiennemann,et al.  Mechanistic Aspects of the Formation of Hydrocarbons and Alcohols from CO Hydrogenation , 1993 .

[45]  R. E. Pauls,et al.  Telomerization Model for Cobalt-Catalyzed Fischer-Tropsch Products , 1993 .

[46]  Enrique Iglesia,et al.  Selectivity Control and Catalyst Design in the Fischer-Tropsch Synthesis: Sites, Pellets, and Reactors , 1993 .

[47]  A. Bell,et al.  Estimates of the Rate Coefficients for Chain Initiation, Propagation, and Termination during Fischer-Tropsch Synthesis over Ru/TiO2 , 1993 .

[48]  Gilbert F. Froment,et al.  Kinetics of the Fischer-Tropsch reaction on a precipitated promoted iron catalyst. 2. Kinetic modeling , 1993 .

[49]  Gilbert F. Froment,et al.  Kinetics of the Fischer-Tropsch reaction on a precipitated promoted iron catalyst. 1. Experimental procedure and results , 1993 .

[50]  E. Iglesia,et al.  Fischer-Tropsch synthesis on cobalt and ruthenium. Metal dispersion and support effects on reaction rate and selectivity , 1992 .

[51]  S. Ledakowicz,et al.  Kinetic model of fischer-tropsch synthesis selectivity in the slurry phase , 1992 .

[52]  Gary J. Stiegel,et al.  Iron-based catalysts for slurry-phase Fischer-Tropsch process : technology review , 1992 .

[53]  S. Reyes,et al.  Primary and secondary reaction pathways in ruthenium-catalyzed hydrocarbon synthesis , 1991 .

[54]  M. Vannice,et al.  Carbon-supported iron catalysts: influence of support porosity and preparation techniques on crystallite size and catalytic behavior , 1991 .

[55]  Ian C. Yates,et al.  The hydrocarbon selectivity of cobalt Fischer-Tropsch catalysts , 1991 .

[56]  S. Reyes,et al.  Transport-enhanced α-olefin readsorption pathways in Ru-catalyzed hydrocarbon synthesis , 1991 .

[57]  S. T. Sie,et al.  Conversion of natural gas to transportation fuels via the shell middle distillate synthesis process (SMDS) , 1991 .

[58]  C. Satterfield,et al.  Intrinsic kinetics of the Fischer-Tropsch synthesis on a cobalt catalyst , 1991 .

[59]  J. W. Mitchell,et al.  Slurry-phase Fischer-Tropsch synthesis and kinetic studies over supported cobalt carbonyl derived catalysts , 1990 .

[60]  J. W. Bramblett,et al.  Gas—solid chromatography and virial analysis of hydrocarbon adsorption on 13X zeolite , 1990 .

[61]  Snehal A. Patel,et al.  Fixed bed and slurry reactor studies of Fischer-Tropsch synthesis on precipitated iron catalyst , 1990 .

[62]  C. Erkey,et al.  Diffusivities of synthesis gas and n-alkanes in Fischer-Tropsch wax , 1990 .

[63]  Dragomir B. Bukur,et al.  Reaction kinetics over iron catalysts used for the fischer‐tropsch synthesis , 1990 .

[64]  E. Shustorovich Metal effects in the Fischer-Tropsch synthesis: Bond-order-conservation-morse-potential approach , 1990 .

[65]  B. Davis,et al.  Fischer-Tropsch synthesis: carbon-14 tracer study of alkene incorporation , 1990 .

[66]  J. H. Gregor Fischer-Tropsch products as liquid fuels or chemicals , 1990 .

[67]  D. Bukur,et al.  Activation studies with a promoted precipitated iron Fischer-Tropsch catalyst , 1989 .

[68]  B. Wojciechowski,et al.  Studies of the fischer‐tropsch synthesis on a colbalt catalyst. III. mechanistic formulation of the kinetics of selectivity for higher hydrocarbon formation , 1989 .

[69]  S. T. Sie,et al.  Diffusion limitations in fischer‐tropsch catalysts , 1989 .

[70]  R. Snel Supported iron catalysis in Fischer8.9çTropsch synthesis: influence of the preparation method , 1989 .

[71]  S. Wise,et al.  Synthesis and characterization of novel bonded phases for reversed-phase liquid chromatography , 1989 .

[72]  D. Bukur,et al.  Effect of particle size on the activity of a fused iron Fischer-Tropsch catalyst , 1989 .

[73]  Bohdan W. Wojciechowski,et al.  Studies of the fischer-tropsch synthesis on a cobalt catalyst II. Kinetics of carbon monoxide conversion to methane and to higher hydrocarbons , 1989 .

[74]  J. Hackett,et al.  Capillary gas chromatographic characterization of Fischer-Tropsch liquefaction products: on-line-analysis , 1989 .

[75]  G. Froment,et al.  Methane steam reforming, methanation and water‐gas shift: I. Intrinsic kinetics , 1989 .

[76]  C. Satterfield,et al.  Product distributions of the Fischer-Tropsch synthesis on precipitated iron catalysts , 1989 .

[77]  C. Satterfield,et al.  Effect of carbon dioxide on the kinetics of the Fischer-Tropsch synthesis on iron catalysts , 1989 .

[78]  Bohdan W. Wojciechowski,et al.  The Kinetics of the Fischer-Tropsch Synthesis , 1988 .

[79]  B. Sarup,et al.  Studies of the fischer‐tropsch synthesis on a cobalt catalyst i. evaluation of product distribution parameters from experimental data , 1988 .

[80]  G. Marin,et al.  Characterization of a promoted precipitated iron catalyst for Fischer-Tropsch synthesis , 1988 .

[81]  Hans Schulz,et al.  Kinetics of Fischer-Tropsch selectivity , 1988 .

[82]  G. Froment,et al.  A versatile bench-scale unit for kinetic studies of catalytic reactions , 1988 .

[83]  Ian C. Yates,et al.  Analysis and prediction of product distributions of the Fischer-Tropsch synthesis , 1988 .

[84]  Eize Stamhuis,et al.  Kinetics of the three phase methanol synthesis , 1988 .

[85]  K. Cavell,et al.  Role of Supports for Cobalt-Based Catalysts Used in Fischer-Tropsch Synthesis of Hydrocarbons , 1988 .

[86]  A. Bell,et al.  The influence of butene on CO hydrogenation over ruthenium , 1987 .

[87]  C. Satterfield,et al.  Reactions of selected 1-olefins and ethanol added during the Fischer-Tropsch synthesis: Topical report , 1987 .

[88]  A. Bell,et al.  The influence of propylene on CO hydrogenation over silica-supported ruthenium , 1987 .

[89]  Aydin Akgerman,et al.  High-temperature diffusion of hydrogen, carbon monoxide, and carbon dioxide in liquid n-heptane, n-dodecane, and n-hexadecane , 1987 .

[90]  T. Inui,et al.  Simple criteria to differentiate a two-site model from a distributed-site model for Fischer-Tropsch synthesis , 1987 .

[91]  B. Wojciechowski,et al.  On interpreting FT product distribution data , 1987 .

[92]  J. Dumesic,et al.  Adsorptive and catalytic properties of supported metal oxides: III. Water-gas shift over supported iron and zinc oxides , 1986 .

[93]  G. Papaefthymiou,et al.  Effect of water on the iron-catalyzed Fischer-Tropsch synthesis , 1986 .

[94]  A. Bell,et al.  INFLUENCE OF ETHYLENE ON THE HYDROGENATION OF CO OVER RUTHENIUM , 1986 .

[95]  W. Deckwer,et al.  Kinetic studies of Fischer-Tropsch synthesis on suspended iron/potassium catalyst - rate inhibition by carbon dioxide and water , 1986 .

[96]  R. Snel On-line gas chromatographic analysis of light Fischer-Tropsch synthesis products , 1986 .

[97]  P. Biloen,et al.  A transient kinetic observation of chain growth in the Fischer-Tropsch synthesis , 1986 .

[98]  M. Rosen,et al.  MATHEMATICAL MODELING OF FISCHER- TROPSCH SLURRY BUBBLE COLUMN REACTORS , 1986 .

[99]  D. S. Vuuren,et al.  On the formation and composition of the liquid phase in Fischer-Tropsch reactors , 1986 .

[100]  Alexis T. Bell,et al.  Fischer-Tropsch synthesis over reduced and unreduced iron oxide catalysts , 1986 .

[101]  S. Chuang,et al.  The Use of Probe Molecules in the Study of CO Hydrogenation over SiO2‐Supported Ni, Ru, Rh, and Pd , 1985 .

[102]  C. Satterfield,et al.  Liquid accumulation in catalyst pores in a Fischer-Tropsch fixed-bed reactor , 1985 .

[103]  Nosa O. Egiebor,et al.  Carbon number distribution of fischer — Tropsch CO‐hydrogenation products from precipitated iron catalysts , 1985 .

[104]  G. Schrader,et al.  Characterization of a fused iron catalyst for Fischer-Tropsch synthesis by in situ laser Raman spectroscopy , 1985 .

[105]  M. Donohue,et al.  Henry's constants for C5 to C9 hydrocarbons in C10 and larger hydrocarbons , 1985 .

[106]  Effect of liquid composition on the slurry Fischer-Tropsch synthesis. 1. Rate of reaction , 1985 .

[107]  Charles N. Satterfield,et al.  Intrinsic kinetics of the Fischer-Tropsch synthesis on a reduced fused-magnetite catalyst , 1984 .

[108]  C. Satterfield,et al.  Some kinetic design considerations in the Fischer-Tropsch synthesis on a reduced fused-magnetite catalyst , 1984 .

[109]  A. Bell,et al.  On-line analysis of Fischer-Tropsch synthesis products , 1984 .

[110]  C. Takoudis POWER RATE LAW STUDIES IN HETEROGENEOUSLY CATALYZED REACTIONS. , 1984 .

[111]  R. Herman Catalytic Conversions of Synthesis Gas and Alcohols to Chemicals , 1984 .

[112]  N. L. Carr,et al.  Mass transfer coefficients and solubilities for hydrogen and carbon monoxide under Fischer-Tropsch conditions , 1984 .

[113]  D. Bianchi,et al.  Nature of surface species on supported iron during CO/H2 reaction , 1983 .

[114]  A. Bell,et al.  An explanation for deviations of Fischer-Tropsch products from a Schulz-Flory distribution , 1983 .

[115]  W. Sachtler,et al.  On the activity of Fischer-Tropsch and methanation catalysts: A study utilizing isotopic transients , 1983 .

[116]  C. Satterfield,et al.  Stirred autoclave apparatus for study of the Fischer-Tropsch synthesis in a slurry bed. 2. Analytical procedures , 1983 .

[117]  M. Röper,et al.  Fischer-Tropsch Synthesis , 1983 .

[118]  L. Tavlarides,et al.  Kinetics of the Fischer-Tropsch synthesis , 1983 .

[119]  J. Gaube,et al.  Fischer-Tropsch-Synthese. Neuere Untersuchungen und Entwicklungen , 1983 .

[120]  C. Satterfield,et al.  Stirred autoclave apparatus for study of the Fischer-Tropsch synthesis in a slurry bed. 1. Reactor and trapping procedures , 1982 .

[121]  M. Dry Catalytic aspects of industrial Fischer-Tropsch synthesis , 1982 .

[122]  C. Frohning,et al.  The raw materials future: critical examination of the roled played by catalysis , 1982 .

[123]  H. Suhl,et al.  Secondary effects in the Fischer-Tropsch synthesis , 1982 .

[124]  C. Satterfield,et al.  Usefulness of a slurry/type fischer‐tropsch reactor for processing synthesis gas of low hydrogen‐carbon monoxide ratios , 1982 .

[125]  W. Sachtler Mechanismus der katalysierten Synthese von Kohlenwasserstoffen , 1982 .

[126]  M. Vannice Catalytic Activation of Carbon Monoxide on Metal Surfaces , 1982 .

[127]  P. L. Silveston,et al.  Steady-state study of the Fischer-Tropsch reaction , 1981 .

[128]  C. K. Rofer-depoorter A comprehensive mechanism for the Fischer-Tropsch synthesis , 1981 .

[129]  Alexis T. Bell,et al.  The kinetics and mechanism of carbon monoxide hydrogenation over alumina-supported ruthenium , 1981 .

[130]  H. Suhl,et al.  Models of hydrocarbon product distributions in Fischer–Tropsch synthesis. I , 1981 .

[131]  D. Ollis,et al.  The chemistry and catalysis of the water gas shift reaction: 1. The kinetics over supported metal catalysts , 1981 .

[132]  P. Jacobs,et al.  On-Line Single Run Analysis of Effluents from a Fischer-Tropsch Reactor , 1981 .

[133]  J. C. Hoogendoorn,et al.  Technology of the Fischer-Tropsch Process , 1981 .

[134]  P. Biloen,et al.  Mechanism of Hydrocarbon Synthesis over Fischer-Tropsch Catalysts , 1982 .

[135]  Alexis T. Bell,et al.  Catalytic Synthesis of Hydrocarbons over Group VIII Metals. A Discussion of the Reaction Mechanism , 1981 .

[136]  J. Niemantsverdriet,et al.  Behavior of metallic iron catalysts during Fischer-Tropsch synthesis studied with Mössbauer spectroscopy, X-ray diffraction, carbon content determination, and reaction kinetic measurements , 1980 .

[137]  D. Newsome The Water-Gas Shift Reaction , 1980 .

[138]  Manfred Baerns,et al.  Prediction of the performance of catalytic fixed bed reactors for Fischer-Tropsch Synthesis , 1980 .

[139]  H. Kölbel,et al.  The Fischer-Tropsch Synthesis in the Liquid Phase , 1980 .

[140]  J. Stein,et al.  Mechanistic features of catalytic carbon monoxide hydrogenation reactions , 1979 .

[141]  V. Ponec,et al.  The Role of Chemisorption of Fischer-Tropsch Synthesis , 1979 .

[142]  G. Raupp,et al.  Mössbauer investigation of supported Fe catalysts: III. In situ kinetics and spectroscopy during Fischer-Tropsch synthesis , 1979 .

[143]  W. Sachtler,et al.  Incorporation of surface carbon into hydrocarbons during Fischer-Tropsch synthesis: Mechanistic implications , 1979 .

[144]  D. Dwyer THE ROLE OF READSORPTION IN DETERMINING THE PRODUCT DISTRIBUTION DURING CO HYDROGENATION OVER Fe SINGLE CRYSTALS , 1979 .

[145]  C. Bennett,et al.  Kinetics of the Fischer-Tropsch Reaction over Iron , 1979 .

[146]  R. Everson,et al.  Fischer-Tropsch reaction studies with supported ruthenium catalysts: I. Product distributions at moderate pressures and catalyst deactivation , 1978 .

[147]  J. Butt,et al.  Carburization of supported iron synthesis catalysts , 1978 .

[148]  G. Tegge Falbe, J. (Herausgeb.): Chemierohstoffe aus Kohle. Georg Thieme Verlag, Stuttgart 1977. 446 Seiten, mit 213 Abb. und 166 Tab., gebunden DM 228,–. , 1978 .

[149]  V. Ponec Some Aspects of the Mechanism of Methanation and Fischer-Tropsch Synthesis , 1978 .

[150]  M. Vannice,et al.  The catalytic synthesis of hydrocarbons from H2CO mixtures over the Group VIII metals: V. The catalytic behavior of silica-supported metals , 1977 .

[151]  M. Dry Advances in Fishcher-Tropsch Chemistry , 1976 .

[152]  M. Vannice CATALYTIC SYNTHESIS OF HYDROCARBONS FROM CARBON MONOXIDE AND HYDROGEN , 1976 .

[153]  M. Vannice,et al.  The catalytic synthesis of hydrocarbons from H2CO mixtures over the group VIII metals: II. The kinetics of the methanation reaction over supported metals , 1975 .

[154]  J. Prausnitz,et al.  Solubilities of gases in high‐boiling hydrocarbon solvents , 1974 .

[155]  A. G. Piken,et al.  Heterogeneous methanation: initial rate of CO hydrogenation on supported ruthenium and nickel , 1974 .

[156]  Reiji Mezaki,et al.  Mechanistic structure of the water-gas shift reaction in the vicinity of chemical equilibrium , 1973 .

[157]  S. Oki,et al.  Identification of rate-controlling steps for the water-gas shift reaction over an iron oxide catalyst , 1973 .

[158]  M. Boudart Two‐step catalytic reactions , 1972 .

[159]  M. Dry,et al.  Rate of the Fischer-Tropsch reaction over iron catalysts , 1972 .

[160]  H. Pichler,et al.  Neuere Erkenntnisse auf dem Gebiet der Synthese von Kohlenwasserstoffen aus CO und H2 , 1970 .

[161]  M. Dry,et al.  Heats of chemisorption on promoted iron surfaces and the role of alkali in Fischer-Tropsch synthesis , 1969 .

[162]  C. Eckert MOLECULAR THERMODYNAMICS OF CHEMICAL REACTIONS , 1967 .

[163]  G. Bond Catalysis By Metals , 1962 .

[164]  P. Emmett,et al.  Mechanism Studies of the Fischer-Tropsch Synthesis: The Incorporation of Radioactive Ethylene, Propionaldehyde and Propanol , 1960 .