Separation of gas mixtures by supported complexes. Final report, 1 October 1982-30 September 1984

Technical Report · Tue Jan 01 00:00:00 EST 1985

DOI:https://doi.org/10.2172/6365212· OSTI ID:6365212

Nelson, D A; Hallen, R T; Lilga, M A

This final report covers research performed to identify and demonstrate advantageous procedures for the chemical separation of gases, such as CO, CO/sub 2/, and H/sub 2/, from medium-Btu gas mixtures by use of supported complexes. Three complexes were chosen for rapid gas uptake and selectivity at 25/sup 0/C from among a group of 22 coordination complexes synthesized during this program. The three complexes showed considerable selectivity toward individual gases. For instance, Pd/sub 2/(dpm)/sub 2/Cl/sub 2/ or bis-..mu..-(bisdiphenylphosphinomethane)-dichlorodipalladium (Pd-Pd), rapidly bound carbon monoxide from solution. This complex could be regenerated, with the carbon monoxide reversibly removed, by warming to 40/sup 0/C. The presence of other gases, such as carbon dioxide, oxygen, nitrogen, hydrogen, ethylene, or acetylene, had no effect upon the rapid uptake of carbon monoxide or its removal. Such selectivity was also noted with Ru(CO)/sub 2/(PPh/sub 3/)/sub 3/, biscarbonyltris(triphenylphosphine)ruthenium. Although this complex bound hydrogen, carbon monoxide, and oxygen in solution, the hydrogen was taken up twice as fast as carbon monoxide and seven times faster than oxygen. These gases could be removed from the complex with mild heat or decreased pressure. Crystalline Rh(OH)(CO)(PPh/sub 3/)/sub 2/, hydroxocarbonylbis(triphenylphosphine)rhodium, rapidly bound carbon dioxide; the complex was regenerated at 50/sup 0/C under reduced pressure. The rapid uptake of carbon dioxide by this complex was not changed in the presence of oxygen. In general the three selected crystalline or solvent dissolved complexes performed well in the absence of polymeric support. The stability and favorable kinetics of the three complexes suggest that they could be utilized in a solution system for gas separation (Conceptual Analyses and Preliminary Economics). Further, these complexes appear to be superb candidates as transport agents for facilitated-transport, membrane systems. 69 references, 21 figures.

• Research Organization: Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
• DOE Contract Number: AC06-76RL01830
• OSTI ID: 6365212
• Report Number(s): PNL-4701; ON: DE85006123
• Resource Relation: Other Information: Portions are illegible in microfiche products. Original copy available until stock is exhausted
• Country of Publication: United States
• Language: English

Related Subjects

37 INORGANIC
ORGANIC
PHYSICAL AND ANALYTICAL CHEMISTRY
CARBON DIOXIDE
ADSORPTION
CARBON MONOXIDE
GASES
SEPARATION PROCESSES
HYDROGEN
HYDROGEN SULFIDES
METHANE
PALLADIUM COMPLEXES
CHEMICAL PREPARATION
NUCLEAR MAGNETIC RESONANCE
SORPTIVE PROPERTIES
RHODIUM COMPLEXES
RUTHENIUM COMPLEXES
ADSORPTION HEAT
DESORPTION
EXPERIMENTAL DATA
KINETICS
PRESSURE DEPENDENCE
REGENERATION
SPECIFICITY
TEMPERATURE DEPENDENCE
THERMAL CONDUCTIVITY
ALKANES
CARBON COMPOUNDS
CARBON OXIDES
CHALCOGENIDES
COMPLEXES
DATA
ELEMENTS
ENTHALPY
FLUIDS
HYDROCARBONS
HYDROGEN COMPOUNDS
INFORMATION
MAGNETIC RESONANCE
NONMETALS
NUMERICAL DATA
ORGANIC COMPOUNDS
OXIDES
OXYGEN COMPOUNDS
PHYSICAL PROPERTIES
RESONANCE
SORPTION
SULFIDES
SULFUR COMPOUNDS
SURFACE PROPERTIES
SYNTHESIS
THERMODYNAMIC PROPERTIES
TRANSITION ELEMENT COMPLEXES
400105* - Separation Procedures