Vapour-Liquid and Solid-Vapour-Liquid Equilibria of the System (CO2 + H2) at Temperatures Between (218 and 303) K and at Pressures up to 15 MPa - David Vega-Maza at UKCCSRC Biannual Meeting, Cambridge, April 2014

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Published on April 24, 2014

Author: UKCCSRC

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Presentation given by Dr David Vega-Maza from University of Aberdeen on "Vapour-Liquid and Solid-Vapour-Liquid Equilibria of the System (CO2 + H2) at Temperatures Between (218 and 303) K and at Pressures up to 15 MPa" in the Effects of Impurities Technical Session at the UKCCSRC Biannual Meeting - CCS in the Bigger Picture - held in Cambridge on 2-3 April 2014

Vapour-Liquid and Solid-Vapour-Liquid Equilibria of the System (CO2 + H2) at Temperatures Between (218 and 303) K and at Pressures up to 15 MPa David Vega-Maza University of Aberdeen Martin Trusler Niall R McGlashan Imperial College London 1

2  Scope  Impact of Phase behaviour  Apparatus  VLE results  SVLE results  Conclusions

3 Scope  Post-combustion capture.  Oxy-combustion capture  Pre-combustion capture  Natural gas reforming  Coal gasification  Integrated Gasification Combined Cycle  Ca looping  Chemical looping  Adsorption • Physical Absorbents • Membranes • Cryogenic Separation SEPARATION

4 Scope  Pre-combustion CO2 capture offers an attractive route to decarbonising coal-fired electricity production  Low-temperature physical separation of the CO2 may offer significant cost savings compared with traditional amine-based absorption processes  Costain’s Next Generation Capture Technology (NGCT) concept embodies these ideas in a practical process

5 Scope

6 Impact of Phase behaviour  NGCT process modelling requires precise VLE data for CO2-rich synthesis gas at low temperatures and high pressures  Also require SVLE data to determine the lower operating temperature locus to avoid solids formation  VLE of CO2 + H2 + impurities moderately well known but much of the data are old and there are some significant gaps – hence this new study

7 Apparatus  Static apparatus with on-line sampling and GC analysis  Ranges: 193 ≤ T/K ≤ 473 and 0.5 ≤ p/MPa ≤ 20  Absolute calibration with pure gases by means of internal GSV with sample loops under temperature and pressure control  Process safety considered carefully

8 Apparatus  Static apparatus with on-line sampling and GC analysis  Ranges: 193 ≤ T/K ≤ 473 and 0.5 ≤ p/MPa ≤ 20  Absolute calibration with pure gases by means of internal GSV with sample loops under temperature and pressure control  Process safety considered carefully

9 Apparatus

10 Apparatus

11 Apparatus 193 K < T < 473 K p < 20 MPa V = 0.14 dm3

12 VLE results

13 p-x-y diagram on H2 + CO2 system at -55 ⁰C, where x represents the molar composition of H2 in the liquid phase and y represents the molar composition of H2 in the vapour phase. Symbols:  y -this work-;  x –this work-;  Tsang et al. [1] ;  Spano et al. [2] 1. C.Y. Tsang, W.B. Streett. Chem. Eng. Sci. 36 (1981) 993-1000 2. J.O. Spano, C.K. Heck, P.L. Barrick. J. Chem. Eng. Data 13 (2) (1968) 168-171 p-x diagram on H2 + CO2 system at -55 ⁰C, where x represents the molar composition of H2 in the liquid. Symbols:  x –this work-; – – Tsang et al. [1] ; – – Spano et al. [2] 1. C.Y. Tsang, W.B. Streett. Chem. Eng. Sci. 36 (1981) 993-1000 2. J.O. Spano, C.K. Heck, P.L. Barrick. J. Chem. Eng. Data 13 (2) (1968) 168-171 0 40 80 120 160 0 0.2 0.4 0.6 0.8 1 p/bar x or y 0 40 80 120 160 0 0.01 0.02 0.03 0.04 p/bar x VLE results

14 VLE results

15 SVLE results

16 SVLE results  SVLE locus determined from p-T behaviour during cooling ramps  Allowance for sub-cooling prior to freezing  SVLE locus modelled with EoS for pure solid CO2 + GERG-2008 EoS for (CO2 + H2) in the gas phase, evaluated at the experimental temperature and vapour-phase composition

17 Conclusions  VLE and SVLE data measured for (CO2 + H2)  VLE results in good agreement with the available  Elementary modelling completed; GERG-2008 mixture model planned for CO2 with impurities  Further measurement on (CO2 + CO), (CO2 + CH4) and (CO2 + H2 + 100 ppm H2S) Acknowledgement We are pleased to acknowledge financial support for this work provided by Costain Energy & Process and the Energy Technology Institute

VLE and SVLE of the System (CO2 + H2) at Temperatures Between (218 and 303) K and at Pressures up to 15 MPa Thank You David Vega-Maza University of Aberdeen Martin Trusler Niall R McGlashan Imperial College London 18

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