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Natural gas-based Chemical Looping for Hydrogen Production 
Letitia Petrescu 
Christoph Müller 
Calin-Cristian Cormos Babes-Bolyai University, Faculty of Chemistry and Chemical Engineering, Cluj -Napoca, Romania Laboratory of Energy Science and Engineering, ETH Zurich, Zurich, Switzerland
Advanced thermo-chemical looping cycles for the poly-generation of decarbonised energy vectors: Material synthesis and characterisation, process modelling and life cycle analysis 
Romanian-Swiss Research Programme 
01 January 2013 - 31 December 2015 
The first objective of this project is the development of novel, multi- functional materials for chemical looping The second objective of the project is a critical technical, economical and environmental assessments of the calcium and iron-based chemical looping cycles
CCS-CLC 
Fuel Reactor (30 bar, 700-750˚C): 
4Fe2O3 +3CH4 → 8Fe+3CO2 + 6H2O 
Steam Reactor (28 bar, 700-800˚C): 3Fe + 4H2O → Fe3O4 + 4H2 
Air Reactor (26 bar, 850-1000˚C): 
4Fe3O4 + O2 → 6Fe2O3
Steam reforming of natural gas 
Chemical Looping 
Steam reforming of natural gas combined with Chemical Looping 
Hydrogen production from NG 
Legend: 
Case 1: Hydrogen production from natural gas using SR technology 
Case 2: Hydrogen production based on CL natural gas conversion 
Case 3: Hydrogen production based on SR combined with CL
Methodology for technical and environmental assesment 
Technical Assessment 
Process Simulation 
Environmental 
Assessment 
ChemCAD 
ASPEN PLUS 
GaBi 
KPI
Technical key performance 
indicators
 
Evaluated plant concepts generate 300 MWth of H2. 
 
The carbon capture rate is almost total (99.25%) in Case 2, while for Case 3 it reaches only 68.5%. 
 
The specific CO2 emissions of the evaluated plant concepts with CCS (Case 2 and Case 3) are in the range of 2 - 213 kg/MWh; the case without CCS (Case 1) has specific CO2 emissions of about 268 kg/MWh. 
 
The capability of capturing almost total carbon of the feedstock and lower plant complexity streamlines once more the attractiveness of the direct chemical looping option (Case 2). 
Conclusions on the technical assessment 
Legend: Case 1: Hydrogen production from natural gas using SR technology Case 2: Hydrogen production based on CL natural gas conversion Case 3: Hydrogen production based on SR combined with CL
LCA
LCA 
Legend: Case 1: Hydrogen production from natural gas using SR technology Case 2: Hydrogen production based on CL natural gas conversion Case 3: Hydrogen production based on SR combined with CL
 
A “cradle-to-grave” approach was assumed for the three cases under study. 
 
The LCA assessment was carried out using GaBi 6 software. 
 
Ten environmental impact categories, according to CML 2001 impact assessment method, were defined, calculated and compared. 
 
The best value for GWP is obtained in Case 2, 240.04 kg CO2-Equiv./MW. Other environemntal impcat cathegories such as: ADP, AP, HT increase when CCS – CL tehcnology is applied. 
Conclusions on the environmental assessment
letitiapetrescu@chem.ubbcluj.ro 
muelchri@ethz.ch 
cormos@chem.ubbcluj.ro

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Natural gas-based Chemical Looping for Hydrogen Production

  • 1. Natural gas-based Chemical Looping for Hydrogen Production Letitia Petrescu Christoph Müller Calin-Cristian Cormos Babes-Bolyai University, Faculty of Chemistry and Chemical Engineering, Cluj -Napoca, Romania Laboratory of Energy Science and Engineering, ETH Zurich, Zurich, Switzerland
  • 2. Advanced thermo-chemical looping cycles for the poly-generation of decarbonised energy vectors: Material synthesis and characterisation, process modelling and life cycle analysis Romanian-Swiss Research Programme 01 January 2013 - 31 December 2015 The first objective of this project is the development of novel, multi- functional materials for chemical looping The second objective of the project is a critical technical, economical and environmental assessments of the calcium and iron-based chemical looping cycles
  • 3. CCS-CLC Fuel Reactor (30 bar, 700-750˚C): 4Fe2O3 +3CH4 → 8Fe+3CO2 + 6H2O Steam Reactor (28 bar, 700-800˚C): 3Fe + 4H2O → Fe3O4 + 4H2 Air Reactor (26 bar, 850-1000˚C): 4Fe3O4 + O2 → 6Fe2O3
  • 4. Steam reforming of natural gas Chemical Looping Steam reforming of natural gas combined with Chemical Looping Hydrogen production from NG Legend: Case 1: Hydrogen production from natural gas using SR technology Case 2: Hydrogen production based on CL natural gas conversion Case 3: Hydrogen production based on SR combined with CL
  • 5. Methodology for technical and environmental assesment Technical Assessment Process Simulation Environmental Assessment ChemCAD ASPEN PLUS GaBi KPI
  • 7.  Evaluated plant concepts generate 300 MWth of H2.  The carbon capture rate is almost total (99.25%) in Case 2, while for Case 3 it reaches only 68.5%.  The specific CO2 emissions of the evaluated plant concepts with CCS (Case 2 and Case 3) are in the range of 2 - 213 kg/MWh; the case without CCS (Case 1) has specific CO2 emissions of about 268 kg/MWh.  The capability of capturing almost total carbon of the feedstock and lower plant complexity streamlines once more the attractiveness of the direct chemical looping option (Case 2). Conclusions on the technical assessment Legend: Case 1: Hydrogen production from natural gas using SR technology Case 2: Hydrogen production based on CL natural gas conversion Case 3: Hydrogen production based on SR combined with CL
  • 8. LCA
  • 9. LCA Legend: Case 1: Hydrogen production from natural gas using SR technology Case 2: Hydrogen production based on CL natural gas conversion Case 3: Hydrogen production based on SR combined with CL
  • 10.  A “cradle-to-grave” approach was assumed for the three cases under study.  The LCA assessment was carried out using GaBi 6 software.  Ten environmental impact categories, according to CML 2001 impact assessment method, were defined, calculated and compared.  The best value for GWP is obtained in Case 2, 240.04 kg CO2-Equiv./MW. Other environemntal impcat cathegories such as: ADP, AP, HT increase when CCS – CL tehcnology is applied. Conclusions on the environmental assessment