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Title: Hierarchical calibration and validation for modeling bench-scale solvent-based carbon capture. Part 1: Non-reactive physical mass transfer across the wetted wall column

A hierarchical model calibration and validation are proposed here for quantifying the confidence level of mass transfer prediction using a computational fluid dynamics (CFD) model, where the solvent-based carbon dioxide (CO 2) capture is simulated and the predicted results are compared to the corresponding bench-scale experimental data. Two unit problems with an increasing level of complexity are proposed to break down the complex physical/chemical processes of solvent-based CO 2 capture into relatively simpler problems to separate the effects of physical transport and chemical reaction. This paper focuses on the calibration and validation of the first unit problem, i.e., the CO 2 mass transfer across a falling ethanolamine (MEA) film in the absence of chemical reaction. This problem is investigated both experimentally and numerically using non-reactive nitrous oxide (N 2O) as a surrogate for CO 2. To capture motion of the gas-liquid interface, a volume of fluid method is employed with a one-fluid formulation to compute the mass transfer between the two phases. Parallel bench-scale experiments are designed and conducted to validate and calibrate the CFD models using a general Bayesian calibration approach. Two important transport parameters, Henry's constant and gas diffusivity, are calibrated to produce the posterior distributions, which willmore » be used as input for the second unit problem to address the chemical absorption of CO 2 across the MEA falling film, where both mass transfer and chemical reaction are involved. Finally, mass transfer coefficients predicted by CFD are also compared with those predicted by the traditional/empirical correlations under both steady and wavy falling film conditions.« less
Authors:
 [1] ;  [1] ;  [1] ;  [2] ;  [3] ;  [1]
  1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Physical and Computational Sciences Directorate
  2. Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Energy and Environment Directorate
  3. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Publication Date:
Report Number(s):
LA-UR-18-21206
Journal ID: ISSN 2152-3878
Grant/Contract Number:
89233218CNA000001; AC05-76RL01830
Type:
Accepted Manuscript
Journal Name:
Greenhouse Gases: Science and Technology
Additional Journal Information:
Journal Volume: 7; Journal Issue: 4; Journal ID: ISSN 2152-3878
Publisher:
Society of Chemical Industry, Wiley
Research Org:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org:
USDOE Office of Fossil Energy (FE)
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES; Bayesian calibration; carbon capture; physical absorption; computational fluid dynamics; hierarchical calibration and validation; wetted wall column
OSTI Identifier:
1482923
Alternate Identifier(s):
OSTI ID: 1374663

Wang, Chao, Xu, Zhijie, Lai, Canhai, Whyatt, Greg, Marcy, Peter, and Sun, Xin. Hierarchical calibration and validation for modeling bench-scale solvent-based carbon capture. Part 1: Non-reactive physical mass transfer across the wetted wall column. United States: N. p., Web. doi:10.1002/ghg.1682.
Wang, Chao, Xu, Zhijie, Lai, Canhai, Whyatt, Greg, Marcy, Peter, & Sun, Xin. Hierarchical calibration and validation for modeling bench-scale solvent-based carbon capture. Part 1: Non-reactive physical mass transfer across the wetted wall column. United States. doi:10.1002/ghg.1682.
Wang, Chao, Xu, Zhijie, Lai, Canhai, Whyatt, Greg, Marcy, Peter, and Sun, Xin. 2017. "Hierarchical calibration and validation for modeling bench-scale solvent-based carbon capture. Part 1: Non-reactive physical mass transfer across the wetted wall column". United States. doi:10.1002/ghg.1682. https://www.osti.gov/servlets/purl/1482923.
@article{osti_1482923,
title = {Hierarchical calibration and validation for modeling bench-scale solvent-based carbon capture. Part 1: Non-reactive physical mass transfer across the wetted wall column},
author = {Wang, Chao and Xu, Zhijie and Lai, Canhai and Whyatt, Greg and Marcy, Peter and Sun, Xin},
abstractNote = {A hierarchical model calibration and validation are proposed here for quantifying the confidence level of mass transfer prediction using a computational fluid dynamics (CFD) model, where the solvent-based carbon dioxide (CO2) capture is simulated and the predicted results are compared to the corresponding bench-scale experimental data. Two unit problems with an increasing level of complexity are proposed to break down the complex physical/chemical processes of solvent-based CO2 capture into relatively simpler problems to separate the effects of physical transport and chemical reaction. This paper focuses on the calibration and validation of the first unit problem, i.e., the CO2 mass transfer across a falling ethanolamine (MEA) film in the absence of chemical reaction. This problem is investigated both experimentally and numerically using non-reactive nitrous oxide (N2O) as a surrogate for CO2. To capture motion of the gas-liquid interface, a volume of fluid method is employed with a one-fluid formulation to compute the mass transfer between the two phases. Parallel bench-scale experiments are designed and conducted to validate and calibrate the CFD models using a general Bayesian calibration approach. Two important transport parameters, Henry's constant and gas diffusivity, are calibrated to produce the posterior distributions, which will be used as input for the second unit problem to address the chemical absorption of CO2 across the MEA falling film, where both mass transfer and chemical reaction are involved. Finally, mass transfer coefficients predicted by CFD are also compared with those predicted by the traditional/empirical correlations under both steady and wavy falling film conditions.},
doi = {10.1002/ghg.1682},
journal = {Greenhouse Gases: Science and Technology},
number = 4,
volume = 7,
place = {United States},
year = {2017},
month = {4}
}

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