TY - JOUR
T1 - Divide-and-conquer density-functional tight-binding molecular dynamics study on the formation of carbamate ions during CO2 chemical absorption in aqueous amine solution
AU - Sakti, Aditya Wibawa
AU - Nishimura, Yoshifumi
AU - Sato, Hiroshi
AU - Nakai, Hiromi
PY - 2017/1/1
Y1 - 2017/1/1
N2 - Divide-and-conquer-type density-functional tight-binding molecular dynamics simulations of the CO2 absorption process in monoethanolamine (MEA) solution have been performed for systems containing thousands of atoms. The formation of carbamate anions has been widely investigated for neutral systems via ab initio molecular dynamics simulations, yet the present study is aimed at identifying the role of hydroxide ions in acidbase equilibrium. The structural and electronic analyses reveal that the hydroxide ion approaches, via Grotthuss-type shuttling, the zwitterionic intermediates and abstracts a proton from the nitrogen atom of MEA. We also estimated the fraction of reacted CO2 and carbamate formed at different initial CO2 concentrations that confirm a high absorbed CO2 concentration decreases the fraction of MEA(C) formed due to the abundance of MEA(Z) in the solution.
AB - Divide-and-conquer-type density-functional tight-binding molecular dynamics simulations of the CO2 absorption process in monoethanolamine (MEA) solution have been performed for systems containing thousands of atoms. The formation of carbamate anions has been widely investigated for neutral systems via ab initio molecular dynamics simulations, yet the present study is aimed at identifying the role of hydroxide ions in acidbase equilibrium. The structural and electronic analyses reveal that the hydroxide ion approaches, via Grotthuss-type shuttling, the zwitterionic intermediates and abstracts a proton from the nitrogen atom of MEA. We also estimated the fraction of reacted CO2 and carbamate formed at different initial CO2 concentrations that confirm a high absorbed CO2 concentration decreases the fraction of MEA(C) formed due to the abundance of MEA(Z) in the solution.
UR - http://www.scopus.com/inward/record.url?scp=85034594447&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=85034594447&partnerID=8YFLogxK
U2 - 10.1246/bcsj.20170142
DO - 10.1246/bcsj.20170142
M3 - Article
AN - SCOPUS:85034594447
VL - 90
SP - 1230
EP - 1235
JO - Bulletin of the Chemical Society of Japan
JF - Bulletin of the Chemical Society of Japan
SN - 0009-2673
IS - 11
ER -