Home
This Title All WIREs
WIREs RSS Feed
How to cite this WIREs title:
WIREs Comput Mol Sci
Impact Factor: 14.016

What can molecular simulation do for global warming?

Full article on Wiley Online Library:   HTML PDF

Can't access this content? Tell your librarian.

Carbon capture is necessary to reduce CO2 emissions from burning fossil fuels, which has led to global warming. Molecular simulations offer chemical insights and design principles for new separation media and for understanding the separation process. In this review, we summarize recent applications of simulation methods from ab initio and density functional theory to classical molecular dynamics and Grand canonical Monte Carlo in understanding ionic liquids and porous carbonaceous materials for CO2 separation, especially the postcombustion CO2/N2 separation. We highlight design and simulation of the porous two‐dimensional (2D) materials as the highly selective membranes for CO2 separation. Simulated structure–property relationships for the materials are discussed in connection to the corresponding chemisorption, physisorption, or membrane process. In chemisorption, the focus is on reducing the heat of reaction with CO2; in physisorption, the key is to increase the binding strength via CO2‐philic groups; in membrane process, the key is to increase solubility for ionic‐liquid membranes and to control pore size for 2D materials. Challenges and opportunities for simulating emerging materials are also discussed. WIREs Comput Mol Sci 2016, 6:173–197. doi: 10.1002/wcms.1241

Monthly average carbon dioxide concentration in the past 50 years measured by Mauna Loa Observatory. Data are from Scripps CO2 program.
[ Normal View | Magnified View ]
(a) Screened expanded porphyrins with large pores. (b) Potential energy curves calculated at BLYP‐D3/def2‐QZVPP level for CO2 and N2 passing through selected porous porphyrins. (Reproduced with permission from Ref . Copyright 2015 American Chemical Society)
[ Normal View | Magnified View ]
(a) Structures of PG‐ES1. (b) Various gas molecules crossings during CMD simulations. (Reproduced with permission from Ref . Copyright 2012 American Chemical Society)
[ Normal View | Magnified View ]
(a) Nanopore on the CNT wall. (b) Initial configuration of CMD simulation, where gas mixture is inside the tube. (c) Snapshot around t = 16 ns; (d) Number of permeate molecules with time. The gas mixture is composed of 80% CO2 and 20% CH4 at initial pressure of 175 atm. (e) Free‐energy profiles of gas passing‐through with the radial distance from the axis of CNT. The gas mixture is composed of 50% CO2 and 50% CH4 at initial pressure of 88 atm. Color code: C, cyan; O, red; H, white; N, blue. (Reproduced with permission from Ref . Copyright 2012 American Chemical Society)
[ Normal View | Magnified View ]
(a) All‐hydrogen‐saturated (8H) and (b) nitrogen‐doped (4N4H) nanopores in a graphene sheet. (Reproduced with permission from Ref . Copyright 2009 American Chemical Society) (c) Schematic of sandwich‐like simulation model and the structure of the nanopore. (Reproduced with permission from Ref . Copyright 2013 Royal Society of Chemistry) (d) Free energy profiles of various gas permeations as a function of the absorption heights. (Reproduced with permission from Ref . Copyright 2015 Elsevier)
[ Normal View | Magnified View ]
(a) Representation of COF composed of tetraphenylsilane and diamino‐tetrahydrofuran. (b) Schematic view of onefold (up) and fivefold (down) interpenetrated framework. (c) Adsorption isotherms of CO2 at 298 K and low pressure in various COFs. (Reproduced with permission from Ref . Copyright 2012 American Chemical Society)
[ Normal View | Magnified View ]
(a) Structures of PAF‐1 and three functionalized frameworks. (b) CO2 adsorption isotherms at 298 K and (a) low or (b) moderate pressure. (Reproduced with permission from Ref . Copyright 2011 American Chemical Society)
[ Normal View | Magnified View ]
(a) Calculated gas‐phase cation–anion interaction versus the experimental CO2 solubility at 1 bar and 298 K for four ionic [emin]‐containing liquids, and (b) correlation between volume expansion and mole fraction of CO2. (Reproduced with permission from Ref . Copyright 2011 American Chemical Society)
[ Normal View | Magnified View ]
Structures of (a) diamond and (b)–(d) various PAFs. (Reproduced with permission from Ref . Copyright 2009 John Wiley & Sons)
[ Normal View | Magnified View ]
(a) Parasitic energy versus the Henry coefficient of CO2 for silica zeolite structures. The green line gives the parasitic energy of the MEA sorbent as a benchmark. (b) Some examples of the potential all‐silica structures. O atoms are in red and Si in tan. Surface with warmer color indicates the dominant CO2 adsorption sites. (Reproduced with permission from Ref . Copyright 2012 Nature Publishing Group)
[ Normal View | Magnified View ]
(a) Simulated permeabilities and Henry's law constants of CO2 in three ionic liquids. (Reproduced with permission from Ref . Copyright 2014 American Chemical Society)
[ Normal View | Magnified View ]
(a) The relative positions of cation and anion in the neat ionic liquid. The approximate directions in which anions displace to accommodate dissolved CO2 is indicated by arrows. (b) The most probable location of CO2 in ionic liquid. (Reproduced with permission from Ref . Copyright 2005 American Chemical Society)
[ Normal View | Magnified View ]
Schematic diagram of gas separation with (a) dense and (b) porous membranes. (Reproduced with permission from Ref . Copyright 2011 American Association for the Advancement of Science)
[ Normal View | Magnified View ]
Binding energies and structures of CO2‐complexes of molecules that have strong physical interaction with CO2. Calculation levels include (a) CCSD(T)/CBS considering BSSE correction and monomer deformation energy, (b) ri‐MP2/def2‐TZVPP, and (c) CCSD(T)/CBS.
[ Normal View | Magnified View ]
Relationships between binding energy and OCO angle in the anionCO2 complexes. (a) Binding energy is derived from optimization in the gas phase; (b) The binding energy is derived from optimization in a solvation model. (Reproduced with permission from Ref . Copyright 2015 John Wiley & Sons)
[ Normal View | Magnified View ]
Distribution functions around an anion (a) before and (b) after CO2 binding. The gray part represents phosphorus atoms and the yellow part represents the centers of mass of the anions. (Reproduced with permission from Ref . Copyright 2014 American Chemical Society).
[ Normal View | Magnified View ]
Examples of hydrogen‐bonding interactions in the studied ionic liquid systems: (a) cation:quaternary ammonium:carbamate species = 0:1:1 and (b) cation:quaternary ammonium:carbamate species = 1:2:2. Color code: C, cyan; N, blue; O, red; H, white. Most hydrogen atoms are omitted for clarity. (Reproduced with permission from Ref . Copyright 2008 American Chemical Society).
[ Normal View | Magnified View ]
Variation of anion–CO2 interaction energy with the calculated atomic charge on anion oxygen atoms. (Reproduced with permission from Ref . Copyright 2010 American Chemical Society)
[ Normal View | Magnified View ]
Reaction enthalpies of several typical anions used in protic ionic liquids. Calculation level is B3LYP/TZVP.
[ Normal View | Magnified View ]
Summary about some representative amine chemistry with CO2. Reaction enthalpies of various reactions were calculated at SCS‐MP2/6‐311+G(2d,2p)//MP2/6‐311G(d,p) level with SMD solvation model.
[ Normal View | Magnified View ]
Linear correlation between rate constants of sorbents and reaction enthalpies. (Reproduced with permission from Ref . Copyright 2012 Nature Publishing Group)
[ Normal View | Magnified View ]

Related Articles

Top Ten WCMS Articles

Browse by Topic

Structure and Mechanism > Computational Materials Science
Electronic Structure Theory > Density Functional Theory

Access to this WIREs title is by subscription only.

Recommend to Your
Librarian Now!

The latest WIREs articles in your inbox

Sign Up for Article Alerts