(6ch) Computational-Accelerated Materials Design for Negative Emission Technologies

Meza-Morales, P., Celmson University
Research Interests:

Aiding limit the increase of the global average temperature, the 2015 Paris Agreement proposed the reduction of carbon dioxide (CO2) emissions throughout this century; however, recent studies suggest that even a rapid atmospheric CO2 removal of energy-related sources is insufficient to keep global heating below 2 °C. Most of climate stabilization scenarios suggest that negative emission technologies (NETs) are required to keep global warming well below 2 °C. NETs are cost-effective mitigation techniques to remove and sequester CO2 from the atmosphere [1, 2]. Herein, we propose to develop NETs that sorb CO2 from the atmosphere and chemically convert it into more useful compounds.

Regarding the CO2 removal, adsorption-based technologies may be considered a cost-efficient option compared with the current prototypical technologies, which are based on aqueous KOH (as capture media) and Ca(OH)2 (as recovery media), which are causticand thus cost and complex to regenerate capture media in addition to its maintain [3, 4]. Porous materials such as metal-organic frameworks (MOFs) have been demonstrated as promising CO2 sorbents [5]. MOFs are particularly attractive for applications such as post-combustion cleanup of coal-fired power plants, where the CO2 concentration is large (ranging from 12 to 70 %); however, the low relative concentration for CO2 in the atmosphere (less than 0.04%) makes designing sorbents for CO2 removal from the atmosphere significantly more challenging. To capture atmospheric CO2, sorbent material must be designed to exhibit high selectivity for the CO2. Coordination pillared-layers (CPLs), which are also porous materials, are excellent candidates for this task and have been shown to demonstrate high selectivity for CO2 over N2, O2, and even CH4 [6]. Moreover, their manifold design allows their textural properties (void volume, surface area, and pore volume) to be systematically tuned, which is critical for optimizing gas adsorption performance. However, property-function relationships that describe how the textural properties of CPLs correlate to their CO2 adsorption performance is lacking. Herein, we propose to develop such relationships in silico. Specifically, we propose to identify CPL-like porous materials, where small amounts of these materials are capable of preferentially sorbing low concentrations of CO2. Furthermore, since the CPL pore-network can act as a host or encapsulating medium for ultra-small metal nanoparticles (< 5nm), such nanoparticles when combined with CPLs can act as catalysts to convert captured CO2 into valuable chemicals. Further it has been demonstrated that the pore-networks of CPLs can prevent agglomeration of the metal nanoparticles, which is critical for the catalyst performance and also promotes shape selectivity. Designing CPL-encapsulated catalysts will require systematic evaluation of hundreds to thousands of materials, including discovery of new materials with unique properties. In the last three decades, the computational materials research community has devised solid rational design/engineering strategies enabling atomic-level control of the structure and composition materials, and molecular simulations have played a pivotal role in accelerating the material properties screening. Herein, we propose to develop high throughput screening strategies based on established methods in rational sorbent and catalyst design, and computational tools—such as machine learning—in order to design materials that possess both gas adsorption and heterogeneous catalytic properties. We will leverage our research expertise in molecular simulations, including Quantum Mechanics, Molecular Dynamics, Monte Carlo to design NETs and other materials that can play pivotal roles in solving energy-related challenges.

Postdoctoral Project:

  • Molecular dynamics studies of liquid water/solid catalyst surfaces
  • Development of a Force Field to model CH3OH and H2O dynamics over a Pt (111) catalyst
  • Quantum chemical study of H2O adsorption on NpO2Surfaces

Under supervision of Rachel B. Getman, Chemical and Biomolecular Engineering, College of Engineering Computing and Applied Sciences, Clemson University.

PhD Dissertation:

  • Quantum mechanics calculations of the CO2 interaction on adsorbents based on porous coordination pillared-layers (CPLs)
  • Monte Carlo analysis of the physical adsorption of CO2 on adsorbents based on porous coordination polymers (CPLs)

Other projects:

  • Determination of Stable Intermediates on CO2 Adsorption Onto Metal(Salen) Complexes: Quantum mechanics calculations

Under supervision of Maria C. Curet-Arana, Chemical Engineering Department, University pf Puerto Rico – Mayaguez Campus.

Research experience:

In my academic career path, I started, as undergrad, doing experimental research studying coal pyrolysis and coal pyrolysis waste reutilization. I earned expertise in managing laboratory equipment for synthesize materials such as zeolites, for water hardness removal, and coal-pyrolysis furnace, to improve coal calorific power. And characterization techniques such as, x-ray diffraction, thermogravimetric analysis, and scanning electron microscopic. However, starting my Ph.D. I did a significant turn to computational chemistry simulations. Since then, I have gained literal expertise in simulation techniques applicable to multiple length and time scales, e.g., Density Functional Theory (femto), Møller–Plesset perturbation theory (MP) (femto), grand canonical Monte Carlo (nano), and Molecular Dynamics (nano). I acquired proficiency modelling the CO2 interaction and adsorption with porous material. During my post-doc, I have earned expertness in modelling surface catalytic intermediates under aqueous phases conditions. My vision for my independent research career is to develop new paradigms in CO2 conversion to chemical commodities in catalyst materials based on encapsulating ultra-small metal nanoparticles in CPL-like porous frameworks. All projects I have worked on have been collaborations with experimentalists and other theoretical groups. Moreover, as result of intense training in various supercomputer center (high performance computing facility at university of Puerto rico–Nanobio, Boqueron and kimkelen–the National Energy Research Scientific Computing Center–NERSC–and in clemson university– Palmetto cluster) I have developed proficient skills performing computer modeling.

Teaching Interests:

Along with my research career, I also have teaching experience. I worked for three terms (one semester plus one summer) at the Portland Community College teaching general chemistry courses. During grad school and post-doc, I TAed and guest-lectured undergrad and grad lecture and laboratory course in Chemical Engineering. I have mentored 10+ undergrad and grad students, conducting training/troubleshooting in programs like Gaussian, VASP, RASPA, and LAMMPS. Moreover, as grad student and post-doc I actively participated in CREST and WIPR2EM social educational activities, as well as, REU programs. I am able to teach all of the core classes in the undergraduate chemical engineering curriculum and would excel at teaching courses in the line of reaction kinetics and catalysis, adsorption fundaments in nanostructures, thermodynamics, numerical methods, data visualization, or computer coding, as well as courses oriented to teaching computational molecular simulation methods for study catalysis and adsorption phenomena.


Dasetty, Siva; Meza-Morales Paul J; Getman, Rachel B; Sarupria, Sapna; Simulations of interfacial processes: recent advances in force field development; Current Opinion in Chemical Engineering; 2019, 23, 138-145.

Meza-Morales, Paul J; Gomez-Gualdron, Diego A; Arrieta-Perez, Rodinson R; Hernandez-Maldonado, Arturo J; Snurr, Randall Q. Curet-Arana, Maria C; CO2 adsorption-induced structural changes in coordination polymer ligands elucidated via molecular simulations and experiments; Dalton Transactions; 2016, 45, 17168–17178.

Meza-Morales, Paul; Alberto Santana-Vargas, Curet-Arana, Maria C; DFT Analysis of Coordination Polymer Ligands: Unraveling the Electrostatic Properties and their Effect on CO2 Interaction; Adsorption; 2015, 21, 533-546.

García-Ricard, Omar J; Meza-Morales, Paul; Silva-Martínez, Juan C; Curet-Arana, Maria C; Hogan, John A; Hernández-Maldonado, Arturo J; Carbon dioxide storage and sustained delivery by Cu2(pzdc)2L [L= dipyridyl-based ligand] pillared-layer porous coordination networks; Microporous and Mesoporous Materials, 2013, 177, 54-58.

Curet-Arana, Maria C; Meza-Morales, Paul; Irizarry, Radames; Soler, Rafael; Quantum Chemical Determination of Stable Intermediates on CO2 Adsorption Onto Metal (Salen) Complexes; Topics in Catalysis, 2012, 55, 260-266.


[1]Eisaman, M. D., Rivest, J. L. B., Karnitz, S. D., de Lannoy, C. F., Jose, A., DeVaul, R. W., & Hannun, K. Indirect ocean capture of atmospheric CO2: Part II. Understanding the cost of negative emissions. International Journal of Greenhouse Gas Control, 70, 254–261, 2018.

[2]de Lannoy, C. F., Eisaman, M. D., Jose, A., Karnitz, S. D., DeVaul, R. W., Hannun, K., & Rivest, J. L. B. Indirect ocean capture of atmospheric CO2: Part I. Prototype of a negative emissions technology. International Journal of Greenhouse Gas Control, 70, 243–253, 2018.

[3]Koytsoumpa, E. I., Bergins, C., & Kakaras, E., The CO2 economy: Review of CO2 capture and reuse technologies. Journal of Supercritical Fluids, 132, 3–16, 2018.

[4]Keith, D. W., Holmes, G., St. Angelo, D., & Heidel, K. A., Process for Capturing CO2 from the Atmosphere. Joule, 2, 1573–1594, 2018.

[5]Trickett, C. A., Helal, A., Al-Maythalony, B. A., Yamani, Z. H., Cordova, K. E., & Yaghi, O. M., The chemistry of metal-organic frameworks for CO2capture, regeneration and conversion. Nature Reviews Materials, 2, 17045, 2017.

[6]García­Ricard, Omar J., Silva-Martínez, Juan C., Hernandez-Maldonado, Arturo J., Systematic evaluation of textural properties, activation temperature and gas uptake of Cu2(pzdc)2L [L = dipyridyl-based ligands] porous coordination pillared-layer networks. Dalton Trans., 41, 8922-8930, 2012.