Solvent Dynamics Are Critical to Understanding Carbon Dioxide Dissolution and Hydration in Water

Martirez, John Mark P.; Carter, Emily A.

doi:10.1021/jacs.3c01283

Title: Solvent Dynamics Are Critical to Understanding Carbon Dioxide Dissolution and Hydration in Water

Journal Article · Mon Jun 05 00:00:00 EDT 2023 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.3c01283· OSTI ID:1992106

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Univ. of California, Los Angeles, CA (United States); Princeton Plasma Physics Laboratory (PPPL), Princeton, NJ (United States)
Univ. of California, Los Angeles, CA (United States); Princeton Plasma Physics Laboratory (PPPL), Princeton, NJ (United States); Princeton Univ., NJ (United States)

Simulations of carbon dioxide (CO₂) in water may aid in understanding the impact of its accumulation in aquatic environments and help advance technologies for carbon capture and utilization (via, e.g., mineralization). Quantum mechanical (QM) simulations based on static molecular models with polarizable continuum solvation poorly reproduce the energetics of CO₂ hydration to form carbonic acid in water, independent of the level of QM theory employed. Only with density-functional-theory-based molecular dynamics and rare-event sampling, followed by energy corrections based on embedded correlated wavefunction theory (in conjunction with density functional embedding theory), can a close agreement between theory and experiment be achieved. Such multilevel simulations can serve as benchmarks for simpler, less costly models, giving insight into potential errors of the latter. The strong influence of sampling/averaging over dynamical solvent configurations on the energetics stems from the difference in polarity of both the transition state and product (both polar) versus the reactant (nonpolar). When a solute undergoes a change in polarity during reaction, affecting its interaction with the solvent, careful assessment of the energetic contribution of the solvent response to this change is critical. Here, we show that static models (without structural sampling) that incorporate three explicit water molecules can yield far superior results than models with more explicit water molecules because fewer water molecules yield less configurational artifacts. Static models intelligently incorporating both explicit (molecules directly participating in the reaction) and implicit solvation, along with a proper QM theory, e.g., CCSD(T) for closed-shell systems, can close the accuracy gap between static and dynamic models.

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Research Organization:: Princeton Plasma Physics Laboratory (PPPL), Princeton, NJ (United States)

Sponsoring Organization:: USDOE Laboratory Directed Research and Development (LDRD) Program

Grant/Contract Number:: AC02-09CH11466

OSTI ID:: 1992106

Journal Information:: Journal of the American Chemical Society, Vol. 145, Issue 23; ISSN 0002-7863

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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