Abstract
Humanity's technological, economic and societal progress since the onset of the industrial revolution has left us facing one of the greatest challenges in history, as well as the tools to solve it: how to power our world sustainably while minimizing environmental harm. In this Perspective, we highlight the important role that quantum chemistry has in sustainable energy research and our vision of its future impact. Important technical problems in the field of sustainable energy and their potential quantum solutions are covered. The development of advanced quantum mechanical methods, which can be combined with other simulation tools, affords insights that will help to secure our energy and environmental future.
This is a preview of subscription content, access via your institution
Access options
Access Nature and 54 other Nature Portfolio journals
Get Nature+, our best-value online-access subscription
$29.99 / 30 days
cancel any time
Subscribe to this journal
Receive 12 digital issues and online access to articles
$119.00 per year
only $9.92 per issue
Rent or buy this article
Prices vary by article type
from$1.95
to$39.95
Prices may be subject to local taxes which are calculated during checkout
Similar content being viewed by others
References
Caine, M. et al. Our high-energy planet — a climate pragmatism project. Breakthrough Institutehttp://thebreakthrough.org/images/pdfs/Our-High-Energy-Planet.pdf (2014).
Carter, E. A. Challenges in modeling materials properties without experimental input. Science 321, 800–803 (2008).
Schrödinger, E. An undulatory theory of the mechanics of atoms and molecules. Phys. Rev. 28, 1049–1070 (1928).
Helgaker, T., Jørgensen, P. & Olsen, J. Molecular Electronic-Structure Theory (Wiley, 2002).
Saebo, S. & Pulay, P. Local treatment of electron correlation. Annu. Rev. Phys. Chem. 44, 213–236 (1993).
Korona, T. et al. in Linear-Scaling Techniques in Computational Chemistry and Physics: Methods and Applications (eds Zalesny, R., Papadopoulos, M. G., Mezey, P. G. & Leszczynski, J. ) 345–407 (Springer Science+Business Media, 2011).
Krisiloff, D. B., Dieterich, J. M., Libisch, F. & Carter, E. A. in Mathematical and Computational Modeling: With Applications in the Natural and Social Sciences, Engineering, and the Arts (ed. Melnick, R. ) 59–91 (Wiley, 2015).
Hohenberg, P. & Kohn, W. Inhomogeneous electron gas. Phys. Rev. 136, B864–B871 (1964).
Kohn, W. & Sham, L. J. Self-consistent equations including exchange and correlation effects. Phys. Rev. 140, A1133–A1138 (1965).
Jensen, F. Describing anions by density functional theory: fractional electron affinity. J. Chem. Theory Comput. 6, 2726–2735 (2010).
Cohen, A. J., Mori-Sanchez, P. & Yang, W. Insights into current limitations of density functional theory. Science 321, 792–794 (2008).
Burke, K. Perspective on density functional theory. J. Chem. Phys. 136, 150901 (2012).
Becke, A. D. Fifty years of density-functional theory in chemical physics. J. Chem. Phys. 140, 18A301 (2014).
Iikura, H., Tsuneda, T., Yanai, T. & Hirao, K. A long-range correction scheme for generalized-gradient-approximation exchange functionals. J. Chem. Phys. 115, 3540–3544 (2001).
Onida, G., Reining, L. & Rubio, A. Electronic excitations: density-functional versus many-body Green's-function approaches. Rev. Mod. Phys. 74, 601–659 (2002).
Lee, K., Murray, E. D., Kong, L., Lundqvist, B. I. & Langreth, D. C. Higher-accuracy van der Waals density functional. Phys. Rev. B 82, 081101 (2010).
Grimme, S. Density functional theory with London dispersion corrections. WIREs Comput. Mol. Sci. 1, 211–228 (2011).
Becke, A. D. Density-functional thermochemistry. III. The role of exact exchange. J. Chem. Phys. 98, 5648–5652 (1993).
Heyd, J., Scuseria, G. E. & Ernzerhof, M. Hybrid functional based on a screened Coulomb potential. J. Chem. Phys. 118, 8207–8215 (2003).
Anisimov, V. I., Zaanen, J. & Andersen, O. K. Band theory and Mott insulators: Hubbard U instead of Stoner I. Phys. Rev. B 44, 943–954 (1991).
Medvedev, M. G., Bushmarinov, I. S., Sun, J., Perdew, J. P. & Lyssenki, K. A. Density functional theory is straying from the path toward the exact functional. Science 355, 49–52 (2017).
Jones, R. O. Density functional theory: its origins, rise to prominence, and future. Rev. Mod. Phys. 87, 897–924 (2015).
Lejaeghere, K. et al. Reproducibility in density functional theory calculations of solids. Science 351, 1415 (2016).
Jacquemin, D., Perpete, E. A., Scuseria, G. E., Ciofini, I. & Adamo, C. Extensive TD-DFT investigation of the first electronic transition in substituted azobenzenes. Chem. Phys. Lett. 465, 226–229 (2008).
Brothers, E. N., Izmaylov, A. F., Normand, J. O., Barone, V. & Scuseria, G. E. Accurate solid-state band gaps via screened hybrid electronic structure calculations. J. Chem. Phys. 129, 011102 (2008).
Neese, F. Prediction of molecular properties and molecular spectroscopy with density functional theory: from fundamental theory to exchange-coupling. Coord. Chem. Rev. 253, 526–563 (2009).
Aarons, J., Sarwar, M., Thompsett, D. & Skylaris, C.-K. Perspective: methods for large-scale density functional calculations on metallic systems. J. Chem. Phys. 145, 220901 (2016).
Wang, Y. A. & Carter, E. A. in Theoretical Methods in Condensed Phase Chemistry Vol. 5 (ed. Schwartz, S. D. ) 117–184 (Springer, 2002).
Hung, L. & Carter, E. A. Accurate simulations of metals at the mesoscale: explicit treatment of 1 million atoms with quantum mechanics. Chem. Phys. Lett. 475, 163–170 (2009).
Chen, M. et al. Introducing PROFESS 3.0: an advanced program for orbital-free density functional theory molecular dynamics simulations. Comp. Phys. Comm. 190, 228–230 (2015).
Chen, M., Jiang, X., Zhuang, H., Wang, L. & Carter, E. A. Petascale orbital-free density functional theory enabled by small-box algorithms. J. Chem. Theory Comput. 12, 2950–2963 (2016).
Wang, Y. A., Govind, N. & Carter, E. A. Orbital-free kinetic energy density functionals with a density-dependent kernel. Phys. Rev. B 60, 16350 (1999).
Wang, Y. A., Govind, N. & Carter, E. A. Erratum: orbital-free kinetic-energy density functionals with a density-dependent kernel [Phys. Rev. B 60 16350 (1999)]. Phys. Rev. B 64, 089903 (2001).
Huang, C. & Carter, E. A. Nonlocal orbital-free kinetic energy density functional for semiconductors. Phys. Rev. B 81, 045206 (2010).
Xia, J. & Carter, E. A. Density-decomposed orbital-free density functional theory for covalently bonded molecules and materials. Phys. Rev. B 86, 235109 (2012).
García-Aldea, D. & Alvarellos, J. E. in Theoretical and Computational Developments in Modern Density Functional Theory (ed. Roy, A. K. ) 255–280 (Nova Science, 2012).
Wesolowski, T. A. & Wang, Y. A. (eds) Recent Progress in Orbital-free Density Functional Theory (World Scientific, 2013).
Shin, I. & Carter, E. A. Enhanced von Weizsäcker Wang–Govind–Carter kinetic energy density functional for semiconductors. J. Chem. Phys 104, 18A531 (2014).
Ke, Y., Libisch, F., Xia, J., Wang, L.-W. & Carter, E. A. Angular momentum dependent orbital free density functional theory. Phys. Rev. Lett. 111, 066402 (2013).
Ke, Y., Libisch, F., Xia, J. & Carter, E. A. Angular momentum dependent orbital free density functional theory: formulation and implementation. Phys. Rev. B 89, 155112 (2014).
Stewart, J. J. P. Optimization of parameters for semiempirical methods. I. Method. J. Comput. Chem. 10, 209–220 (1989).
Wahiduzzaman, M. et al. DFTB Parameters for the periodic table: part 1, electronic structure. J. Chem. Theory Comput. 9, 4006–4017 (2013).
Thiel, W. Semiempirical quantum-chemical methods. WIREs Comput. Mol. Sci. 4, 145–157 (2013).
Stewart, J. J. P. Application of localized molecular orbitals to the solution of semiempirical self-consistent field equations. Int. J. Quantum Chem. 58, 133–146 (1996).
Gordon, M. S., Fedorov, D. G., Pruitt, S. R. & Slipchenko, L. V. Fragmentation methods: a route to accurate calculations on large systems. Chem. Rev. 112, 632–672 (2012).
Libisch, F., Huang, C. & Carter, E. A. Embedded correlated wavefunction schemes: theory and applications. Acc. Chem. Res. 47, 2768–2775 (2014).
Senn, H. M. & Thiel, W. QM/MM methods for biomolecular systems. Angew. Chem. Int. Ed. 48, 1198–1229 (2009).
Wales, D. J. Energy Landscapes: Applications to Clusters, Biomolecules and Glasses (Cambridge Univ. Press, 2004).
Sutto, L., Marsili, S. & Gervasio, F. L. New advances in metadynamics. WIREs Comput. Mol. Sci. 2, 771–779 (2012).
Oyeyemi, V. B., Dieterich, J. M., Krisiloff, D. B., Tan, T. & Carter, E. A. Bond dissociation energies of C10 and C18 methyl esters from local multireference averaged-coupled pair functional theory. J. Phys. Chem. A 119, 3429–3439 (2015).
Frequently Asked Questions: What Is U.S. Electricity Generation by Energy Source?. EIA https://www.eia.gov/tools/faqs/faq.cfm?id=427&t3 (US Energy Information Administration, 2016).
Fusion Energy via Magnetic Confinement. http://acee.princeton.edu/distillates/fusion-energy-via-magnetic-confinement/ (Andlinger Center for Energy and the Environment, 2016).
Johnson, D. F. & Carter, E. A. Hydrogen in tungsten: absorption, diffusion, vacancy trapping, and decohesion. J. Mater. Res. 25, 315–327 (2010).
Christofilos, N. C. Design for a high power-density Astron reactor. J. Fusion Energy 8, 97–105 (1989).
Abdou, M. A. et al. On the exploration of innovative concepts for fusion chamber technology. Fusion Eng. Des. 54, 181–247 (2001).
Majeski, R. et al. Performance projections for the lithium tokamak experiment (LTX). Nucl. Fusion 49, 055014 (2009).
Chen, M., Abrams, T., Jaworski, M. & Carter, E. A. Rock-salt structure lithium deuteride formation in liquid lithium with high-concentrations of deuterium: a first-principles molecular dynamics study. Nucl. Fusion 56, 016020 (2016).
Abrams, T. et al. Suppressed gross erosion of high-temperature lithium via rapid deuterium implantation. Nucl. Fusion 56, 016022 (2016).
Biswas, K. et al. High-performance bulk thermoelectrics with all-scale hierarchical architectures. Nature 489, 414–418 (2012).
Liu, G., Larson, E. D., Williams, R. H. & Guo, X. Gasoline from coal and/or biomass with CO2 capture and storage. 1. Process designs and performance analysis. Energy Fuels 29, 1830–1844 (2015).
Liu, G., Larson, E. D., Williams, R. H. & Guo, X. Gasoline from coal and/or biomass with CO2 capture and storage. 2. Economic analysis and strategic context. Energy Fuels 29, 1845–1859 (2015).
Barton, E., Rampulla, D. M. & Bocarsly, A. B. Selective solar-driven reduction of CO2 to methanol using a catalyzed p-GaP based photoelectrochemical cell. J. Am. Chem. Soc. 130, 6342–6344 (2008).
Verlage, E. et al. A monolithically integrated, intrinsically safe, 10% efficient, solar-driven water-splitting system based on active, stable Earth-abundant electrocatalysts in conjunction with tandem III–V light absorbers protected by amorphous TiO2 films. Energy Environ. Sci. 8, 3166–3172 (2015).
Agrafiotis, C., Roeb, M. & Sattler, C. A review on solar thermal syngas production via redox pair-based water/carbon dioxide splitting thermochemical cycles. Renewable Sustainable Energy Rev. 42, 254–285 (2015).
Felsmann, D. et al. Contributions to improving small ester combustion chemistry: theory, model and experiments. Proc. Comb. Inst. 36, 543–551 (2017).
Hoeinghaus-Kohse, K. et al. Biofuel combustion chemistry: from ethanol to biodiesel. Angew. Chem. Int. Ed. 49, 3572–3597 (2010).
D'Allessandro, D. M., Smit, B. & Long, J. R. Carbon dioxide capture: prospects for new materials. Angew. Chem. Int. Ed. 49, 6058–6082 (2010).
Liao, P. & Carter, E. A. New concepts and modeling strategies to design and evaluate photo-electro-catalysts based on transition metal oxides. Chem. Soc. Rev. 42, 2401–2422 (2013).
Chen, M., Hung, L., Huang, C., Xia, J. & Carter, E. A. The melting point of lithium: an orbital-free first-principles molecular dynamics study. Mol. Phys. 111, 3448–3456 (2013).
Chen, M. et al. Liquid Li structure and dynamics: a comparison between OFDFT and second nearest-neighbor embedded-atom method. AlChE J. 6, 2841–2853 (2015).
Chen, M. et al. Effect of temperature on the desorption of lithium from molybdenum (110) surfaces: implications for fusion reactor first wall materials. J. Phys. Chem. B 120, 6110–6119 (2016).
Shu, H. et al. Amorphous TiO2 coatings stabilize Si, GaAs, and GaP photoanodes for efficient water oxidation. Science 344, 1005–1009 (2014).
Alidoust, N., Toroker, M. C. & Carter, E. A. Revisiting photoemission and inverse photoemission spectra of nickel oxide from first principles: implications for solar energy conversion. J. Phys. Chem. B 118, 7963–7971 (2014).
Alidoust, N., Toroker, M. C., Keith, J. A. & Carter, E. A. Significant reduction in nickel(ii) oxide band gap upon alloying with lithium oxide: applications to solar energy conversion. ChemSusChem 7, 195–201 (2014).
Alidoust, N. & Carter, E. A. First-principles assessment of hole transport in pure and Li-doped NiO. Phys. Chem. Chem. Phys. 17, 18098–18110 (2015).
Alidoust, N. & Carter, E. A. Three-dimensional hole transport in nickel oxide by alloying with MgO or ZnO. J. Appl. Phys. 118, 185102 (2015).
Lessio, M., Senftle, T. P. & Carter, E. A. Is the surface playing a role during pyridine-catalyzed CO2 reduction on p-GaP photoelectrodes? ACS Energy Lett. 1, 464–468 (2016).
Calle-Vallejo, F. & Koper, M. T. M. First-principles computational electrochemistry: achievements and challenges. Electrochim. Acta 84, 3–11 (2012).
Lessio, M., Riplinger, C. & Carter, E. A. Stability of surface protons in pyridine-catalyzed CO2 reduction at p-GaP photoelectrodes. Phys. Chem. Chem. Phys. 18, 26434–26443 (2016).
Chen, M. S. & Goodman, D. W. The structure of catalytically active gold on titania. Science 306, 252–255 (2004).
Fujitani, T., Nakamura, I., Akita, T., Okamura, M. & Haruta, M. Hydrogen dissociation by gold clusters. Angew. Chem. Int. Ed. 48, 9515–9518 (2009).
Brongersma, M. L., Halas, N. J. & Nordlander, P. Plasmon-induced hot carrier science and technology. Nat. Nanotechnol. 10, 25–34 (2015).
Linic, S., Aslam, U., Boerigter, C. & Morabito, M. Photochemical transformations on plasmonic metal nanoparticles. Nat. Mater. 14, 567–576 (2015).
DeSantis, C. J., McClain, M. J. & Halas, N. J. Walking the walk: a giant step toward sustainable plasmonics. ACS Nano 10, 9772–9775 (2016).
Mukherjee, S. et al. Hot electrons do the impossible: plasmon-induced dissociation of H2 on Au. Nano Lett. 13, 240–247 (2013).
Zhuo, L. et al. Aluminium nanocrystal as a plasmonic photocatalyst for hydrogen dissociation. Nano Lett. 16, 1478–1484 (2016).
Oyeyemi, V. B., Keith, J. A. & Carter, E. A. Accurate bond energies of biodiesel methyl esters from multireference averaged coupled-pair functional calculations. J. Phys. Chem. A 118, 7392 (2014).
Tan, T., Yang, X., Krauter, C. M., Ju, Y. & Carter, E. A. Ab initio kinetics of hydrogen abstraction from methyl acetate by hydrogen, methyl, oxygen, hydroxyl and hydroperoxy radicals. J. Phys. Chem. A 119, 6377–6390 (2015).
Tan, T., Yang, X., Ju, Y. & Carter, E. A. Ab initio unimolecular reaction kinetics of CH2C(=O)OCH3 and CH3C(=O)OCH2 radicals. J. Phys. Chem. A 119, 10553–10562 (2015).
Tan, T., Yang, X., Ju, Y. & Carter, E. A. Ab initio pressure-dependent reaction kinetics of methyl propanoate radicals. Phys. Chem. Chem. Phys. 17, 31061– 31072 (2015).
Tan, T., Yang, X., Yu, Y. & Carter, E. A. Ab initio reaction kinetics of CH3OC(=O) and CH2OC(=O)H radicals. J. Phys. Chem. B 120, 1590–1600 (2016).
Tan, T., Yang, X., Yu, Y. & Carter, E. A. Ab initio kinetics studies of hydrogen atom abstraction from methyl propanoate. Phys. Chem. Chem. Phys. 18, 4594–4607 (2016).
Acknowledgements
The authors thank N. Baughman for assistance with the manuscript and G. Turk, W. C. Witt and E. Dieterich for reviews. E.A.C. thanks the US Air Force Office of Scientific Research, the US National Science Foundation, the US Office of Naval Research, the US Army Research Office, and the US Department of Energy, Basic Energy Sciences and Fusion Energy Sciences, for their support of her sustainable energy and quantum mechanics research programmes over many years.
Author information
Authors and Affiliations
Corresponding author
Ethics declarations
Competing interests
The authors declare no competing interests.
PowerPoint slides
Glossary
- Complexity scaling
-
The time that a given algorithm takes to produce a solution as a function of input data size (N). Marked as O(Nx), where O is order, x = 1 denotes linear complexity scaling, x = 2 is quadratic and so on.
- Excited states
-
All allowed energy states of a quantum mechanical system that are not the ground state.
- Quasi-linear
-
Complexity scaling of O(N log(N)) difficulty, where O is order and N is some measure of system size (for example, number of electrons, number of atoms or number of orbitals).
Rights and permissions
About this article
Cite this article
Dieterich, J., Carter, E. Opinion: Quantum solutions for a sustainable energy future. Nat Rev Chem 1, 0032 (2017). https://doi.org/10.1038/s41570-017-0032
Published:
DOI: https://doi.org/10.1038/s41570-017-0032
This article is cited by
-
Optimizing biodiesel production from waste with computational chemistry, machine learning and policy insights: a review
Environmental Chemistry Letters (2024)
-
Analysis of the single reference coupled cluster method for electronic structure calculations: the full-coupled cluster equations
Numerische Mathematik (2023)