Abstract
Zero-global-warming-potential cooling technologies can mitigate the climate change effects attributed to the use of conventional vapour compression refrigeration. In this work, we conceptualize an electrochemical refrigeration cycle and demonstrate a proof-of-concept prototype in continuous operation. The refrigerator is based on the Brayton cycle and draws inspiration from redox flow battery technologies. A peak coefficient of performance of 8.09 was measured with a small temperature drop of 0.07 K. A peak cooling load of 0.934 W with a coefficient of performance of 0.93 was measured, however, with only a modest measured temperature drop of 0.15 K. This is still much lower than the theoretical maximum temperature drop of 2–7 K for these electrolytes. This work could inspire research into high-cooling-capacity redox-active species, multi-fluid heat exchanger design and high-efficiency electrochemical refrigeration cell architectures.
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
Buy this article
- Purchase on Springer Link
- Instant access to full article PDF
Prices may be subject to local taxes which are calculated during checkout
Similar content being viewed by others
Data availability
The data that support the results of this study are provided as Supplementary Data. Source data are provided with this paper.
References
Hansen, J. et al. Global temperature change. Proc. Natl Acad. Sci. USA 103, 14288–14293 (2006).
IPCC Climate Change 2014: Synthesis Report (eds Core Writing Team, Pachauri, R. K. & Meyer, L. A.) (IPCC, 2014).
Ritchie, H. & Roser, M. Urbanization. Our World in Data https://ourworldindata.org/urbanization (2018).
Efficient and Climate-Friendly Cooling (United Nations Environment Programme, 2020); https://wedocs.unep.org/bitstream/handle/20.500.11822/31587/ECFC.pdf?sequence=1&isAllowed=y
The Future of Cooling (International Energy Agency, 2018); https://www.iea.org/futureofcooling/
IPCC. Safeguarding the Ozone Layer and the Global Climate System (eds Metz, B. et al.) (Cambridge Univ. Press, 2005).
Velders, G. J. M., Fahey, D. W., Daniel, J. S., McFarland, M. & Andersen, S. O. The large contribution of projected HFC emissions to future climate forcing. Proc. Natl Acad. Sci. USA 106, 10949–10954 (2009).
Velders, G. J. M. et al. Preserving Montreal Protocol climate benefits by limiting HFCs. Science 335, 922–923 (2012).
Chum, H. & Osteryoung, R. Review of Thermally Regenerative Electrochemical Systems (Solar Energy Research Institute, 1981).
Hammond, R. H. & Risen, W. M. An electrochemical heat engine for direct solar energy conversion. Sol. Energy 23, 443–449 (1979).
Lee, S. W. et al. An electrochemical system for efficiently harvesting low-grade heat energy. Nat. Commun. 5, 3942 (2014).
Poletayev, A. D., McKay, I. S., Chueh, W. C. & Majumdar, A. Continuous electrochemical heat engines. Energy Environ. Sci. 11, 2964–2971 (2018).
Kreysa, G. & Darbyshire, G. F. Theoretical consideration of electrochemical heat pump systems. Electrochim. Acta 35, 1283–1289 (1990).
Dittmar, L., Jüttner, K. & Kreysa, G. in Electrochemical Engineering and Energy (eds Lapicque, F., Storck, A. & Wragg, A. A.) 57–65 (Springer, 1995).
Gerlach, D. W. & Newell, T. A. Basic modelling of direct electrochemical cooling. Int. J. Energy Res. 31, 439–454 (2007).
Newell, Ty. A. Thermodynamic analysis of an electrochemical refrigeration cycle. Int. J. Energy Res. 24, 443–453 (2000).
Duan, Z. N., Qu, Z. G. & Zhang, J. F. Thermodynamic and electrochemical performance analysis for an electrochemical refrigeration system based on iron/vanadium redox couples. Electrochim. Acta 389, 138675 (2021).
McKay, I. S., Kunz, L. Y. & Majumdar, A. Electrochemical redox refrigeration. Sci. Rep. 9, 13945 (2019).
Yang, Y. et al. Charging-free electrochemical system for harvesting low-grade thermal energy. Proc. Natl Acad. Sci. USA 111, 17011–17016 (2014).
Henry, A. A new take on electrochemical heat engines. Joule 2, 1660–1661 (2018).
Rajan, A., McKay, I. S. & Yee, S. K. Electrolyte engineering can improve electrochemical heat engine and refrigeration efficiency. Trends Chem. https://doi.org/10.1016/j.trechm.2021.12.006 (2022).
Fogler, H. Essentials of Chemical Reaction Engineering 2nd edn (Pearson, 2017).
Marcus, R. A. & Sumi, H. Solvent dynamics and vibrational effects in electron transfer reactions. J. Electroanal. Chem. Interfacial Electrochem. 204, 59–67 (1986).
Kim, T. et al. High thermopower of ferri/ferrocyanide redox couple in organic-water solutions. Nano Energy 31, 160–167 (2017).
Zhou, H., Yamada, T. & Kimizuka, N. Supramolecular thermo-electrochemical cells: enhanced thermoelectric performance by host–guest complexation and salt-induced crystallization. J. Am. Chem. Soc. 138, 10502–10507 (2016).
Jacobs, S. et al. The performance of a large-scale rotary magnetic refrigerator. N. Dev. Magn. Refrig. 37, 84–91 (2014).
Energy Savings Potential and RD&D Opportunities for Non-Vapor-Compression HVAC Technologies (US DOE-BTO, 2014); https://doi.org/10.2172/1220817
Whitman, B., Tomczyk, J., Johnson, B. & Silberstein, E. Refrigeration & Air Conditioning Technology (Cengage Learning, 2013).
Engelbrecht, K. et al. Experimental results for a novel rotary active magnetic regenerator. Int. J. Refrig. 35, 1498–1505 (2012).
Atta, R. M. Solar thermoelectric cooling using closed loop heat exchangers with macro channels. Heat Mass Trans. 53, 2241–2254 (2017).
Lima, A. A. S. et al. Absorption refrigeration systems based on ammonia as refrigerant using different absorbents: review and applications. Energies 14, 48 (2021).
Feng, Q. et al. Development of a metal hydride refrigeration system as an exhaust gas-driven automobile air conditioner. Renewable Energy 32, 2034–2052 (2007).
Thermodynamic Properties of DuPont Suva 410A Refrigerant (Chemours, 2019); https://www.freon.com/en/-/media/files/freon/freon-410a-si-thermodynamic-properties.pdf?rev=6b72bfaa299142d697540982b88a56eb
Pecharsky, V. K. & Gschneidner, K. A. Jr Giant magnetocaloric effect in Gd5(Si2Ge2). Phys. Rev. Lett. 78, 4494–4497 (1997).
Worswick, R. D., Dunn, A. G. & Staveley, L. A. K. The enthalpy of solution of ammonia in water and in aqueous solutions of ammonium chloride and ammonium bromide. J. Chem. Thermodyn. 6, 565–570 (1974).
Kim, J. H. et al. Iron (II/III) perchlorate electrolytes for electrochemically harvesting low-grade thermal energy. Sci. Rep. 9, 8706 (2019).
Duan, J. et al. Aqueous thermogalvanic cells with a high Seebeck coefficient for low-grade heat harvest. Nat. Commun. 9, 5146 (2018).
Makarov, D. M. & Egorov, G. I. Density and volumetric properties of the aqueous solutions of urea at temperatures from T=(278 to 333) K and pressures up to 100MPa. J. Chem. Thermodyn. 120, 164–173 (2018).
Acknowledgements
A.R. was partially supported by the Office of Naval Research (award no. N00014-19-1-2162).
Author information
Authors and Affiliations
Contributions
A.R. and S.K.Y. conceptualized the work. A.R. developed the methodology, performed the experiments, analysed the data and wrote the original draught. A.R., I.S.M. and S.K.Y. reviewed and edited the draught. S.K.Y. supervised the research and acquired funding.
Corresponding author
Ethics declarations
Competing interests
A.R. and S.K.Y. are inventors on a US patent (application no. 63/172,925, patent pending) detailing the architecture, chemistry and operation of the BECR. I.S.M. declares no competing interests.
Peer review
Peer review information
Nature Energy thanks Shien-Ping Feng, Neil Mathur, Nini Pryds and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.
Additional information
Publisher’s note Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Supplementary information
Supplementary Information
Supplementary Notes 1 and 2, Figs. 1–17 and Tables 1–4.
Supplementary Data
Supplementary data file for Fig. 16.
Source data
Source Data Fig. 3
Source data for Fig. 3.
Source Data Fig. 4
Source data for Fig. 4.
Rights and permissions
About this article
Cite this article
Rajan, A., McKay, I.S. & Yee, S.K. Continuous electrochemical refrigeration based on the Brayton cycle. Nat Energy 7, 320–328 (2022). https://doi.org/10.1038/s41560-021-00975-7
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1038/s41560-021-00975-7
This article is cited by
-
Cool redox reactions
Nature Energy (2022)