Thermodynamic Guiding Principles for Designing Nonstoichiometric Redox Materials for Solar Thermochemical Fuel Production: Ceria, Perovskites, and Beyond

Sha Li, Vincent M. Wheeler, Apurv Kumar, Mahesh B. Venkataraman, Christopher L. Muhich, Yong Hao, Wojciech Lipiński

Research output: Contribution to journalArticlepeer-review

Abstract

Two-step solar thermochemical water splitting is a promising pathway for renewable fuel production due to its potential for high thermal efficiency via full-spectrum sunlight utilization. Such a promise critically relies on simultaneous innovation in the redox materials and the reactor systems. Most prior efforts on material design are focused on improving the fuel yield at lower reduction temperatures. However, developing materials with both high fuel output and efficiency remains a key challenge, requiring a rigorous understanding of the effects of material thermodynamic properties. Herein, a generic thermodynamic framework is described to decipher the material effects by studying both the state-of-the-art and hypothetical materials within a counterflow reactor system. A global efficiency map is presented for redox materials, revealing inevitable tradeoffs among competing factors such as thermal losses, sweep gas and oxidizer demand, solid preheating, and reduction enthalpy. The choice of the most efficient material is closely linked to the system conditions. Ceria-based materials outperform perovskites under most scenarios, and the optimal hypothetical materials tend to favor higher reduction enthalpies and entropies than existing materials. This work offers a valuable material design roadmap to identify solutions toward efficient solar fuel production.

Original languageEnglish (US)
JournalEnergy Technology
DOIs
StateAccepted/In press - 2021

Keywords

  • ceria
  • materials by design
  • perovskites
  • solar fuels
  • thermochemical water splitting
  • thermodynamic efficiency

ASJC Scopus subject areas

  • Energy(all)

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