Single-atom
catalysts (SACs) have emerged as one of the most promising
alternatives to noble metal-based catalysts for highly efficient oxygen
reduction reaction (ORR). While SACs can offer notable benefits in
terms of lowering overall catalyst cost, there is still room for improvement
regarding catalyst activity. To this end, we designed and successfully
fabricated an ORR electrocatalyst in which atomic clusters are embedded
in an atomically dispersed Fe–N–C matrix (FeAC@FeSA–N–C), as shown by comprehensive measurements
using aberration-corrected scanning transmission electron microscopy
(AC-STEM) and X-ray absorption spectroscopy (XAS). The half-wave potential
of FeAC@FeSA–N–C is 0.912 V (versus
reversible hydrogen electrode (RHE)), exceeding that of commercial
Pt/C (0.897 V), FeSA–N–C (0.844 V), as well
as the half-wave potentials of most reported non-platinum-group metal
catalysts. The ORR activity of the designed catalyst stems from single-atom
active centers but is markedly enhanced by the presence of Fe nanoclusters,
as confirmed by both experimental measurements and theoretical calculations.
One of the key challenges that hinders broad commercialization of proton exchange membrane fuel cells is the high cost and inadequate performance of the catalysts for oxygen reduction reaction (ORR)....
Reversible protonic ceramic electrochemical cells (R-PCECs) are a promising option for efficient and low-cost generation of electricity and hydrogen. Commercialization of R-PCECs, however, hinges on the development of highly active and robust air electrodes. Here, we report an air electrode consisting of PrBa 0.8 Ca 0.2 Co 2 O 5+δ and in situ exsolved BaCoO 3−δ nanoparticles (PBCC−BCO) that shows minimal polarization resistance (∼0.24 Ω cm 2 at 600 °C) and high stability when exposed to humidified air with 3−50% H 2 O. An R-PCEC utilizing PBCC-BCO demonstrates remarkable performances at 600 °C: achieving a peak power density of 1.06 W cm −2 in the fuel cell mode and a current density of 1.51 A cm −2 at 1.3 V in an electrolysis mode. More importantly, the R-PCECs demonstrate an exceptionally high durability over 1833 h of continuous operation in the electrolysis mode. This work offers an efficient approach to design of high-performance and durable electrodes for R-PCECs.
Reversible solid oxide cells based on ceramic proton conductors have potential to be the most efficient system for large‐scale energy storage. The performance and long‐term durability of these systems, however, are often limited by the ionic conductivity or stability of the proton‐conducting electrolyte. Here new family of solid oxide electrolytes, BaHfxCe0.8−xY0.1Yb0.1O3−δ (BHCYYb), which demonstrate a superior ionic conductivity to stability trade‐off than the state‐of‐the‐art proton conductors, BaZrxCe0.8−xY0.1Yb0.1O3−δ (BZCYYb), at similar Zr/Hf concentrations, as confirmed by thermogravimetric analysis, Raman, and X‐ray diffraction analysis of samples over 500 h of testing are reported. The increase in performance is revealed through thermodynamic arguments and first‐principle calculations. In addition, lab scale full cells are fabricated, demonstrating high peak power densities of 1.1, 1.4, and 1.6 W cm−2 at 600, 650, and 700 °C, respectively. Round‐trip efficiencies for steam electrolysis at 1 A cm−2 are 78%, 72%, and 62% at 700, 650, and 600 °C, respectively. Finally, CO2H2O electrolysis is carried out for over 700 h with no degradation.
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