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Developing Proton-Conductive Metal Coordination Polymer as Highly Efficient Electrocatalyst toward Oxygen Reduction.

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Earth-abundant transition metal electrocatalysts offer a cost-effective alternative for fuel cells. Iron (Fe) and cobalt (Co) based coordination polymers show promise as durable oxygen reduction reaction (ORR) catalysts.

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Catalysis

Background:

  • Developing cost-effective electrocatalysts for the oxygen reduction reaction (ORR) is crucial for advancing fuel cell technology.
  • Platinum-based catalysts are highly effective but prohibitively expensive for widespread adoption.

Purpose of the Study:

  • To investigate the ORR performance of earth-abundant transition metal (TM)-based coordination polymers (TM-DHBQs).
  • To identify promising TM-DHBQs as alternatives to platinum for ORR catalysis.

Main Methods:

  • Synthesized proton-conductive coordination polymers (TM-DHBQs) using transition metals (3d, 4d, 5d).
  • Screened TM-DHBQs for ORR performance.
  • Utilized formation energy and adsorption free energy calculations.
  • Employed Sabatier-type volcano plots and microkinetic modeling.

Main Results:

  • Most 3d TM-DHBQs demonstrated excellent durability under ORR conditions.
  • Formation energy of TM-DHBQs correlated well with TM ion's outer electrons, serving as an ORR activity descriptor.
  • Fe- and Co-DHBQs were identified as promising alternatives to platinum catalysts.
  • Active sites involve TM ions strongly bonding with ORR intermediates.

Conclusions:

  • Earth-abundant TM-DHBQs, particularly Fe- and Co-based ones, are viable alternatives to platinum for ORR catalysis.
  • Formation energy is a reliable descriptor for predicting ORR activity in these materials.
  • Understanding intermediate binding is key to designing efficient electrocatalysts.