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Carbon-Shielded Single-Atom Alloy Material Family for Multi-Functional Electrocatalysis

Journal Article


Abstract


  • Encapsulating metal-based catalysts inside carbon sheaths is a frequently-adopted strategy to enhance their durability under various harsh situations and improve their catalytic activity simultaneously. Such carbon encapsulation, however, imposes significant complications for directly modifying materials’ surface atomic/electronic configurations, fundamentally impeding the accurate tuning of their catalytic capabilities. Herein, a universal single-atom alloy (SAA) strategy is reported to indirectly yet precisely manipulate the surface electronic structure of carbon-encapsulated electrocatalysts. By versatilely constructing a SAA core inside an N-doped carbon sheath, material's electrocatalytic capability can be flexibly tuned. The one with Ru-SAA cores serves as an excellent bifunctional electrocatalyst for oxygen/hydrogen evolution, exhibiting minimal cell voltage of 1.55 V (10 mA cm−2) and outstanding mass activity of 1251 mA m (Formula presented.) for overall water splitting, while the one with Ir-SAA cores possesses superior oxygen reduction activity with a half-wave potential of 919 mV. Density functional theory calculations reveal that the doped atoms can simultaneously optimize the adsorption of protons (H*) and oxygenated intermediates (OH*, O*, and OOH*) to achieve the remarkable thermoneutral hydrogen evolution and enhanced oxygen evolution. This work thus demonstrates a versatile strategy to precisely modify the surface electronic properties of carbon-shielded materials for optimized performances.

UOW Authors


  •   Dou, Shi
  •   Liang, Ji (external author)

Publication Date


  • 2022

Citation


  • Tong, Y., Liu, J., Wang, L., Su, B. J., Wu, K. H., Juang, J. Y., . . . Liang, J. (2022). Carbon-Shielded Single-Atom Alloy Material Family for Multi-Functional Electrocatalysis. Advanced Functional Materials. doi:10.1002/adfm.202205654

Scopus Eid


  • 2-s2.0-85135829555

Abstract


  • Encapsulating metal-based catalysts inside carbon sheaths is a frequently-adopted strategy to enhance their durability under various harsh situations and improve their catalytic activity simultaneously. Such carbon encapsulation, however, imposes significant complications for directly modifying materials’ surface atomic/electronic configurations, fundamentally impeding the accurate tuning of their catalytic capabilities. Herein, a universal single-atom alloy (SAA) strategy is reported to indirectly yet precisely manipulate the surface electronic structure of carbon-encapsulated electrocatalysts. By versatilely constructing a SAA core inside an N-doped carbon sheath, material's electrocatalytic capability can be flexibly tuned. The one with Ru-SAA cores serves as an excellent bifunctional electrocatalyst for oxygen/hydrogen evolution, exhibiting minimal cell voltage of 1.55 V (10 mA cm−2) and outstanding mass activity of 1251 mA m (Formula presented.) for overall water splitting, while the one with Ir-SAA cores possesses superior oxygen reduction activity with a half-wave potential of 919 mV. Density functional theory calculations reveal that the doped atoms can simultaneously optimize the adsorption of protons (H*) and oxygenated intermediates (OH*, O*, and OOH*) to achieve the remarkable thermoneutral hydrogen evolution and enhanced oxygen evolution. This work thus demonstrates a versatile strategy to precisely modify the surface electronic properties of carbon-shielded materials for optimized performances.

UOW Authors


  •   Dou, Shi
  •   Liang, Ji (external author)

Publication Date


  • 2022

Citation


  • Tong, Y., Liu, J., Wang, L., Su, B. J., Wu, K. H., Juang, J. Y., . . . Liang, J. (2022). Carbon-Shielded Single-Atom Alloy Material Family for Multi-Functional Electrocatalysis. Advanced Functional Materials. doi:10.1002/adfm.202205654

Scopus Eid


  • 2-s2.0-85135829555