In:
Advanced Functional Materials, Wiley, Vol. 32, No. 43 ( 2022-10)
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 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.
Type of Medium:
Online Resource
ISSN:
1616-301X
,
1616-3028
DOI:
10.1002/adfm.202205654
Language:
English
Publisher:
Wiley
Publication Date:
2022
detail.hit.zdb_id:
2029061-5
detail.hit.zdb_id:
2039420-2
SSG:
11
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