Journal
ADVANCED MATERIALS
Volume 34, Issue 15, Pages -Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.202110128
Keywords
chemical order; high-entropy alloy nanoparticles; L1; (2) phase; nitrogen-rich mesoporous carbon; oxygen reduction reaction
Categories
Funding
- NSF of China [51822202, 52173233]
- Innovation Program of Shanghai Municipal Education Commission [2021-01-07-00-03-E00109]
- Science and Technology Commission of Shanghai Municipality [19520713200]
- Shuguang Program - Shanghai Education Development Foundation
- Shanghai Municipal Education Commission [20SG33]
- Shanghai Scientific and Technological Innovation Project [19JC1410400]
- DHU Distinguished Young Professor Program
- Fundamental Research Funds for the Central Universities [2232020D-02]
- Opening Project of Key Laboratory of Inorganic Functional Materials and Devices [KLIFMD202104]
- Shanghai Sailing Program [20YF1400500]
- Shanghai Natural Science Foundation [20ZR1401500]
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Structurally ordered high-entropy alloy nanoparticles (OHEA-mNC NPs) with excellent catalytic performance have been successfully constructed on a novel 2D nitrogen-rich mesoporous carbon sandwich framework using ligand-assisted interfacial assembly and NH3 annealing.
Recent efforts have observed nanoscaled chemical short-range order in bulk high-entropy alloys (HEAs). Simultaneously inspired with the nanostructuring technology, HEA nanoparticles (NPs) with complete chemical order may be achieved. Herein, structurally ordered HEA (OHEA) NPs are constructed on a novel 2D nitrogen-rich mesoporous carbon sandwich framework (OHEA-mNC) by combining a ligand-assisted interfacial assembly with NH3 annealing. Characterization results show that the resultant materials possess an ultrathin 2D nanosheet structure with large mesopores (approximate to 10 nm), where structurally ordered HEA NPs with an L1(2) phase are homogeneously dispersed. The atom-resolved chemical analyses explicitly determine the location of each atomic site. When being evaluated for the oxygen reduction reaction, the OHEA-mNC NPs afford a greatly enhanced catalytic performance, including a large half-wave potential (0.90 eV) and a high durability (0.01 V decay after 10 000 cycles) compared with the disordered HEA and commercial Pt/C catalysts. The excellent performance is attributed to the enhanced mass transfer rate, improved electron conductivity, and the presence of the stable chemically ordered HEA phase, as revealed by both the experimental results and theoretical calculation. This study suggests a highly feasible process to achieve structurally ordered HEA NPs with advanced mesoporous function in the electrochemical field.
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