Journal
NANO ENERGY
Volume 78, Issue -, Pages -Publisher
ELSEVIER
DOI: 10.1016/j.nanoen.2020.105211
Keywords
Alloy cluster; Heteropolyacid; Molecule template; Nitrogen reduction reaction; Operando X-ray absorption spectroscopy
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Funding
- National Natural Science Foundation of China [21673014, 21975010, 51731002]
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Alloy clusters are attractive electrocatalysts that have adjustable activity through the synergistic effects of alloy components. However, the synthesis of atomically-precise alloy clusters is still a challenge. Here, we report a molecular template method in which phosphomolybdic acid adsorbs foreign noble metal ions, and then anneals into a series of Mo-based alloy oxide clusters (PtMo, IrMo, AuMo and PdMo), where oxygen is the terminal oxygen outside the cluster. The as-prepared alloy clusters have tunable atomic ratio and uniform size around 1 nm. Taking PtMo clusters as an example, their electrocatalytic nitrogen reduction reaction (NRR) has been investigated in depth. Among all compositions, PtMo-6 cluster (Pt:Mo atomic ratio 1:2) exhibits the highest NRR activity with a Faradaic efficiency of 14.37% and a NH3 yield rate of 65.3 mu g h(-1) mg(cat.)(-1) in 0.1 M KOH, surpassing the known Mo-based catalysts. The combination of operando X-ray absorption spectroscopy and DFT calculations reveals that the oxide cluster in working state is the partially reduced. An unusual synergy is discovered, namely that Pt acts as a proton donor, providing *H to promote the hydrogenation of N-2 on the adjacent Mo atom. This work provides a simple and universal method for the precise synthesis of alloy clusters and new guidance for designing highly efficient NRR catalysts.
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