New atomically precise M1Ag21 (M = Au/Ag) nanoclusters as excellent oxygen reduction reaction catalysts.

New atomically precise M1Ag21 (M = Au/Ag) nanoclusters as excellent oxygen reduction reaction catalysts.
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新型原子级精确的 M1Ag21 (M = Au/Ag) 纳米团簇作为优异的氧还原反应催化剂

DOI:
10.1039/d0sc05923d
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发表时间:
2021-01-07
期刊:
影响因子:
8.4
通讯作者:
Zhu M
Zhu M
中科院分区:
化学1区
文献类型:
--
作者:
Zou X;He S;Kang X;Chen S;Yu H;Jin S;Astruc D;Zhu M

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通过引入1,1 ′-双(二苯基膦基)二茂铁(dppf)作为活化配体,可控合成了两种新型纳米团簇M1 Ag 21(M = Au/Ag),并对其结构进行了表征.通过SCXC确定了M1Ag 21纳米团簇的原子精确结构,并通过ESI-TOF-MS,TGA,XPS,DPV和FT-IR测量进一步证实。活性炭(C)负载的M1Ag 21纳米团簇在碱性溶液中被用作有效的氧还原反应(ORR)催化剂。密度泛函理论(DFT)计算表明,两个团簇体系的催化活性均源于M1Ag 21中M13核与dppf配体之间的协同效应.这项工作揭示了制备团簇基电催化剂和其他催化剂的活化和修饰的外围配体。新型纳米团簇M1Ag 21(dppf)3(SAdm)12(M = Au/Ag)中1,1 ′-双(二苯基膦基)二茂铁配体的存在和系综效应提供了优异的ORR性能。
By introducing 1,1′-bis-(diphenylphosphino)ferrocene (dppf) as an activating ligand, two novel nanoclusters, M1Ag21 (M = Au/Ag), have been controllably synthesized and structurally characterized. The atomically precise structures of the M1Ag21 nanoclusters were determined by SCXC and further confirmed by ESI-TOF-MS, TGA, XPS, DPV, and FT-IR measurements. The M1Ag21 nanoclusters supported on activated carbon (C) are exploited as efficient oxygen reduction reaction (ORR) catalysts in alkaline solutions. Density functional theory (DFT) calculations verify that the catalytic activities of the two cluster-based systems originate from the significant ensemble synergy effect between the M13 kernel and dppf ligand in M1Ag21. This work sheds lights on the preparation of cluster-based electrocatalysts and other catalysts that are activated and modified by peripheral ligands. The presence of 1,1′-bis-(diphenylphosphino)ferrocene ligands and ensemble effects in novel nanoclusters M1Ag21(dppf)3(SAdm)12 (M = Au/Ag) provide excellent ORR performances.
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