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Synthesis, structure anatomy, and catalytic properties of Ag14Cu2 nanoclusters co-protected by alkynyl and phosphine ligands
Dalton Transactions ( IF 3.5 ) Pub Date : 2023-10-20 , DOI: 10.1039/d3dt02838k
Quanli Shen 1 , Xuzi Cong 2 , Leyi Chen 1 , Lei Wang 1 , Yonggang Liu 1 , Likai Wang 2 , Zhenghua Tang 1
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We report the synthesis, structure anatomy, and catalytic properties of Ag14Cu2(C[triple bond, length as m-dash]CArF)14(PPh3)4 (C[triple bond, length as m-dash]CArF: 3,5-bis(trifluoromethyl)phenylacetylene) nanoclusters, denoted as Ag14Cu2. Ag14Cu2 has a robust electronic structure with two free valence electrons, and it has a distinctive absorbance feature. Single-crystal X-ray diffraction (SC-XRD) disclosed that Ag14Cu2 possesses an octahedral Ag6 metal kernel capped by two Ag4Cu1(C[triple bond, length as m-dash]CArF)7(PPh3)2 metal–ligand units. Remarkably, it exhibits excellent bifunctional catalytic performance for 4-nitrophenol reduction and the electrochemical CO2 reduction reaction (eCO2RR). In 4-nitrophenol reduction, it adopts first-order reaction kinetics with a rate constant of 0.137 min−1, while in the eCO2RR, it shows a CO faradaic efficiency (FECO) of 83.71% and a high current density of 92.65 mA cm−2 at −1.6 V vs. RHE. Moreover, Ag14Cu2 showed robust long-term stability with no significant decay in current density and FECO over 10 h of continuous operation in the eCO2RR. This study not only enriches the potpourri of alkynyl-protected bimetallic AgCu nanoclusters, but also demonstrates the great potential of employing metal nanoclusters for bifunctional catalytic applications.

中文翻译:

炔基和膦配体共保护的Ag14Cu2纳米团簇的合成、结构解剖及催化性能

我们报道了Ag 14 Cu 2 (C [三键,长度为m-破折号]CAr F ) 14 (PPh 3 ) 4 (C [三键,长度为m-破折号]CAr F : 3,5-bis(三氟甲基)苯乙炔)纳米团簇的合成、结构解剖和催化性能,表示为Ag 14 Cu 2。Ag 14 Cu 2具有坚固的电子结构,具有两个自由价电子,并且具有独特的吸收特征。单晶X射线衍射(SC-XRD)表明Ag 14 Cu 2具有八面体Ag 6金属核,其由两个Ag 4 Cu 1 (C [三键,长度为m-破折号]CAr F ) 7 (PPh 3 ) 2金属配体单元覆盖。值得注意的是,它对4-硝基苯酚还原和电化学CO 2还原反应(eCO 2 RR)表现出优异的双功能催化性能。在4-硝基苯酚还原中,采用一级反应动力学,速率常数为0.137 min -1,而在eCO 2 RR中,CO法拉第效率(FE CO)为83.71%,电流密度为92.65 mA cm -2(-1.6 V vs. RHE)。此外,Ag 14 Cu 2显示出强大的长期稳定性,在 eCO 2 RR 中连续运行 10 小时后,电流密度和 FE CO没有显着衰减。这项研究不仅丰富了炔基保护的双金属AgCu纳米团簇的种类,而且展示了金属纳米团簇在双功能催化应用中的巨大潜力。
更新日期:2023-10-20
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