Size Stability and H2/CO Selectivity for Au Nanoparticles during Electrocatalytic CO2 Reduction

Journal of the American Chemical Society
Jamie A TrindellRichard M Crooks

Abstract

In this paper, we show that Au nanoparticles (AuNPs) stabilized with either citrate or by low-generation dendrimers rapidly grow during electrocatalytic reduction of CO2. For example, citrate-stabilized AuNPs and AuNPs encapsulated within sixth-generation, hydroxyl-terminated, poly(amidoamine) dendrimers (G6-OH DENs) having diameters of ∼2 nm grow substantially in size (to 6-7 nm) and polydispersity during just 15 min of electrolysis at -0.80 V (vs RHE). This degree of instability makes it impossible to correlate the structure of AuNPs determined prior to electrocatalysis to their catalytic function. In contrast to the G6-OH dendrimer, the higher generation G8-OH analogue stabilizes AuNPs under the same conditions that lead to instability of the other two materials. More specifically, G8-OH DENs having an initial size of 1.7 ± 0.3 nm increase to only 2.2 ± 0.5 nm during electrolysis in 0.10 M NaHCO3 at -0.80 V (vs RHE). Even when the electrolysis is carried out at -1.20 V, the higher-generation dendrimer stabilizes encapsulated AuNPs. This is presumably due to the compactness of the periphery of the G8-OH dendrimer. Although the G8-OH dendrimer nearly eliminates AuNP growth, the surface of the AuNP is still accessible for elect...Continue Reading

References

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Citations

Jul 20, 2018·Nanoscale·Yichuan DingReinhold H Dauskardt
Aug 22, 2018·Advanced Materials·Tingting ZhengHaotian Wang
Apr 22, 2020·Chemistry : a European Journal·Zhao-Qing LiuXiao-Tong Wang
May 22, 2018·Journal of Colloid and Interface Science·Yuanxing WangDunwei Wang
Jun 8, 2021·Langmuir : the ACS Journal of Surfaces and Colloids·Dhruba K PattadarFrancis P Zamborini
Jun 13, 2018·Analytical Chemistry·Matthew W Glasscott, Jeffrey E Dick
Oct 29, 2019·Chemical Reviews·Jamie A TrindellRichard M Crooks
Oct 28, 2019·Langmuir : the ACS Journal of Surfaces and Colloids·Dhruba K Pattadar, Francis P Zamborini
Jun 12, 2020·The Journal of Physical Chemistry Letters·Zhuo-Qun ZhangAnthony Shoji Hall
Nov 19, 2019·Nano Letters·Kam Sang KwokDavid H Gracias
Oct 5, 2018·Journal of the American Chemical Society·Dhruba K Pattadar, Francis P Zamborini

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