Ligand-regulated ORR activity of Au nanoparticles in alkaline medium: the importance of surface coverage of ligands†,Catalysis Science & Technology

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Ligand-regulated ORR activity of Au nanoparticles in alkaline medium: the importance of surface coverage of ligands†
Catalysis Science & Technology ( IF 4.4 ) Pub Date : 2017-12-13 00:00:00 , DOI: 10.1039/c7cy02101a
Linfang Lu _{1,

2,

3,

4,

5} , Shihui Zou _{1,

2,

3,

4,

5} , Yuheng Zhou _{1,

2,

3,

4,

5} , Juanjuan Liu _{5,

6,

7,

8} , Renhong Li _{5,

9,

10,

11,

12} , Zhen Xu _{1,

2,

3,

4,

5} , Liping Xiao _{1,

2,

3,

4,

5} , Jie Fan _{1,

2,

3,

4,

5}

Affiliation

The functionalization of organic ligands on nanoparticles (NPs) to create metal–organic interfaces can tune their activity and selectivity in catalytic reactions. Compared to the well-documented electronic and steric contribution of organic ligands, the coverage of ligands is also a significant factor but has been rarely investigated. Herein, we employ two methods, potential cycling and thermal annealing, to judiciously remove surface ligands from gold nanoparticles (AuNPs) and systematically investigate the influence of surface coverage of ligands on the catalytic performance. Potential cycling enables mild removal of ligands without changing the size of AuNPs and thus provides ideal models to identify the intrinsic influence of the surface coverage of ligands on oxygen reduction reaction (ORR). The ORR activity and selectivity is quantitatively evaluated by plotting the half potential and electron transfer number versus the surface coverage of ligands. Thermal annealing at different temperatures produces differently sized AuNPs with various surface ligand coverages. Compared to the size effect, we found that the surface coverage of ligands played a dominant role in the ORR activity of AuNPs. Most importantly, capping AuNPs with oleylamine and sodium citrate and reverse poisoning clean AuNPs with thiol, butylamine and CTAB further reveal that the difference in the ORR activity/selectivity of the capped AuNPs is directly related to the surface coverage of the ligands regardless of the diverse chemical nature of these ligands. This work highlights that the surface coverage of ligands should be considered as an important factor for catalytic reactions accounting for metal–organic interfaces.

中文翻译：

碱性介质中金纳米粒子的配体调节的ORR活性：配体表面覆盖的重要性†

纳米颗粒（NPs）上有机配体的功能化可创建金属-有机界面，可调节其在催化反应中的活性和选择性。与有据可查的有机配体的电子和空间贡献相比，配体的覆盖率也是一个重要因素，但很少进行研究。在这里，我们采用潜在的循环和热退火两种方法，明智地从金纳米颗粒（AuNPs）中去除表面配体，并系统地研究配体表面覆盖率对催化性能的影响。电位循环可在不改变AuNPs大小的情况下温和地除去配体，因此提供了理想的模型来鉴定配体表面覆盖对氧还原反应（ORR）的内在影响。相对于配体的表面覆盖率。在不同温度下进行热退火会产生具有不同表面配体覆盖率的尺寸不同的AuNP。与尺寸效应相比，我们发现配体的表面覆盖在AuNPs的ORR活性中起着主导作用。最重要的是，用油胺和柠檬酸钠封端AuNP，并用硫醇，丁胺和CTAB进行中毒的清洁AuNP进一步揭示，封端AuNPs的ORR活性/选择性的差异与配体的表面覆盖率直接相关，而不管其种类如何。这些配体的化学性质。这项工作强调，配体的表面覆盖率应被视为考虑金属-有机界面的催化反应的重要因素。

更新日期：2017-12-13

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