A synchronous nucleation and passivation strategy for controllable synthesis of Au 36 (PA) 24 : unveiling the formation

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synchronous nucleation and passivation strategy for controllable synthesis of Au36(PA)24: unveiling the formation process and the role of Au22(PA)18 intermediate 1

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Xiaoshuang Ma , Guanyu Ma , Lubing Qin , Guangxu Chen , 3* 1,2* Shaowei Chen & Zhenghua Tang 1

Guangzhou Key Laboratory for Surface Chemistry of Energy Materials and New Energy Research Institute, School of Environment and

Energy, South China University of Technology, Guangdong 510006, China; Guangdong Engineering and Technology Research Center for Surface Chemistry of Energy Materials, School of Environment and Energy,

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South China University of Technology, Guangzhou Higher Education Mega Centre, Guangdong 510006, China; Department of Chemistry and Biochemistry, University of California, 1156 High Street, Santa Cruz, California, 95064, United States Received June 23, 2020; accepted July 7, 2020; published online September 1, 2020

Despite the recent progress on controllable synthesis of alkynyl-protected Au nanoclusters, the effective synthetic means are very limited and the cluster formation process still remains puzzling. Here, we develop a novel synchronous nucleation and passivation strategy to fabricate Au36(PA)24 (PA=phenylacetylenyl) nanoclusters with high yield. In Au36(PA)24 formation process, Au22(PA)18 as key intermediate was identified. Meanwhile, Au22(PA)18 can be synthesized under a low amount of reductant, and by employing more reductants, Au22(PA)18 can turn into Au36(PA)24 eventually. Moreover, the structure evolution from Au22(PA)18 to Au36(PA)24 is proposed, where four Au13 cuboctahedra can yield one Au28 kernel. Finally, the ratiocination is verified by the good accordance between the predicted intermediate/product ratio and the experimental value. This study not only offers a novel synthetic strategy, but also sheds light on understanding the structural evolution process of alkynyl-protected Au nanoclusters at atomic level. synchronous nucleation and passivation, Au36(PA)24, Au22(PA)18, unveiling the formation process, structure evolution, intermediate/product ratio Citation:

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Ma X, Ma G, Qin L, Chen G, Chen S, Tang Z. A synchronous nucleation and passivation strategy for controllable synthesis of Au36(PA)24: unveiling the formation process and the role of Au22(PA)18 intermediate. Sci China Chem, 2020, 63, https://doi.org/10.1007/s11426-020-9819-4

Introduction

Atomically precise coinage metal nanoclusters with molecular purity have been gaining tremendous research attention in the past decade [1–8], as their well-defined structures provide an ideal platform to establish the relationship between the structure and the physiochemical properties including luminescence [5,9,10], catalytic reactivities [6,11,12], electrochemical behaviors [13], and biomedical *Corresponding authors (email: [email protected]; [email protected])

capabilities as biolabeling agents [14] or biomarkers [15,16]. The last decade has witnessed the great success on controllable synthesis and structural determination of thiolate Au nanoclusters,