PPh3: Converts Thiolated Gold Nanoparticles to [Au25(PPh3)10(SR)5Cl2]2+

Citation: ZHU Min, LI Manbo, YAO Chuanhao, XIA Nan, ZHAO Yan, YAN Nan, LIAO Lingwen, WU Zhikun. PPh_3: Converts Thiolated Gold Nanoparticles to [Au₂₅(PPh₃)₁₀(SR)₅Cl₂]²⁺[J]. Acta Physico-Chimica Sinica, 2018, 34(7): 792-798. doi: 10.3866/PKU.WHXB201710091 shu

三苯基膦：转换硫醇保护的纳米粒子成[Au₂₅(PPh₃)₁₀(SR)₅Cl₂]²⁺

祝敏 ^1,2,†, ,
李漫波 ^1,†, ,
姚传好 ^1, ,
夏楠 ^1, ,
赵燕 ^1,2, ,
闫楠 ^1, ,
廖玲文 ^1, ,
伍志鲲 ^{1,
,}

1.
中国科学院固体物理研究所，中国科学院材料物理重点实验室，安徽省纳米材料与技术重点实验室，中国科学院纳米卓越心，合肥 230031
2.
中国科学技术大学，合肥 230026

通讯作者: 伍志鲲, zkwu@issp.ac.cn

基金项目:
国家自然科学基金 21222301

合肥物质科学技术中心方向项目培育基金 2014FXCX002

国家自然科学基金 21528303

国家自然科学基金 21771186

国家自然科学基金(21222301, 21528303, 21603234, 21771186, 21171170, 21601193)、国家重大科学研究计划(2013CB934302)、合肥物质科学技术中心方向项目培育基金(2014FXCX002)、中国科学院创新国际团队资助项目

国家自然科学基金 21171170

国家重大科学研究计划 2013CB934302

国家自然科学基金 21601193

国家自然科学基金 21603234

摘要: 我们在此报道了一种未曾发现的有趣现象：尽管[Au₂₃(SC₆H₁₁)₁₆]⁻、Au₂₄(SC₂H₄Ph)₂₀ (Ph:苯环)、Au₃₆(TBBT)₂₈ (TBBTH:对叔丁基苯硫酚)、Au₃₈(SC₂H₄Ph)₂₄、混合Au_x(SC₂H₄Ph)_y团簇及3 nm的金纳米粒子有不同的组成、结构、尺寸和保护性硫醇配体，但它们在三苯基膦(PPh₃)作用下，均能统一地经由亚稳的[Au₁₁(PPh₃)₈Cl₂]²⁺最终转化为稳定的双二十面体[Au₂₅(PPh₃)₁₀(SR)₅Cl₂]²⁺ (SR:硫醇配体)。换句话说，三苯基膦是这些硫醇保护的纳米粒子的统一转化器。然而，聚乙烯吡咯烷酮(PVP)/柠檬酸盐(Citrate)保护的金纳米粒子和[Ag₂₅(SPhMe₂)₁₈]⁻ (Me:甲基)在同样的条件下，却不能转化为[Au₂₅(PPh₃)₁₀(SR)₅Cl₂]²⁺或[Ag₂₅(PPh₃)₁₀(SR)₅Cl₂]²⁺，暗示了硫醇保护的金纳米粒子具有与三苯基膦反应的独特性能。另外，我们考察了配体对双二十面体[Au₂₅(PPh₃)₁₀(SR)₅Cl₂]²⁺团簇荧光性能的影响。

关键词:

English

PPh_3: Converts Thiolated Gold Nanoparticles to [Au₂₅(PPh₃)₁₀(SR)₅Cl₂]²⁺

1.
Key Laboratory of Materials Physics, Anhui Key Laboratory of Nanomaterials and Nanotechnology, CAS Center for Excellence in Nanoscience, Institute of Solid State Physics, Chinese Academy of Sciences, Hefei 230031, P. R. China
2.
University of Science and Technology of China, Hefei 230026, P. R. China
^† These authors contributed equally to this work

Corresponding author: WU Zhikun, zkwu@issp.ac.cn

Received Date: 12 September 2017
Accepted Date: 28 September 2017
Revised Date: 28 September 2017
Available Online: 15 July 2018
Fund Project:

The project was supported by the National Natural Science Foundation of China (21222301, 21528303, 21603234, 21771186, 21171170, and 21601193), the National Basic Research Program of China (2013CB934302), the Innovative Program of Development Foundation of Hefei Center for Physical Science and Technology (2014FXCX002), and the CAS/SAFEA International Partnership Program for Creative Research Teams

Abstract: Research on gold nanoclusters is at the frontier of nanoscience and nanotechnology. The introduction of the first phosphine-protected gold nanocluster, Au₁₁(PPh₃)₇(SCN)₃ (where PPh₃ stands for triphenylphosphine and Ph stands for benzene), can be dated back to 1969. As research in the field progressed, many structures of phosphine-protected nanoclusters such as Au₅, Au₈, Au₁₃, and Au₃₉ were reported. However, the stability of these phosphine-protected nanoclusters was not satisfactory, which handicapped their research and application. In an attempt to find alternatives for phosphine-protected nanoclusters, thiolated gold nanoclusters have attracted extensive attention in recent years. So far, there has been great progress primarily owing to the development of wet-chemical synthesis techniques, among which the utilization of ligand-exchange has been proved to be very effective to synthesize thiolated gold nanoclusters. It can be easily understood that phosphine in gold nanoclusters can be exchanged with thiolate because the latter has stronger affinity for gold. However, we recently found that the reverse ligand-exchange, i.e., the exchange of thiolate with phosphine, can also take place. Some questions have naturally arisen: Is the reverse ligand-exchange only applicable to superatomic [Au₂₅(SR)₁₈]⁻ (SR: thiolate) nanoclusters? Can it occur in other thiolated gold nanoclusters? If so, is this reverse ligand-exchange also dependent on the starting nanoclusters? These intriguing issues have inspired us to conduct this work. We investigated the reactions of PPh₃ with some thiolated gold nanoparticles, including [Au₂₃(SC₆H₁₁)₁₆]⁻, Au₂₄(SC₂H₄Ph)₂₀, Au₃₆(TBBT)₂₈ (where TBBT stands for 4-(tert-butyl) benzene-1-thiolate), Au₃₈(SC₂H₄Ph)₂₀, mixed nanoclusters, and 3 nm Au nanoparticles. Surprisingly, the experimental results showed that under the action of PPh₃, thiolated gold nanoclusters (or nanoparticles) with different compositions, structures, sizes, and protecting thiolates can be uniformly transformed to [Au₁₁(PPh₃)₈Cl₂]⁺ and then [Au₂₅(PPh₃)₁₀(SR)₅Cl₂]²⁺. In other words, PPh₃ is a universal converter for these thiolated gold nanoparticles. However, gold nanoparticles that are protected by polyvinylpyrrolidone (PVP) or citrate and [Ag₂₅(SPhMe₂)₁₈]⁻ particles cannot be transformed to [Au₂₅(PPh₃)₁₀(SR)₅Cl₂]²⁺ and [Ag₂₅(PPh₃)₁₀(SR)₅Cl₂]²⁺, respectively, under the same conditions, which indicated that the special reactivity with PPh₃ is unique to thiolated gold nanoparticles. Our preliminary investigation on a possible reaction path between thiolated gold nanoparticles and PPh₃ also revealed that the peeling process found in Au₂₅ nanoclusters may be applicable to the conversion of [Au₂₃(SC₆H₁₁)₁₆]⁻, but not other nanoclusters like Au₂₄(SC₂H₄Ph)₂₀ and Au₃₆(TBBT)₂₈. Employing this special chemistry, we synthesized seven [Au₂₅(PPh₃)₁₀(SR)₅Cl₂]²⁺ species with various ligands and investigated the effect of the ligand on the luminescence properties of [Au₂₅(PPh₃)₁₀(SR)₅Cl₂]²⁺. We found that the luminescence quantum yields decreased in the following order: [Au₂₅(PPh₃)₁₀(SCH₂Ph-t-Bu)₅Cl₂]²⁺ (1.32 × 10⁻⁴) > [Au₂₅(PPh₃)₁₀(SCH₂Ph)₅Cl₂]²⁺ (8.23 × 10⁻⁵) > [Au₂₅(PPh₃)₁₀(SC₂H₄Ph)₅Cl₂]²⁺ (5.35 × 10⁻⁶) > [Au₂₅(PPh₃)₁₀(SC₁₂H₂₅)₅Cl₂]²⁺ (5.02 × 10⁻⁶) > [Au₂₅(PPh₃)₁₀(SPh-t-Bu)₅Cl₂]²⁺ (3.97 × 10⁻⁶) > [Au₂₅(PPh₃)₁₀(SC₆H₁₃)₅Cl₂]²⁺ (3.73 × 10⁻⁶) > [Au₂₅(PPh₃)₁₀(S-c-C₆H₁₁)₅Cl₂]²⁺ (1.53 × 10⁻⁶). Therefore, it can be concluded that SCH₂Ph-t-Bu is the best ligand, while S-c-C₆H₁₁ is the worse one for triggering luminescence from gold nanoparticles in the investigated thiolates. Since such diversity in surface ligands is not found in other nanoclusters (e.g., [Au₂₅(SR)₁₈]⁻), the special chemistry between thiolated gold nanoparticles and PPh₃ provides excellent opportunities to investigate the effect of ligands on the properties of gold nanoparticles and to screen ligands for special applications. In summary, in this work we reveal the unique chemistry of thiolated gold nanoparticles with PPh₃ and provide excellent opportunities for investigating ligand effects of gold nanoparticles and screening ligands for special applications.

Key words:

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沈阳化工大学材料科学与工程学院沈阳 110142

三苯基膦：转换硫醇保护的纳米粒子成[Au₂₅(PPh₃)₁₀(SR)₅Cl₂]²⁺

通讯作者: 伍志鲲, zkwu@issp.ac.cn

English

PPh_3: Converts Thiolated Gold Nanoparticles to [Au₂₅(PPh₃)₁₀(SR)₅Cl₂]²⁺

Corresponding author: WU Zhikun, zkwu@issp.ac.cn

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三苯基膦：转换硫醇保护的纳米粒子成[Au25(PPh3)10(SR)5Cl2]2+

通讯作者: 伍志鲲, zkwu@issp.ac.cn

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