长期探寻的Au23(S-Adm)16结构及未曾预期的掺杂效应

doi:10.3866/PKU.WHXB202305029

物理化学学报 >> 2024, Vol. 40 >> Issue (5): 2305029.doi: 10.3866/PKU.WHXB202305029

长期探寻的Au₂₃(S-Adm)₁₆结构及未曾预期的掺杂效应

冯磊¹^,², 朱泽敏¹, 杨颖¹^,², 何宗兵¹^,², 邹家丰¹^,², 李漫波¹^,²^,*(), 赵燕¹^,²^,*(), 伍志鲲¹^,²^,*()

¹ 安徽大学物质科学与信息技术研究院, 合肥 230601
² 中国科学院合肥物质科学研究院固体物理研究所, 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中心, 合肥 230031

收稿日期:2023-05-15 修回日期:2023-06-10 录用日期:2023-06-12 发布日期:2023-06-27
通讯作者: Email: mbli@ahu.edu.cn (李漫波)20231@ahu.edu.cn (赵燕)zkwu@issp.ac.cn; Tel.: +86-551-65595395 (伍志鲲)
基金资助:
国家自然科学基金(21925303); 国家自然科学基金(21771186); 国家自然科学基金(21829501); 国家自然科学基金(21222301); 国家自然科学基金(21528303); 国家自然科学基金(21171170); 国家自然科学基金(92061110); 中国科学院合肥研究院院长基金(BJPY2019A02); 中国科学院合肥研究院十三五重点计划(KP-2017-16); 中国科学院合肥科学中心协同创新项目(2020HSC-CIP005); 中国科学院合肥科学中心协同创新项目(2022HSC-CIP018); 安徽省自然科学基金(2108085Y05); 合肥微尺度物理科学国家实验室(KF2020102); 安徽大学启动经费(S020318006/037)

Long-Pursued Structure of Au₂₃(S-Adm)₁₆ and the Unexpected Doping Effects

Lei Feng¹^,², Ze-Min Zhu¹, Ying Yang¹^,², Zongbin He¹^,², Jiafeng Zou¹^,², Man-Bo Li¹^,²^,*(), Yan Zhao¹^,²^,*(), Zhikun Wu¹^,²^,*()

¹ Institute of Physical Science and Information Technology, Anhui University, Hefei 230601, China
² Key Laboratory of Materials Physics, Anhui Key Laboratory of Nanomaterials and Nanotechnology, CAS Center for Excellence in Nanoscience, Institute of Solid State Physics, Hefei Institutes of Physical Science, Chinese Academy of Sciences, Hefei 230031, China

Received:2023-05-15 Revised:2023-06-10 Accepted:2023-06-12 Published:2023-06-27
Contact: Email: mbli@ahu.edu.cn (Man-Bo Li)20231@ahu.edu.cn (Yan Zhao)zkwu@issp.ac.cn; Tel.: +86-551-65595395 (Zhikun Wu)
Supported by:
the National Natural Science Foundation of China(21925303); the National Natural Science Foundation of China(21771186); the National Natural Science Foundation of China(21829501); the National Natural Science Foundation of China(21222301); the National Natural Science Foundation of China(21528303); the National Natural Science Foundation of China(21171170); the National Natural Science Foundation of China(92061110); CASHIPS Director's Fund(BJPY2019A02); Key Program of 13th Five-year Plan, CASHIPS(KP-2017-16); Collaborative Innovation Program of Hefei Science Center, CAS(2020HSC-CIP005); Collaborative Innovation Program of Hefei Science Center, CAS(2022HSC-CIP018); Anhui Provincial Natural Science Foundation(2108085Y05); Hefei National Laboratory for Physical Sciences at the Microscale(KF2020102); the Startup Fund of Anhui University(S020318006/037)

1. WHXB202305029-SI-6p.pdf(2292KB)

摘要/Abstract

摘要：

一锅同时获得单个金属原子掺杂的纳米团簇与母体团簇富有挑战性。这样的合成可排除微量杂质的影响，使得掺杂和未掺杂纳米团簇的性质对比更加合理可靠。在此，我们首次实现了这种合成，得到了长期追寻的纳米团簇Au₂₃(S-Adm)₁₆和其单镉掺杂的Au₂₂Cd₁(S-Adm)₁₆纳米团簇，并通过单晶X射线晶体学解析了其结构。令人惊讶的是，与以前的报道结果相反，Au₂₃(S-Adm)₁₆比Au₂₂Cd₁(S-Adm)₁₆更稳定。另一方面，由于掺入镉原子后，内核Au―Au键长度增加，光激发电子转移阻力增加，导致Au₂₂Cd₁(S-Adm)₁₆吸收和发射强度明显下降。因而，不仅团簇的稳定性，而且团簇的吸收和发射强度也与内核Au―Au键的长度关联。这项工作表明了两种团簇结构上的微小差异就可导致光学、热稳定性等方面的显著区别，也为研究金属纳米团簇的构效关系提供了良好的借鉴。

关键词: 金属纳米团簇, 合成, Au―Au键长, 性质, 构效关系

Abstract:

Metal nanoclusters are rising stars in material science, and one advantage is their atomically precise tunability. It is well known that metal doping can efficiently modify the properties of metal nanoclusters. In particular, without altering the parent nanocluster framework, doping a single heterometal atom can tailor the properties of metal nanoclusters and aid investigations of the structure–property relationship of metal nanoclusters. To our knowledge, the simultaneous synthesis of a single heterometal-doped nanocluster and its parent nanocluster is challenging and has not been previously reported; however, this is highly desirable because it can prevent the influence of trace impurities and allow comparison between doped and undoped nanoclusters. The single Cd-doped gold nanocluster Au₂₂Cd₁(S-Adm)₁₆ (S-Adm = 1-adamantanethiolate) has been previously synthesized and structurally elucidated. However, the structure of the parent nanocluster, Au₂₃(S-Adm)₁₆, remains unknown, inspiring this investigation. In this study, we synthesized Au₂₃(S-Adm)₁₆ and its single-doped Au₂₂Cd₁(S-Adm)₁₆ nanocluster in one pot for the first time, and we resolved their structures using single-crystal X-ray crystallography. The structure of Au₂₂Cd₁(S-Adm)₁₆ is similar to that of Au₂₃(S-Adm)₁₆ except that a kernel Au atom in Au₂₃(S-Adm)₁₆ is replaced with a Cd atom. This Cd replacement causes the kernel Au―Au bond length to increase owing to the loosening of the original closely packed structure. In contrast to prior reports, Au₂₃(S-Adm)₁₆ is surprisingly more stable than Au₂₂Cd₁(S-Adm)₁₆, as determined via ultraviolet visible-near infrared (UV-Vis-NIR) spectroscopy at 80 ℃. This stability was attributed to the decrease in the kernel Au―Au bond length. Although the maximum absorption of Au₂₂Cd₁(S-Adm)₁₆ slightly red-shifted from 605 to 608 nm after Cd doping, the molar extinction coefficient of Au₂₃(S-Adm)₁₆ at 605 nm was approximately twice that of Au₂₂Cd₁(S-Adm)₁₆ at 608 nm. Thus, the increase in kernel Au―Au bond length may decrease the photoexcitation electron transfer efficiency owing to lengthening of the photoexcitation electron transfer pathway. As further support for this opinion, although the two nanoclusters showed similar emission profiles and maxima (750 nm for Au₂₃(S-Adm)₁₆ and 760 nm for Au₂₂Cd₁(S-Adm)₁₆), they exhibited obvious emission intensity differences. Specifically, the quantum yield of Au₂₃(S-Adm)₁₆ (approximately 3.160 × 10⁻⁵) was found to be 1.13 times that of Au₂₂Cd₁(S-Adm)₁₆ (approximately 2.793 × 10⁻⁵). Thus, the stability and absorption and emission intensities correlate with the kernel Au―Au bond length.This study shows that two metal nanoclusters with slight structural differences can exhibit different properties in terms of optical and thermal stability, providing a good reference for studying their structure–property relationships.

Key words: Metal nanoclusters, Synthesis, Au―Au bond length, Property, Property–structure correlation

冯磊, 朱泽敏, 杨颖, 何宗兵, 邹家丰, 李漫波, 赵燕, 伍志鲲. 长期探寻的Au₂₃(S-Adm)₁₆结构及未曾预期的掺杂效应[J]. 物理化学学报, 2024, 40(5), 2305029. doi: 10.3866/PKU.WHXB202305029

Lei Feng, Ze-Min Zhu, Ying Yang, Zongbin He, Jiafeng Zou, Man-Bo Li, Yan Zhao, Zhikun Wu. Long-Pursued Structure of Au₂₃(S-Adm)₁₆ and the Unexpected Doping Effects[J]. Acta Phys. -Chim. Sin. 2024, 40(5), 2305029. doi: 10.3866/PKU.WHXB202305029

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB202305029

https://www.whxb.pku.edu.cn/CN/Y2024/V40/I5/2305029

图/表 3

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长期探寻的Au₂₃(S-Adm)₁₆结构及未曾预期的掺杂效应

Long-Pursued Structure of Au₂₃(S-Adm)₁₆ and the Unexpected Doping Effects

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