单分子荧光成像研究单颗粒纳米催化机制

doi:10.6023/A23040147

化学学报 ›› 2023, Vol. 81 ›› Issue (8): 1002-1014.DOI: 10.6023/A23040147 上一篇下一篇

综述

单分子荧光成像研究单颗粒纳米催化机制

王晓^a^,^*(), 王星文^a, 肖乐辉^b^,^*()

a 南开大学化学学院天津 300071
b 中南大学化学化工学院长沙 410083

投稿日期:2023-04-20 发布日期:2023-09-14

作者简介:

王晓, 2017年本科毕业于南京师范大学, 2022年博士毕业于南开大学, 师从肖乐辉教授, 现任南开大学科研助理, 主要从事单分子荧光成像、单颗粒纳米催化方向的研究.

王星文, 南开大学在读硕士, 主要从事单分子荧光成像、荧光探针及色谱填料合成方向的研究.

肖乐辉, 现任中南大学特聘教授, 博士生导师, 国家自然科学基金优秀青年基金获得者, 主持多项国家自然科学基金面上课题, 在国际顶尖期刊发表SCI论文80余篇, 发现了等离激元热点诱导的快速晶格重排规律, 开创性提出了金属异质结模型用于光催化体系热载流子的高效传递, 近年来主要围绕分子识别、动态示踪以及单分子反应开展研究工作.

基金资助:
项目受国家自然科学基金(22174079); 项目受国家自然科学基金(21974073)

Nanocatalytic Mechanisms Investigated by Single Molecule Fluorescence Imaging at the Single-Particle Level

Xiao Wang^a(), Xingwen Wang^a, Lehui Xiao^b()

a College of Chemistry, Nankai University, Tianjin 300071
b College of Chemistry and Chemical Engineering, Central South University, Changsha 410083

Received:2023-04-20 Published:2023-09-14
Contact: *E-mail: wangxiao_wx2017@163.com; lehuixiao@163.com
Supported by:
National Natural Science Foundation of China(22174079); National Natural Science Foundation of China(21974073)

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摘要/Abstract

纳米颗粒通常具有优异的催化性能, 但由于其内在的异质性, 宏观水平的表征难以确定单个纳米颗粒可靠的构效关系和潜在的催化反应机制. 单分子荧光成像技术具有单分子灵敏度、高时空分辨率的优点, 可以在单颗粒水平实现反应产物的超灵敏检测, 因而在纳米催化领域得到了广泛应用. 本文综述了单分子荧光成像的发展以及该技术在揭示单颗粒纳米催化反应机制中的应用, 主要包括尺寸效应、晶面效应、表面缺陷、等离激元效应、双金属效应、活化能、纳米限域效应以及单颗粒催化通讯等方面. 最后总结和展望了单分子荧光成像技术在纳米催化研究中的挑战与发展方向.

关键词: 单分子荧光, 单颗粒, 时空分辨率, 纳米催化机制, 构效关系

With the ever-increasing demands for energy and declining reserves of fossil fuels, efficient use of fossil fuels and energy extraction from alternative raw materials are critical to the sustainable future of humanity. Catalysis is one of the key technologies capable of helping address this energy challenge. Nanocatalysts are an integral part of catalysis technology, and they can catalyze chemical transformation for petroleum processing and energy conversions, which are more efficient than their bulk materials. With the rapid development of nanoscience, new nanocatalysts and novel catalytic properties continue to emerge. Tremendous work has been done in characterizing the catalytic properties of nanoparticles at the ensemble level. However, due to heterogeneous properties of nanoparticles in size, morphology or surface composition, traditional ensemble methods can only provide averaged behavior of numerous nanoparticles. Therefore, it is difficult to determine the reliable structure-activity relationship for individual nanoparticles. In addition, owing to the surface structural reconstruction, the active sites of nanocatalysts are variable under catalysis. Revealing the dynamic evolution of active sites is helpful to understand the process and mechanism of catalytic reaction. Consequently, developing a direct approach to study the nanocatalysis at the single-particle level and in real-time with sufficient spatiotemporal resolution is highly demanding. Recently, due to the single-molecule sensitivity and high spatiotemporal resolution, single-molecule fluorescence imaging (SMFI) has been proved to be an effective tool for studying the heterogeneous nanocatalysts at the single-particle level. By adopting fluorogenic reactions and monitoring the fluorescence signal of a product, the reaction process on a single nanoparticle can be followed in real-time at single-turnover resolution under steady-state reaction kinetics. In this review, we discuss recent processes of SMFI in investigating nanocatalysis at the single-particle level. The discussion focuses on the development and application of SMFI in probing catalytic mechanisms, including the size effect, facet effect, surface defects, plasmonic effect, activation energy, bimetallic effect, nanoconfined effect and catalytic communication. Finally, challenges and prospects of the SMFI for investigating nanocatalysis are put forward.

Key words: single-molecule fluorescence, single-particle, spatiotemporal resolution, nanocatalytic mechanisms, structure-property relationship

引用此文

王晓, 王星文, 肖乐辉. 单分子荧光成像研究单颗粒纳米催化机制[J]. 化学学报, 2023, 81(8): 1002-1014.

Xiao Wang, Xingwen Wang, Lehui Xiao. Nanocatalytic Mechanisms Investigated by Single Molecule Fluorescence Imaging at the Single-Particle Level[J]. Acta Chimica Sinica, 2023, 81(8): 1002-1014.

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图/表 11

图1. (a)全内反射荧光显微装置(左)和单个纳米催化剂表面荧光反应示意图(右)[67]. (b)基于单分子定位的超分辨成像原理图示[39]

Figure 1. (a) The scheme of a TIRF microscope (left) and a fluorogenic reaction on the surface of a single nanocatalyst (right)[67]. Copyright 2013, American Chemical Society. (b) Principles of single-molecule localization-based super-resolution imaging[39]. Copyright 2017, American Chemical Society

图2. (a)纳米颗粒表面单分子催化反应的荧光成像. (b)图a标记颗粒在催化过程中表面荧光强度随时间变化的轨迹

Figure 2. (a) Typical image of single-molecule nanocatalysis on the surface of nanoparticles. (b) Segment trajectory of the fluorescence intensity versus time from the spot marked by the arrow in (a)

图3. (a) C-FDA的水解反应. (b) RZ的还原反应和AR的氧化反应, 反应产物均为RF. (c)糠醇的低聚反应. (d) APF的氧化反应. (e)苯基丁二烯基取代的BODIPY环氧化反应. (f) DN-BODIPY的还原反应.

Figure 3. (a) The transesterification of C-FDA. (b) The reduction of RZ and oxidation of AR. The reaction products are all RF. (c) The condensation of furfuryl alcohol. (d) The oxidation of APF. (e) The epoxidation reaction of phenylbutadienyl-substituted BODIPY. (f) The reduction of DN-BODIPY

图4. (a) AuNPs表面重构速率对催化反应速率和纳米颗粒尺寸的依赖[85]. (b)不同尺寸PdNCs的产物生成速率对RZ浓度的依赖[86]. (c)浓度依赖的Au15, Au18, Au25的产物生成速率[87]

Figure 4. (a) Surface restructuring rate from AuNPs dependence on the rate of turnovers and the nanoparticle diameter[85]. Copyright 2010, American Chemical Society. (b) RZ concentration dependence of product formation rates ?τoff??1 on PdNCs with different sizes[86]. Copyright 2016, Royal Society of Chemistry. (c) RZ concentration dependence of turnover rates on Au15, Au18, and Au25[87]. Copyright 2018, National Academy of Sciences of the United States of American

图5. (a)激光调控金纳米结构的形貌变化和单分子催化示意图[30]. (b)对苯二酚生成苯醌的氧化反应. (c)当HQ浓度为0和500 μmol/L时, AR氧化事件的二维直方图. 白线表示来自SEM成像的粒子轮廓. (d)当HQ浓度为100和500 μmol/L时, BiVO4表面COMPEITS成像图?[92].所有比例尺均为500 nm

Figure 5. (a) Schematic diagram of the procedures for laser-controlled shape modulation and single-molecule catalysis of gold nanostructures?[30]. Copyright 2019, Royal Society of Chemistry. (b) Oxidative reaction of HQ to Quinone. (c) 2D histogram of AR oxidation events for [HQ]=0 and 500 μmol/L. The white lines indicate the particle contour from SEM imaging. (d) COMPEITS images of BiVO4 surface corresponding to 100 and 500 μmol/L HQ, respectively[92]. All scale bars are 500 nm. Copyright 2020, American Chemical Society

图6. (a) AuTNP@SiO2的(111)晶面催化活性分布图. (b) AuTNP@SiO2的(111)晶面从中心到外围的径向催化活性[67]. (c)二维层状InSe表面光催化活性的局域映射图, 插图为InSe的明场成像图. (d) InSe中四种不同结构特征的催化速率分布直方图[97]

Figure 6. (a) Distribution of catalytic activity on the (111) facet of AuTNP@SiO2. (b) Distribution of the specific activities along the surface of the nanoplate, where r is the distance from the nanoplate center to the midpoint of the segment along the center-corner vector[67]. Copyright 2013, American Chemical Society. (c) Localization mapping of photocatalytic activities on 2D layered InSe, inset is the optical bright-field image. (d) Histogram distributions of turnover rates from four structural features from InSe[97]. Copyright 2021, American Association for the Advancement of Science

图7. (a) AuCM和AuCD单分子催化示意图[44]. (b)单个TiO2颗粒表面催化DN-BODIPY还原反应示意图. (c)同一个TiO2催化剂荧光成像(上)和透射电子显微镜(TEM)图像(下). TEM图像中的斑点表示(001)晶面和(101)晶面的荧光爆发位点[50]. 比例尺为4 μm. (d)从左到右依次是AuNBPs、aPt-AuNBPs和ePt-AuNBPs纳米结构的催化机制示意图[42].

Figure 7. (a) Scheme of the single-molecule catalysis from AuCM and AuCD[44]. Copyright 2022, Chinese Chemical Society. (b) Illustration of the DN-BODIPY reduction catalyzed by single TiO2 catalyst. (c) Fluorescence (upper) and TEM (lower) images of the same TiO2 catalyst. The spots in TEM image represent the location of fluorescence bursts on the (001) and (101) facets[50]. Scale bars: 4 μm. Copyright 2011, American Chemical Society. (d) Schematic diagram of the catalytic mechanism from AuNBPs, aPt-AuNBPs, and ePt-AuNBPs[42]. Copyright 2022, American Chemical Society

图8. (a) PdAu NP模型示意图. (b)激光辐射前后Pt-Au NR表面可能的反应路径[120]. (c) Au@AuAg NP (左)和Ag NP (右)催化反应机制示意图[43]

Figure 8. (a) Scheme of a typical PdAu NP. (b) Possible reaction pathway from Pt-Au NR surface before and after light irradiation[120]. Copyright 2020, American Chemical Society. (c) Schematic mechanism of a catalytic reaction on Au@AuAg NP (left) and Ag NP (right), respectively[43]. Copyright 2022, American Chemical Society

图9. (a)金纳米颗粒表面产物形成和脱附过程的能量图示[123]. (b) SiO2纳米颗粒催化RZ还原反应的基元化学步骤[124]. (c)光照条件下，AuNR催化AR氧化反应原理示意图. (d, e)中间产物和终产物生成过程多个纳米颗粒活化能的分布[125]

Figure 9. (a) Energy profile for product formation and dissociation steps on the surface of single Au nanoparticle[123]. Copyright 2016, American Chemical Society. (b) Elementarychemical steps of RZ reduction catalyzed by SiO2 nanoparticles[124]. Copyright 2019, American Chemical Society. (c) Schematic principles of AR oxidation catalyzed with AuNR under laser irradiation. (d, e) Distribution of activation energy Ea for the intermediate and final product formation process from multiple individual nanoparticles[125]. Copyright 2020, American Chemical Society

图10. (a)纳米催化剂以及单粒子单分子纳米催化装置示意图. (b)不同长度和孔径的纳米孔在单分子/单颗粒水平上的催化动力学[134]. (c)具有不同表面化学环境纳米孔中的催化动力学示意图, 孔隙分别用-SO3H(上)和-CF3(下)做亲水和疏水性修饰. (d)在亲水性(黑色)和疏水性(紫色)纳米孔中不同AR浓度下的产物脱附速率[136]

Figure 10. (a) Scheme of the nanocatalyst and single-molecule nanocatalysis setup. (b) Reaction kinetics from nanopores with different lengths and diameters at the single-molecule/particle level[134]. Copyright 2019, Nature Publishing Group. (c) Schematic diagram of the catalytic kinetics under hydrophilic (-SO3H, upper) and hydrophobic (-CF3, lower) chemical environments. (d) Reactant concentration [AR] dependence of dissociation rates in hydrophilic (black) and hydrophobic (violet) nanopores[136]. Copyright 2020, American Chemical Society

图11. 光诱导RZ歧化反应、AR脱乙酰基反应以及RZ脱氧反应

Figure 11. Photo-induced disproportionation reaction of RZ, a deacetylation reaction of AR, and a deoxygenation reaction of RZ

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单分子荧光成像研究单颗粒纳米催化机制

Nanocatalytic Mechanisms Investigated by Single Molecule Fluorescence Imaging at the Single-Particle Level

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