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

doi:10.6023/A23040147

Acta Chimica Sinica ›› 2023, Vol. 81 ›› Issue (8): 1002-1014.DOI: 10.6023/A23040147 Previous Articles Next Articles

Review

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)

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

Cite this article

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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Fig. & Tab. 11

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

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)

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

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

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

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

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

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

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

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

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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