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化学进展 2022, Vol. 34 Issue (9): 1911-1934 DOI: 10.7536/PC211101 前一篇   后一篇

• 综述 •

多功能核壳结构纳米反应器的构筑及其催化性能

陈浩, 徐旭, 焦超男, 杨浩, 王静*(), 彭银仙*()   

  1. 江苏科技大学环境与化学工程学院 镇江 212100
  • 收稿日期:2021-11-03 修回日期:2022-03-15 出版日期:2022-09-20 发布日期:2022-04-01
  • 基金资助:
    国家工业和信息化部船舶涂装排放治理及危废物处理技术与装备研发项目(MC-202003-Z01-07); 江苏省研究生科研与实践创新计划项目(KYCX20_3151)
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Fabrication of Multifunctional Core-Shell Structured Nanoreactors and Their Catalytic Performances

Hao Chen, Xu Xu, Chaonan Jiao, Hao Yang, Jing Wang(), Yinxian Peng()   

  1. School of Environmental and Chemical Engineering, Jiangsu University of Science and Technology,Zhenjiang 212100, China
  • Received:2021-11-03 Revised:2022-03-15 Online:2022-09-20 Published:2022-04-01
  • Contact: *e-mail: wangjingalice@just.edu.cn (Jing Wang);pyxhx@just.edu.cn (Yinxian Peng)
  • About author:
    †These authors contributed equally to this work.
  • Supported by:
    Discharge Control of Ship Painting and Hazardous Waste Treatment Technology and Equipment Program of the Ministry of Industry and Information Technology of China(MC-202003-Z01-07); Postgraduate Research & Practice Innovation Program of Jiangsu Province(KYCX20_3151)

随着纳米科学技术的不断发展,通过调节纳米材料的组成、结构、形貌以及尺寸等,已经能够实现对纳米材料性能调控的目的。为了进一步赋予纳米材料以新的功能,拓展其在材料、化学、生物和医学等领域的应用,开发能够同时实现多种功能的新型纳米材料是非常有意义的。多功能纳米材料的获得方法之一是通过对简单纳米粒子表面包覆具有功能性的材料来实现,形成的复合结构称为核壳结构。核壳结构的核和壳可以由相同或不同的材料组成。通过改变内核和外壳材料的组成、结构以及表面性质等,从而可以赋予核壳结构纳米材料以特殊的光、电、磁、催化、吸附以及生物活性等。在核壳结构的基础上对核与壳进行可控化与功能化的改造,可形成空心结构以及蛋黄壳结构(或称拨浪鼓结构),其中的空腔可作为高效纳米反应器应用于催化的各个分支领域。本综述首先讨论了不同核壳结构纳米反应器的设计,然后重点介绍了这些纳米反应器在催化降解染料污染物、催化加氢反应、催化氧化反应以及催化级联反应这几类反应中的应用。最后,对多功能核壳纳米反应器未来的研究和发展提出了一些展望。

关键词： 纳米反应器, 催化, 介孔硅, 贵金属纳米粒子, 过渡金属氧化物

With the development of nanotechnology, it has been possible to easily adjust the compositions, morphologies, and sizes of nanomaterials to control their properties. In order to endow nanomaterials with new functions and expand their applications in the fields of materials, chemistry, biology and medicine, it is very meaningful to develop new types of nanomaterials that can achieve multiple functions at the same time. One of the methods for obtaining multifunctional nanomaterials is achieved by coating the surface of simple nanoparticles with functional materials, and the resulting composite structure is called a core-shell structure. The core and shell of the core-shell structure can be composed of the same or different materials. By changing the compositions, structures and surface properties of the core and shell materials, the nanomaterials can be endowed with special optical, electrical, magnetic, catalytic, adsorption and biological activities. The hollow and yolk-shell structure can be formed by the controllable transformation of the core and the shell, in which the inner cavity can be used as a high-performance nanoreactor in various fields of catalysis. In this review, the design and application of core-shell structured nanoreactors with different structures in the field of catalysis are discussed, with emphases on the applications in catalytic degradation of dye pollutants, catalytic hydrogenation, catalytic oxidation, and catalytic cascade reactions. Finally, some prospects are put forward for the future research and development of multifunctional core-shell structured nanoreactors.

Contents

1 Introduction

2 Classification of core-shell structured nanoreactors

2.1 Traditional core-shell structure

2.2 Hollow core-shell structure

3 Application of core-shell nanoreactors in catalytic reactions

3.1 Catalytic degradation of dye pollutants

3.2 Catalytic hydrogenation

3.3 Catalytic oxidation

3.4 Catalytic cascade reaction

4 Conclusion and outlook

Key words: nanoreactor, catalysis, mesoporous silica, noble metal nanoparticles, transition metal oxide
()
图1 各种核壳纳米结构。(a)传统核壳结构,(b)去除部分壳形成的蛋黄壳结构,(c)去除部分核形成的蛋黄壳结构
Fig. 1 Various core-shell nanostructures. (a) Traditional core-shell nanostructure, (b) yolk-shell nanostructure formed by partial removal of shell, (c) yolk-shell nanostructure formed by partial removal of core
图2 各种类型的球形核壳纳米结构。 (a)含有单个或多个粒子的核,(b)具有不同形状的核,(c)具有不同类型的壳体
Fig.2 Various types of spherical core-shell structures. (a) Cores with single or multiple particles, (b) cores with different shapes, (c) shells of various types
图3 其他形状的核壳纳米结构, 包括(a)纳米管,(b)纳米立方体,(c)纳米十二面体,(d)纳米环
Fig. 3 Other shapes of core-shell nanostructures, including (a) nanotubes, (b) nanocubes, (c) dodecahedrons, (d) nanorings
表1 核壳结构纳米反应器
Table 1 Core-shell structured nanoreactors
Schematic diagram Structure Specialty
Core-shell Regular shape and stable performance
Yolk-shell Inner space facilitates the occurrence of various chemical reactions and inner core is easy to be functionalized
Multi-core yolk-shell Multiple small nano-sized catalyst particles in the shell are more advantageous than a relatively large nano-sized catalytic core
Mesoporous shell Very high specific surface area, regular pore structure, narrow pore size distribution, continuously adjustable pore size
Mesoporous multi-shell Pore size of the inner and outer shells is adjustable, which provides favorable conditions for shape-selective catalysis and helps to improve the selectivity
nanotube Large aspect ratio and surface area, the restricted space in the tube will increase the interaction between the substrate molecule and the active sites
图4 常见中空核壳结构。 (a, b) 多个核单个壳, (c) 蛋黄壳, (d) 多核蛋黄壳, (e)多层壳, (f)单个核多个壳, (g, h)多个核/壳
Fig. 4 Some common hollow core-shell structures. (a, b) multiple cores single shell, (c) yolk-shell, (d) multi-core yolk-shell, (e) multi shells, (f) single core multi shells, (g, h) multi-cores/shells
表2 用于费托合成反应的核壳结构纳米反应器
Table 2 Core-shell structured nanoreactors for Fischer-Tropsch synthesis reaction
Catalyst Reaction conditions CO conversion
CO (%)		 Hydrocarbon selectivity (mol%) ref
H2/CO T(K) p(MPa) CH4 C2-4 C5+ C5-12 C13+
Ru-PVP@SiO2 YSNs 2.0 423 3.0 20 1.8 3.7 86.9 63.8 23.1 89
WOM-0.45-Ru@SiO2 2.0 483 2.0 25 4.1 13.4 82.7 16.7 66 90
Co@SiO2-5 2.0 513 2.0 30 11.2 9.6 78.7 / / 91
Fe3O4@MnO2@HZSM-5 1.0 593 4.0 69.3 4.0 15.6 80.4 80.4a 0b 92
CoRu@HCS 2.0 493 1.0 18.3 37 14 49 / / 93
Co@HCS@Ru 2.0 493 1.0 12.4 21 8 71 / / 93
Co/SiO2@H-ZSM-5 2.0 533 1.0 11 12 12 76 72a 4b 94
R-Fe@H-ZSM-5 2.0 543 2.0 93 7.5 21.5 71 71a / 95
Fe3O4@H-ZSM-5 1.0 543 2.0 87 16 36.2 47.8 44.6 3.2 96
Co/Nanoβ-Zeolite 2.0 493 1.0 30.2 33.3 33c 26.2d / / 97
Co/TiO2 NTs 2.0 493 1.0 7.65 52.8 0.23 47.0 / / 98
Ru/meso-ZSM-5 1.0 533 2.0 29.6 5.9 14.6 79.5 79a 0.5b 99
Co/SiO2 2.0 493 2.0 80.6 8.7 11.3 80 62.4a / 100
Ru/HB-S 2.0 533 1.0 78.8 10.7 17.4 71.9 71.7a 0.3b 101
Co/NS-MFI 2.0 493 2.0 74 7.9 5.4 81 73.8a 7.2b 102
Co/Ce-meso-Y 1.0 523 2.0 34 11 6.6 82.4 74a 8.6b 103
图5 (a) 制备空心和蛋黄壳HSN的策略; (b) 硝基苯在不同催化剂下的加氢反应[110]
Fig. 5 (a) Strategy for preparing hollow and yolk-shell HSNs. (b) Hydrogenation of nitrobenzene with different catalysts[110]. Copyright 2020, American Chemical Society
图6 (a) 纳米反应器Gd2O3@Pt@ZIF的多步自组装图示[114]. (b) Gd2O3@ZIF-8和Gd2O3@Pt@ZIF-8 催化还原4-NP的紫外-可见光谱. (c) 纳米反应器Gd2O3@Pt@ZIF-8催化还原4-NP的循环性能
Fig. 6 (a) Multistep self-assembly illustration of preparation of the Gd2O3@Pt@ZIF nanoreactor[114]. (b) UV-vis spectra of the reduction of 4-NP with Gd2O3@ZIF-8 and with Gd2O3@Pt@ZIF-8. (c) The recycling of Gd2O3@Pt@ZIF-8 nanoreactor for the reduction of 4-NP. Copyright 2020, American Chemical Society
图7 (a) 具有有序微相分离结构的PS-b-P2VP粒子的TEM图像[120]; (b) 在无NIR照射以及在NIR照射下分别使用Au@PDA颗粒作为纳米反应器还原4-硝基苯酚的紫外-可见光谱; (c) PNIPAM/Au@meso-SiO2合成过程示意图[124]; (d) PNIPAM/Au@SiO2分别在30℃和50℃下催化还原4-硝基苯酚的转化率与时间的关系曲线
Fig. 7 (a) TEM images of a PS-b-P2VP particle with ordered microphase separation structure[120]. (b) UV-Vis spectra of the reduction of 4-nitrophenol using Au@PDA particles as nanoreactors without NIR irradiation at 39.3℃ and under NIR irradiation. (c) Schematic illustration for the synthesis process of PNIPAM/Au@meso-SiO2[124]. (d) Time-dependence conversion curves of reduction of 4-nitrophenol catalyzed by PNIPAM/Au@SiO2 at 30℃ and 50℃. Copyright 2012, American Chemical Society
表3 各种核壳结构纳米反应器在催化硝基芳烃化合物加氢反应中的应用
Table 3 The performances of nanoreactors with different core-shell structures in the hydrogenation of nitroaromatic compounds
Nanostructure Catalyst Reducing
substance		 Reduction conversion Rate constant
k (s-1)		 ref
Yolk-shell Co-N-C@SiO2 nitrobenzene >80%a 12.7 × 10-3 110
Yolk-shell Pt@SiO2-Ph nitrobenzene 99% / 113
Core-shell ZIF-8 Gd2O3@Pt@ZIF-8 4-nitrophenol >99.9%b / 114
Core-shell MOFs UiO-66-NH2@COP@Pd nitrobenzene >92% a 5.2 × 10-3 115
Hollow nanocapsules Pd@SiO2 NACs 4-nitrophenol >99%c / 116
Yolk-shell Pd/N-Cs@SnO2 4-nitrophenol >92%c 1 × 10-3 117
Core-shell Au triangular
nanoplates@SiO2		 4-nitrophenol >90%d 2.6 × 10-3 118
Core-shell Au-coated Fe3O4@SiO2 4-nitrophenol > 90% 7.5 × 10-4 119
Core-shell Au-coated Fe3O4@SiO2
(808 nm radiation)		 4-nitrophenol > 95% 3.4 × 10-3 119
Multi-compartment Au@PDA 4-nitrophenol >89.9% 1.9 × 10-5 120
Megranate-like Pd-silica nanorattles-SO3H 4-methoxy-nitrobenzene >98%c / 129
Megranate-like Ag@mSiO2 4-nitrophenol >90%c 13.8 × 10-3 130
Megranate-like Fe3O4@SiO2-Au@C 4-nitrophenol >95% a 11 × 10-3 19
multi-shelled MSNs Au@MMSNs 4-nitrophenol >95%c / 132
Yolk-shell Au@MgSiO3 4-nitrophenol >97%c 2.5 × 10-3 133
Yolk-shell YS-Au@Ph-PMOs 4-nitrophenol >88%a 5 × 10-3 134
Yolk-shell YS-Au@SiO2 4-nitrophenol / 2 × 10-3 134
Hollow doughnut Ag/Hd-MSN-NH2 4-nitrophenol >97%a 4.1 × 10-3 135
图8 (a) 多功能两亲纳米反应器的制备示意图[141]; (b) 4-甲氧基苄醇在不同催化剂下的有氧氧化动力学曲线; (c) PIL@SiO2-Pd纳米反应器的合成路线示意图[143]; (d) 通过三个连续步骤构筑Y@HWS-TiO2的总体流程图[146]; (e) 在紫外和可见光条件下C-TiO2、Y@S-TiO2、Y@WS-TiO2和Y@HWS-TiO2结构对选择性氧化苯甲醇的光催化活性比较
Fig. 8 (a) Schematic illustration for the preparation of multifunctional amphiphilic nanoreactor[141]; (b) Kinetic plots of aerobic oxidation of 4-methoxybenzyl alcohol over different catalysts. Copyright 2018, American Chemical Society; (c) Schematic illustration of the synthetic route to the PIL@SiO2-Pd nanoreactor[143]. Copyright 2015, American Chemical Society; (d) Overall flowchart for the fabrication of the Y@HWS-TiO2 via three sequential steps[146]; (e) Comparison of photocatalytic activity of C-TiO2, Y@S-TiO2, Y@WS-TiO2 and Y@HWS-TiO2 structures in selective oxidation of benzyl alcohol under UV and visible conditions
图9 (a) 由AuPt@RF@SiO2气溶胶粒子得到分散在有序介孔二氧化硅微球中的AuPt纳米合金蛋黄壳结构空心粒子[150]; (b)苯乙烯的转化率和氧化苯乙烯的选择性与反应时间的关系
Fig. 9 (a) Formation of AuPt nanoalloy yolk@shell hollow particles in ordered mesoporous silica microspheres from AuPt@RF@SiO2 aerosol particles[150]. (b) Conversion of styrene and selectivity to styrene oxide at different reaction times. Copyright 2016, American Chemical Society
图10 Co3O4 (a)、CeO2@Co3O4 (b)和CeO2 (c) 的 TEM图像; (d) 以Co3O4、CeO2@Co3O4、CeO2为催化剂时甲苯的转化率[156]; (e) Pd/h-NiCoOx和NiCoOx纳米片的构筑示意图[158]; (f) 不同Pd负载量下的h-NiCoOx样品的催化活性; (g) PtxRuy/ZrO2纳米复合物的合成示意图[159]; (h) 在不同催化剂作用下甲苯转化率与反应温度的关系
Fig. 10 TEM images of Co3O4 (a), CeO2@Co3O4 (b), CeO2 (c). (d) Toluene conversion over Co3O4, CeO2@Co3O4, CeO2[156]. Copyright 2020, American Chemical Society. (e) A schematic illustration of the fabrication of Pd/h-NiCoOx and NiCoOx nanosheets[158]. (f) The catalytic activities of h-NiCoOx samples with different Pd loadings. Copyright 2020, American Chemical Society. (g) Schematic illustration for synthesizing PtxRuy/ZrO2 nanocomposites[159]. (h) Toluene conversion as a function of reaction temperature over different catalysts. Copyright 2020, American Chemical Society
图11 (a) 用于全身给药癌症协同治疗的聚合物纳米反应器的制备示意图[168]; (b) 随时间G@R-NRs和G@N-NRs产生H2O2的情况; (c) 经过24 h孵育后, 分别在葡萄糖存在与否下, Fe/G@R-NRs和Fe/G@NNRs释放Fe2/3+的情况
Fig. 11 (a) Schematic illustration for preparation of polymersome nanoreactors for cooperative cancer therapy via systemic administration[168]. (b) Time-dependent H2O2 production of G@R-NRs and G@N-NRs. (c) Fe2/3+ release from Fe/G@R-NRs and Fe/G@NNRs in the absence or presence of glucose after 24 h incubation. Copyright 2019, American Chemical Society
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