Research Progress on the Preparation of Metal-Organic Frameworks Encapsulated Metal Nanoparticle Composites and Their Catalytic Applications★

doi:10.6023/A23040146

Acta Chimica Sinica ›› 2023, Vol. 81 ›› Issue (6): 669-680.DOI: 10.6023/A23040146 Previous Articles Next Articles

Special Issue: 庆祝《化学学报》创刊90周年合辑

Review

金属有机骨架封装金属纳米粒子复合材料的制备及其催化应用研究进展^★

郑奉斌^a^,^b, 王琨^a^,^b, 林田^b^,^c, 王英龙^a^,^*(), 李国栋^b^,^d^,^*(), 唐智勇^b^,^d^,^*()

a 青岛科技大学化工学院青岛 266042
b 国家纳米科学中心纳米科学卓越创新中心中国科学院纳米系统与多级次制造重点实验室北京 100190
c 中国科学院大学化学科学学院北京 100049
d 中国科学院大学纳米科学与技术学院北京 100049

投稿日期:2023-04-20 发布日期:2023-05-25

作者简介:

郑奉斌, 青岛科技大学化工学院在读博士研究生, 目前在国家纳米科学中心联合培养, 研究方向为金属有机骨架及其复合材料的设计和制备以及其在催化选择性加氢中的应用.

王琨, 青岛科技大学化工学院在读博士研究生, 目前在国家纳米科学中心联合培养, 研究方向为金属有机骨架及其复合材料的设计和制备以及其在催化CO₂加氢中的应用.

林田, 中国科学院大学化学科学学院在读硕士研究生, 目前在国家纳米科学中心联合培养, 研究方向为金属有机骨架及其复合材料的设计和制备以及其在催化加氢脱氧中的应用.

王英龙, 青岛科技大学教授、博士生导师. 2000年和2003年分别于青岛科技大学获得学士学位和硕士学位, 2006年在中国海洋大学获得博士学位后任教于青岛科技大学. 研究工作主要集中于反应与分离过程的集成与强化、功能纳米材料催化与降解等方面, 主持国家自然科学基金3项. 获山东省科技进步一等奖、中国化工学会科技进步一等奖和第十九届中国专利优秀奖等9项省部级奖励, 2021年入选全球顶尖前10万科学家及2022年入选全球前2%顶尖科学家榜单.

李国栋, 国家纳米科学中心研究员, 博士生导师. 2004年于济南大学获得学士学位, 2007年于中国海洋大学获得硕士学位, 2011年于北京化工大学获得博士学位. 之后加入国家纳米科学中心工作, 期间在美国斯坦福大学进行访学. 研究工作主要集中在新型多孔纳米催化剂的结构设计、可控合成及其催化性能调控方面. 曾获国家自然科学基金委优秀青年基金资助, 获国家重点研发计划资助(课题负责人), 入选中科院青年创新促进会优秀会员.

唐智勇, 国家纳米科学中心研究员, 博士生导师, 科技部973(纳米重大研究计划)首席科学家, 国家自然科学基金委创新群体负责人, 国家杰出青年基金获得者. 1993和1996年分别于武汉大学获得学士学位和硕士学位, 2000年在中国科学院长春应用化学研究所获得博士学位. 之后, 在瑞士苏黎世联邦高等工业学院、美国密歇根大学进行博士后研究工作, 2006年回国加入国家纳米科学中心. 研究工作主要集中于功能无机纳米粒子组装体的构筑、功能调控及其在能源、催化中的应用研究. 入选科技部中青年科技创新领军人才、第二批国家“万人计划”科技创新领军人才、英国皇家化学会会士. 获得国家自然科学奖二等奖(第一完成人).

^★庆祝《化学学报》创刊90周年.

基金资助:
国家重点研发计划(2021YFA1500403); 国家重点研发计划(2021YFA1200302); 中国科学院战略性先导研究计划(XDB36000000); 国家自然科学基金(92056204); 国家自然科学基金(21890381); 国家自然科学基金(21721002); 国家自然科学基金(22173024); 国家自然科学基金(21722102); 以及中国科学院青年创新促进会的资助.

Research Progress on the Preparation of Metal-Organic Frameworks Encapsulated Metal Nanoparticle Composites and Their Catalytic Applications^★

Fengbin Zheng^a^,^b, Kun Wang^a^,^b, Tian Lin^b^,^c, Yinglong Wang^a(), Guodong Li^b^,^d(), Zhiyong Tang^b^,^d()

a College of Chemical Engineering, Qingdao University of Science and Technology, Qingdao 266042
b CAS Key Laboratory of Nanosystem and Hierarchical Fabrication, CAS Center for Excellence in Nanoscience, National Center for Nanoscience and Technology, Beijing 100190
c School of Chemical Science, University of Chinese Academy of Sciences, Beijing 100049
d School of Nanoscience and Technology, University of Chinese Academy of Sciences, Beijing 100049

Received:2023-04-20 Published:2023-05-25
Contact: *E-mail: wangyinglong@qust.edu.cn, liguodong@nanoctr.cn, zytang@nanoctr.cn
About author:
^★Dedicated to the 90th anniversary of Acta Chimica Sinica.
Supported by:
National Key Research and Development Program of China(2021YFA1500403); National Key Research and Development Program of China(2021YFA1200302); Strategic Priority Research Program of Chinese Academy of Sciences(XDB36000000); National Natural Science Foundation of China(92056204); National Natural Science Foundation of China(21890381); National Natural Science Foundation of China(21721002); National Natural Science Foundation of China(22173024); National Natural Science Foundation of China(21722102); and the Youth Innovation Promotion Association CAS.

Metal-organic frameworks (MOFs) are characteristic of high specific surface area, abundant metal nodes, diverse organic ligands, and ordered pore structure. More importantly, its composition and structure are easy to be designed and controlled, so it is very promising to become a new class of catalytic carrier materials. In recent years, the composites of metal nanoparticles encapsulated by MOFs have attracted great attention in the field of catalysis due to their unique structural features. However, more in-depth and systematic research is still needed in terms of its precise preparation and the relationship of the structure and catalytic performance. Based on above, the recent research progress on the preparation methods of metal nanoparticles encapsulated by MOFs and their catalytic applications are systematically summarizd. First, the synthesis methods of metal nanoparticles encapsulated by MOFs are summarized. Then, the catalytic applications are discussed in term of synergy among metal nanoparticles, pore structure, organic ligands or/and metal nodes of MOFs. Moreover, the relationships among active component, structure and their properties are illustrated. Finally, the challenges, opportunities and future development prospects of this research direction are discussed from the aspects of synthesis methods and catalytic applications.

Key words: metal-organic framework, metal nanoparticle, encapsulation, catalytic property, synergistic effect

Cite this article

Fengbin Zheng, Kun Wang, Tian Lin, Yinglong Wang, Guodong Li, Zhiyong Tang. Research Progress on the Preparation of Metal-Organic Frameworks Encapsulated Metal Nanoparticle Composites and Their Catalytic Applications^★[J]. Acta Chimica Sinica, 2023, 81(6): 669-680.

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Fig. & Tab. 12

Figure 1. Schematic illustration of (a) “ship-in-a-bottle” method, (b) “bottle-around-ship” method, (c) one-pot method, and (d) step-by-step method

Figure 2. (a) TEM image of Pt@MIL-101(Cr) (w=2%)[57], (b) low- magnification TEM image of PdCu@UiO-S@PDMS, (c) high-magnifi- cation TEM image of PdCu@UiO-S@PDMS and (d) elemental mapping images for PdCu@UiO-S@PDMS[7]

Figure 3. (a) TEM image of Au@MIL-100(Fe)[72], (b) TEM image of Au@MOF-808(Zr), (c) FT-IR spectra of treated Au@MOF-808(Zr) and PVP, and (d) a partial enlarged view of image c[75]

Figure 4. (a) Schematic diagram of the synthesis of Pd@NH2-UiO- 66(Zr), (b) TEM image of Pd@NH2-UiO-66(Zr) synthesized at 150 ℃ and the corresponding size distribution of Pd nanoparticles, (c) TEM image of Pd@NH2-UiO-66(Zr) synthesized at 90 ℃ and the corresponding size distribution of Pd nanoparticles[76], (d, e) TEM images of Au@BUT-17(Zr), and (f~i) EDX elemental mapping of the Au, Zr, C, and O in Au@BUT-17(Zr)[77]

Figure 5. (a) Schematic diagram of the synthesis of UiO-67(Zr)@Pd@UiO-X, (b) HAADF-STEM image of the cross-section of UiO-67(Zr)@Pd@UiO-67(Zr) (50 nm), (c) the enlarged image of the red rectangle in (b) and the corresponding EDX element mapping[78], (d) SEM image of Fe3O4@MIL-100(Fe)@Pt@MIL-100(Fe)@Pt@MIL-100(Fe)@Pt@MIL-100(Fe), (e) HAADF-STEM image of Fe3O4@MIL-100(Fe)@Pt@MIL- 100(Fe)@Pt@MIL-100(Fe)@Pt@MIL-100(Fe) and (f) EDX element mapping of Fe3O4@MIL-100(Fe)@Pt@MIL-100(Fe)@Pt@MIL-100(Fe) @Pt@MIL-100(Fe)[79]

合成方法	优点	缺点	影响因素
“瓶中造船”法	(1)孔限制生长超小纳米粒子 (2)高度的分散性 (3)抑制纳米粒子聚集	(1)难以精准控制纳米粒子的位置、组成和形态 (2)需要严格控制还原方法和还原条件	MOF的孔尺寸、还原剂、还原温度和时间
“瓶绕船”法	(1)实现单个或多个纳米粒子的封装 (2)纳米粒子的尺寸、形状和组成不受 MOF的影响	(1)表面活性剂阻碍纳米粒子活性位点的暴露 (2)在合成过程中MOF易自成核	表面活性剂、MOF的种类
一锅法	(1)合成过程简单 (2)降低生产成本和时间 (3)易于规模化生产	(1)纳米粒子和MOF的自成核生长 (2)难以控制MOF和纳米粒子的尺寸和组成	金属纳米粒子前驱体的种类、MOF前驱体的种类
逐步合成法	(1)纳米粒子在MOF中位置可控 (2)纳米形状、组成和尺寸不受MOF限制	(1)内核和壳的异质MOF需要精细控制反应参数 (2)合成步骤较繁琐	不同MOF的晶格参数、纳米粒子的种类

Table 1. Characteristics of different synthetic methods of metal nanoparticles encapsulated by MOF

Figure 6. (a) Catalytic reactions of Pt@AM1-UiO-66(Zr), Pt@AM3- UiO-66(Zr) and Pt@AM5-UiO-66(Zr) composites, (b) catalytic performance of Pt@NH2-UiO-66(Zr), Pt@AM1-UiO-66(Zr), Pt@AM3- UiO-66(Zr) and Pt@AM5-UiO-66(Zr)[80], (c) conversion and selectivity of CAL hydrogenation catalyzed by different catalysts and (d) schematic diagram of the window size of Al-TCPP and its steric hindrance effect on CAL molecules[81]

Figure 7. (a) Schematic diagram of the synthesis of Au@La-ZIF- 90(Zn)[82], (b) CO conversion curves of Pt@UiO-66(Zr), Pt@Br-UiO- 66(Zr) and Pt@Me2-UiO-66(Zr), and (c) NMR spectra of Pt@UiO-66(Zr), Pt@Br-UiO-66(Zr) and Pt@Me2-UiO-66(Zr)[84]

Figure 8. (a) Conversion of CAL on different catalysts and (b) selectivity of different catalysts to HCAL, HCOL and COL[85]

Figure 9. (a) Schematic diagram of the hydrogenation of citronellal catalyzed by Pt nanoparticles encapsulated in different MOFs[87] and (b) potential energy distribution of phenylacetylene (PA) hydrogenation on Pd(111)[78]

Figure 10. (a) Synergistic catalysis of Lewis acid sites and Pd nanoparticles in 1-OTf-PdNP and (b) stability test of 1-OTf-PdNP[88]

催化剂种类	合成方法	纳米粒子尺寸	反应类型	参考文献
Pt@AM3-UiO-66(Zr)	“瓶绕船”法	3 nm	三苯乙烯、反式-二苯乙烯和环辛烯的择形催化	[80]
MIL-88B(Fe)@Pt@Al-TCPP	逐步合成法	2.2 nm	肉桂醛选择性加氢制肉桂醇	[81]
Au@La-ZIF-90(Zn)	“瓶中造船”法	2.6 nm	3-硝基苯乙炔选择性氢化为3-氨基苯乙炔	[82]
Pd@F₅-MIL-101(Cr)	“瓶中造船”法	0.8~2 nm	三乙基硅烷脱氢生成三乙基硅烷醇	[83]
Pt@Me2-UiO-66(Zr)	“瓶绕船”法	7.9±1.0 nm	水煤气变换反应	[84]
Pt@HP-UiO-66(Zr)-0.8	“瓶绕船”法	8 nm	肉桂醛选择性加氢制肉桂醇	[85]
Cu@HOOC-UiO-66(Zr)	“瓶中造船”法	19.6±4.0 nm	CO₂加氢制甲醇	[86]
Pt@ZIF-67(Co)	“瓶绕船”法	2.9 nm	香茅醛的加氢反应	[87]
UiO-67(Zr)@Pd@UiO-67(Zr) (50 nm)	逐步合成法	3.5 nm	苯乙炔半加氢制苯乙烯	[78]
1-OTf-Pd^NP	“瓶中造船”法	≈5 nm	脱氢烷氧基化和加氢串联反应	[88]

Table 2. Summary of encapsulation of metal nanoparticles in MOFs for catalytic applications

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金属有机骨架封装金属纳米粒子复合材料的制备及其催化应用研究进展^★

Research Progress on the Preparation of Metal-Organic Frameworks Encapsulated Metal Nanoparticle Composites and Their Catalytic Applications^★

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金属有机骨架封装金属纳米粒子复合材料的制备及其催化应用研究进展★

Research Progress on the Preparation of Metal-Organic Frameworks Encapsulated Metal Nanoparticle Composites and Their Catalytic Applications★

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Knowledge

Abstract

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Fig. & Tab. 12

References 88

Related Articles 15

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金属有机骨架封装金属纳米粒子复合材料的制备及其催化应用研究进展^★

Research Progress on the Preparation of Metal-Organic Frameworks Encapsulated Metal Nanoparticle Composites and Their Catalytic Applications^★