Challenges and Opportunities in Preserving Key Structural Features of 3D-Printed Metal/Covalent Organic Framework

doi:10.1007/s40820-024-01373-w

Abstract

Abstract:

Metal-organic framework (MOF) and covalent organic framework (COF) are a huge group of advanced porous materials exhibiting attractive and tunable microstructural features, such as large surface area, tunable pore size, and functional surfaces, which have significant values in various application areas. The emerging 3D printing technology further provides MOF and COFs (M/COFs) with higher designability of their macrostructure and demonstrates large achievements in their performance by shaping them into advanced 3D monoliths. However, the currently available 3D printing M/COFs strategy faces a major challenge of severe destruction of M/COFs’ microstructural features, both during and after 3D printing. It is envisioned that preserving the microstructure of M/COFs in the 3D-printed monolith will bring a great improvement to the related applications. In this overview, the 3D-printed M/COFs are categorized into M/COF-mixed monoliths and M/COF-covered monoliths. Their differences in the properties, applications, and current research states are discussed. The up-to-date advancements in paste/scaffold composition and printing/covering methods to preserve the superior M/COF microstructure during 3D printing are further discussed for the two types of 3D-printed M/COF. Throughout the analysis of the current states of 3D-printed M/COFs, the expected future research direction to achieve a highly preserved microstructure in the 3D monolith is proposed.

Key words: Metal-organic frameworks, Covalent organic frameworks, 3D printing, Microstructure, Monolith

Ximeng Liu, Dan Zhao, John Wang. Challenges and Opportunities in Preserving Key Structural Features of 3D-Printed Metal/Covalent Organic Framework[J]. Nano-Micro Letters, 2024, 16(1): 157-.

Ximeng Liu, Dan Zhao, John Wang. [J]. Nano-Micro Letters, 2024, 16(1): 157-.

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URL: https://www.qk.sjtu.edu.cn/nml/EN/10.1007/s40820-024-01373-w

https://www.qk.sjtu.edu.cn/nml/EN/Y2024/V16/I1/157

Figures/Tables 9

Fig. 1 a Illustration of different 3D printing technologies. b Illustration of reasons contributing to the current challenges for 3D-printed M/COF monoliths

Fig. 2 a Illustration of the two types of 3D-printed M/COF monolith. b Number of published works in terms of different applications. c Distribution of reported values on surface area, compressive strength, and M/COF loading mass in the published works about 3D-printed M/COF. The red dash line is the 5th degree polynomial fitting curve

Fig. 3 a Illustration of three types of M/COF pastes. b Comparison of different properties among the three M/COF pastes. c Viscosity of pastes formulated with 35 wt% (green) and 51 wt % (red) of CPL-1 MOF (left), and viscosity plots of a pure HEC solution (black), and HKUST-1-based pastes formulated with 11 wt% of large crystals (red) and with 16 wt% of nanocrystals (green) (right). Reprinted from Ref. [13] Copyright 2020, American Chemical Society. d Photographs of CPL-1-based monolith printed under the same conditions with pastes formulated with 35 wt% (left) and 51 wt% (right) of CPL-1. Reprinted from Ref. [13] Copyright 2020, American Chemical Society. e Stress and strain curves of pure P, E, T, U and 2/3 T + 1/3E 3D-printed materials (dotted lines) and their MOF-based composites (solid lines). Reprinted from Ref. [37] Copyright 2021, Royal Society of Chemistry. f Photograph images showing the gel state of PUG-ZIF-8 composite bioinks at 25 °C and the sol state at 37 °C. Reprinted from Ref. [25] Copyright 2021, American Chemical Society. g Viscosity plot and the photo of MOF-74@Torlon paste. Reprinted from Ref. [39] Copyright 2020, American Chemical Society. h Illustration of meniscus-guided 3D printing of HKUST-1. Reprinted from Ref. [55] Copyright 2022, American Chemical Society. i Synthesis route of 3D-TpPa-1 through Pluronic F127-templated coassembly followed by postprinting framework reorganization. Inset: a robust 3D-TpPa-1 cubic lattice loaded with a 100 g weight. Reprinted from Ref. [56] Copyright 2019, American Chemical Society. (Color figure online)

Fig. 4 a Representation of MIL-53(Al)-NH₂ structure in the open pore configuration, where AlO₆ are indicated as green polyhedra, and gray and navy dots are carbon and nitrogen atoms, respectively (top); the schematic of the modification of MIL-53(Al)-NH₂ structure with methyl methacrylic anhydride (bottom). Reprinted from Ref. [37] Copyright 2021, Royal Society of Chemistry. b Schematic for the in-situ synthesis of ZIF-L in TOCNF. Reprinted from Ref. [57] Copyright 2023, Royal Society of Chemistry. c Schematic of the preparation of ZIF67-PA12 nanocomposite powders. Reprinted from Ref. [59] Copyright 2020, The Authors. Published by Elsevier B.V. d Schematic of HKUST-1 monolith formulation by novel GPG technique. Reprinted from Ref. [60] Copyright 2020, American Chemical Society. e N₂ physisorption isotherms for DIW monolith, HKUST-1 powder, and 120 °C-synthesized samples washed in acetone solvents. Reprinted from Ref. [60] Copyright 2020, American Chemical Society. f Four-channel droplet microfluidic synthesis of E-BP/ZIF-67 (Inset: optical images of E-BP, E-BP/Co²⁺ and E-BP/ZIF-67 microdroplets). Reprinted from Ref. [51] Copyright 2021, Wiley‐VCH GmbH. g Images of MIL-53@ABS film and MIL-53 particle patterns in the MIL-53@ABS film. Reprinted from Ref. [61] Copyright 2020, Elsevier B.V

Fig. 5 a Appearance of binder-free 3D printed COF using different drying substrate. Reprinted from Ref. [63] Copyright 2020 Elsevier B.V. b Schematic of the drying mechanism of 3D-printed monoliths on porous and non-porous substrates. Reprinted from Ref. [63] Copyright 2020, Elsevier B.V. c CO₂ and N₂ adsorption curve of SNW-1 monolith, SNW-1 powder, and SNW-1/F127 monolith at 273 K. Reprinted from Ref. [63] Copyright 2020, Elsevier B.V. d Formation processes for pre- and post-impregnated MIL-101 monoliths. Reprinted from Ref. [64] Copyright 2019, American Chemical Society. e N₂ physisorption isotherms for TEPA-MIL-101 powder, 3D monolith with pre-penetrated MOF, and 3D monolith with post-treatment. Reprinted from Ref. [64] Copyright 2019, American Chemical Society

Fig. 6 a Schematic of the two different M/COF covering methods. b Schematic of the pZIF-8 nanoMOFs attaching to the substrate. Reprinted from Ref. [87] Copyright 2021, Elsevier Ltd. c Strategies employed to immobilize active nanoparticles on the plasma-treated PLA support. Reprinted from Ref. [81] Copyright 2020, American Chemical Society. d Schematic of the preparation of pZIF-8 and SBS-QCSC substrate. Reprinted from Ref. [88] Copyright 2022, Royal Society of Chemistry. e in situ MOF growth and encapsulation process. Reprinted from Ref. [92] Copyright 2020, WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim

Fig. 7 a Schematic of the construction of the COF on 3D-printed COOH-modified nanocarbon electrodes. Reprinted from Ref. [93] Copyright 2022, American Chemical Society. b Preparing of ZIF 8 and ZIF 8-Ag coating on Ti₆AlV₄ sheet. Reprinted from Ref. [94] Copyright 2022, Jilin University. c SEM observation of an ABS filter coated with ZnO. Reprinted from Ref. [71] Copyright 2020, The Korean Society of Industrial and Engineering Chemistry. d Schematic of the preparation of ZIF-8 and ZnO-NP composite filaments for FDM 3D printing; the monolith obtained by conversion of ZnO to ZIF-8 shows better malachite green removal ability. Reprinted from Ref. [72] Copyright 2021, Elsevier Ltd. e SEM images of the 3D-printed hydrogel samples; the HKUST-1 is grown both at the outer and core regions. Reprinted from Ref. [70] Copyright 2020, American Chemical Society

Table 1 State-of-the-arts 3D printed M/COFs

Materials	Loadings (wt%)	Surface area (m² g⁻¹)	Compressive strength (MPa)	Type
3D-printed UTSA-16(Co) [38]	85	568 (Powder: 727)	0.56	Mixed monolith
3DP ZIF-8-ZnO@TOCNF [34]	70	2330	NA
3DP MOF-74/Torlon [39]	13	80 (Powder: 1180)	637
3DP HKUST-1 [55]	100	1192	NA
Mg-MOF 74@3DP Ti [85]	NA	NA	71.42	Covered monolith
UTSA-16@3DP Kaolin [78]	90	620	4.75	Covered monolith

Fig. 8 Proposed future development directions

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