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According to XRD results, the printed objects retained the original crystal structure of HKUST-1 upon formulation. A certain peak broadening was observed for all materials, suggesting small MOF crystals. Indeed, as confirmed by SEM, the shaped objects were composed of HKUST-1 crystals with sizes in the 20–50 nm range. However, a significant decrease of the S BET was measured, from 1850 m 2 g −1 for the parent powder to 1134 m 2 g −1 for the 3D-printed solids. As no binder was present, this decrease might be ascribed to the partial collapse of the HKUST-1 framework. L. Wang, M. Zheng and Z. Xie, Nanoscale metal–organic frameworks for drug delivery: a conventional platform with new promise, J. Mater. Chem. B, 2018, 6, 707–717, 10.1039/C7TB02970E.

Typically, MOFs are produced in polycrystalline powder form, with the size of individual crystals ranging from several tens of nanometers to a few microns. Continuous studies on synthesis optimization and product characterization have stimulated the production of MOFs on a larger scale. Thus, a number of them are now commercially available and provided by BASF (HKUST-1/Basolite C300, ZIF-8/Basolite Z1200, Fe-BTC/Basolite F300), Strem Chemicals (CAU-10, MIL-53(Al), MIL-101(Al), PCN-250(Fe), UiO-66), and others. Linker codes: BDC – benzene-1,4-dicarboxylic acid; BTB – 1,3,5-benzenetribenzoate; MIM – 2-methyl imidazole; MIC – 4-methyl-5-imidazolecarboxaldehyde; BTC – benzene-1,3,5-tricarboxylic acid; DHBDC – 2,5-dihydroxy-1,4-benzenedicarboxylic acid; BPDC – biphenyl-4,4′-dicarboxylic acid; and FA – formic acid. Binder codes: PVA – polyvinyl alcohol; SB – pseudoboehmite; and PVB – polyvinyl butyral. “—” not specified. a Used as an additive to improve thermal conductivity. The process parameters entirely depend on the initial powder to be shaped. Mainly, the pressure applied on it should be carefully selected to avoid the complete destruction of the crystal structure (amorphization) and therefore loss of intrinsic properties. Additionally, the rate of pressure increase should be adequate for the same reason. a Attrition tests were performed by rotating a cylinder containing a baffle and the shaped UiO-66-COOH at 60 rpm for 30 min. The percentage corresponds to the total mass of the fine particles – less than 425 μm – after sieving. For those outside of France, the hospitality industry, or both, the initials MOF may not ring a bell, but those three letters hold an incredible amount of significance. To be a “Meilleur Ouvrier de France” or "Best Craftsman of France" as you'll soon discover, is a very prestigious title indeed. Here's how it happens.As is evident from Table 13, both extrusion and DIW can yield shaped objects while preserving the textural properties of pristine MOFs. The loss in surface area in the case of the 3D printed objects is somewhat higher than the binder content which is due to the presence of the plasticizer. The final printed objects have a developed network of millimeter-sized channels thanks to the layer-by-layer deposition upon printing. This can significantly improve the diffusion of gas or liquid within the shaped objects. Spray-drying The spray-drying technique has been known for over a century. As the name suggests, it is used to dry powder-like materials in a continuous fashion. Compared with ovens and conveyor belts, spray-dryers allow treating several tons per hour of wet product. Over the past few decades, the application potential of spray-drying has considerably expanded and now includes the food industry, 125 the pharmaceutical industry, 126 and many others. 127 Less than 10,000 people have ever won the right to call themselves one of the Best Craftsmen in France. MOF winners retain their title for life. Many choose to join the National Society of Meilleur Ouvrier de France, a sort of alumni society for winners. The title is taken so seriously that sporting such a collar fraudulently is a crime punishable by prison-time. Generally, extruders are divided into screw and piston types. The former allows continuous processing and might consist of one (single screw), two (twin screw) or multiple screws which operate in simultaneous and parallel rotations. On the other hand, piston extruders operate in batch mode; however, they enable the extrusion of pastes with high viscosity and compaction.

Granulation is the last industrially-mature technology reviewed herein, and allows producing millimeter-sized grains. Two types of granulation techniques are typically discussed: wet granulation, when powders are aggregated in a high-shear rate mixer in the presence of a solvent; and dry granulation, when grains are obtained from a previously shaped object either mildly crushed and sieved, or spheronized. Due to higher stresses applied, the dry granulation implies more severe losses in the initial physicochemical properties of the MOFs, while the wet granulation has a less pronounced effect and therefore might be more adequate. Especially, replacing water with another solvent with a lower surface tension is highly beneficial. The MOF competition and its preparation are definitely in my top lifetime memories. The hours of preparation, the stress of the competition, the recognition for all the work and commitment, have alla All has changed me forever. I have pushed myself beyond what I imagined possible and it certainly contributed in making me a better professional.” continues Meilleur Ouvrier de France Chef Thomas Marie The culinary connection In 2014 Ahmed et al. 156 proposed a different method for MOF shaping based on controlled freezing. According to it, a MOF powder in suspension can be shaped into monoliths upon controlled freezing of the solvent with its subsequent elimination via freeze-drying. The authors applied this methodology to obtain Cu-based HKUST-1 monoliths. For this, the MOF precursors were dissolved in DMSO and left for 24 h at 80 °C. After that, the solution was frozen in liquid nitrogen for 1 min and placed into a freeze-dryer to sublime the solvent. This procedure yielded highly crystalline HKUST-1 monoliths as confirmed by XRD. Moreover, the specific surface area was 870 m 2 g −1 with characteristics of both micropores and mesopores, as visible from the N 2 physisorption isotherms. Additionally, as shown by Hg intrusion, the monoliths exhibited macropores with diameters around 0.4 and 10 μm. Importantly, these macropores generated upon ice-templating were oriented in one particular direction due to the orientational growth of ice crystals during freezing. Lastly, the authors showed that the size of these macropores could be varied by altering the freezing temperature. Thus, upon freezing at 5 °C the macropores were two times bigger (∼50 μm) than the macropores generated upon freezing at −80 and −20 °C (32 and 25 μm, respectively).and their applications as anodes in lithium and sodium ion batteries, Coord. Chem. Rev., 2019, 388, 172–201, DOI: 10.1016/j.ccr.2019.02.029. Y. H. Hu and L. Zhang, Amorphization of metal–organic framework MOF-5 at unusually low applied pressure, Phys. Rev. B: Condens. Matter Mater. Phys., 2010, 81, 174103, DOI: 10.1103/PhysRevB.81.174103. J. J. Purewal, D. Liu, J. Yang, A. Sudik, D. J. Siegel, S. Maurer and U. Mu, Increased volumetric hydrogen uptake of MOF-5 by powder densification, Int. J. Hydrogen Energy, 2012, 37, 2723–2727, DOI: 10.1016/j.ijhydene.2011.03.002. Jean-Philippe Dacquin obtained his PhD from the Université Sciences et Technologies de Lille 1 (France) in 2008. After two postdoctoral years at the Cardiff Catalysis Institute following the University of York with Karen Wilson and Adam F. Lee, he returned to the University of Lille where he holds a position of Associate Professor. He's the administrative head of the bachelor of Chemistry and teaches courses on inorganic chemistry and analytical chemistry. His research is devoted to the preparation of solid catalysts with controlled porosity and their application in environmental catalysis.