Ligand‐Directed Strategy for Zeolite‐Type Metal–Organic Frameworks: Zinc(<scp>II</scp>) Imidazolates with Unusual Zeolitic Topologies

Huang, Xiao‐Chun; Lin, Yan‐Yong; Zhang, Jie‐Peng; Chen, Xiaoming

doi:10.1002/ange.200503778

Cited by 332 publications

(136 citation statements)

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“…Just like single crystals and optical ceramics, increasing the block size with high optical quality is always a great challenge for many materials. Here, we show that by simply slowing down the solvent evaporation rate, nanocrystals of the prototypical MOF SOD-[Zn(mim) 2 ] (MAF-4/ZIF-8 [17,18], Hmim = 2-methylimidazole, Fig. 2) with the cubic crystal symmetry can fuse at room temperature to form large transparent blocks.…”

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confidence: 94%

Room-temperature sintered metal-organic framework nanocrystals: A new type of optical ceramics

Zhou

Wang

et al. 2018

Sci. China Mater.

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Ceramic is a rigid material consisting of an infinite threedimensional network of sintered non-oriented inorganic, non-metallic crystalline grains, which are generally nontransparent. If the inner light scatter is eliminated, ceramics can become transparent or optical ceramics [1,2]. With great potentials in optical windows, sensors and lasers, optical ceramics have received great attentions since 1950s [1]. As the gain medium of solid-state lasers, optical ceramics can combine the advantages of large size, high transparency, high mechanical and thermal stabilities, and ease for dispersing the luminous atoms and groups [3]. For comparison, single-crystal gain mediums can suffer high power density but are difficult to grow into large size, while glasses and polymers have reversed characteristics.To make ceramics transparent, the inner pore and impurity should be minimized to zero, which requires highly pure, nanosized, and very uniform crystallite precursors as well as complicated fusing technology ( Fig. 1) [4,5]. The cubic crystal symmetries (absence of the birefringence which causes extremely high scattering losses) are generally required for the crystallites of optical ceramics, meaning that only a few inorganic materials can be used. Besides, ceramics sintering usually operates above 1000 o C, which excludes organic and organic-inorganic hybrid materials [1].Porous coordination polymers (PCPs) or metal-organic frameworks (MOFs) are crystalline materials consisting of metal ions and organic ligands, which have captured widespread attentions for adsorption, catalysis, sensing, optics [6] and also laser gain mediums [7][8][9][10][11]. As can be seen in membranes and photonic crystals [12,13], MOF nanocrystals may merge to form seamless microscopic blocks under mild conditions [14][15][16]. Nevertheless, macroscopic and optical transparent blocks of MOF nanocrystals/microcrystals are still unknown so far. Just like single crystals and optical ceramics, increasing the block size with high optical quality is always a great challenge for many materials. Here, we show that by simply slowing down the solvent evaporation rate, nanocrystals of the prototypical MOF SOD-[Zn(mim) 2 ] (MAF-4/ZIF-8 [17,18], Hmim = 2-methylimidazole, Fig. 2) with the cubic crystal symmetry can fuse at room temperature to form large transparent blocks. After doping laser dye, this metal-organic optical ceramic (MOOC) can show the amplified spontaneous emission (ASE) with a very low energy-density threshold.MAF-4 nanocrystals with uniform size (ca. 20 nm) can be easily synthesized by reaction of Zn(NO 3 ) 2 and Hmim in methanol or ethanol at room temperature (Fig. S1). Compared with the commonly used solvent methanol [19], ethanol is nontoxic and more environment-friendly. After centrifugation and washed, the residual nanocrystals and solvent form a white gel-like (semi-fluidic) block.

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confidence: 94%

Room-temperature sintered metal-organic framework nanocrystals: A new type of optical ceramics

Zhou

Wang

et al. 2018

Sci. China Mater.

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“…33 First, the separation of oil from water requires PCPs to be water stable. Although some water-stable PCPs have been developed, [34][35][36][37][38][39][40] most PCPs are actually sensitive toward moisture. Second, PCPs need to have hydrophobic surfaces to prevent the entry of water molecules into the pores.…”

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confidence: 99%

Coating sponge with a hydrophobic porous coordination polymer containing a low-energy CF3-decorated surface for continuous pumping recovery of an oil spill from water

et al. 2016

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For the remediation of oil spills and organic solvent leakage into water, it is desirable to develop not only advanced sorbents with a high adsorption capability but also labor-and time-saving apparatuses that can work continuously without human intervention. In this work, we synthesized a novel and highly stable porous coordination polymer (PCP, also called metal-organic framework), University of Science and Technology of China-6 (USTC-6), with a corrugated -CF 3 surface that features high hydrophobicity. The uniform growth of USTC-6 throughout a graphene oxide (GO)-modified sponge was achieved and yielded a macroscopic USTC-6@GO@sponge sorbent, which repels water and exhibits a superior adsorption capacity for diverse oils and organic solvents. Remarkably, the sorbent can be further assembled with tubes and a self-priming pump to build a model apparatus that affords consecutive and efficient oil recovery from water. The easy and fast recovery of oils/organic solvents from water based on such an apparatus indicates that it has great potential for future water purification and treatment.

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“…Due to its high porosity and excellent resistance to pressure, temperature and steam, ZIF-8 has been extensively studied for applications in carbon sequestration and is also one the four metal-organic frameworks being manufactured commercially (Basolite Z1200) [17][18][19][20][21][22][23][24][25] . Crystallization of ZIF-8 from solution has been explored by several groups 26,27 , and a non-porous polymorph of ZIF-8 with a diamondoid (dia) topology was recently reported 28,29 .…”

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In situ X-ray diffraction monitoring of a mechanochemical reaction reveals a unique topology metal-organic framework

et al. 2015

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Chemical and physical transformations by milling are attracting enormous interest for their ability to access new materials and clean reactivity, and are central to a number of core industries, from mineral processing to pharmaceutical manufacturing. While continuous mechanical stress during milling is thought to create an environment supporting nonconventional reactivity and exotic intermediates, such speculations have remained without proof. Here we use in situ, real-time powder X-ray diffraction monitoring to discover and capture a metastable, novel-topology intermediate of a mechanochemical transformation. Monitoring the mechanochemical synthesis of an archetypal metal-organic framework ZIF-8 by in situ powder X-ray diffraction reveals unexpected amorphization, and on further milling recrystallization into a non-porous material via a metastable intermediate based on a previously unreported topology, herein named katsenite (kat). The discovery of this phase and topology provides direct evidence that milling transformations can involve short-lived, structurally unusual phases not yet accessed by conventional chemistry.

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Ligand‐Directed Strategy for Zeolite‐Type Metal–Organic Frameworks: Zinc(II) Imidazolates with Unusual Zeolitic Topologies

Cited by 332 publications

References 38 publications

Room-temperature sintered metal-organic framework nanocrystals: A new type of optical ceramics

Room-temperature sintered metal-organic framework nanocrystals: A new type of optical ceramics

Coating sponge with a hydrophobic porous coordination polymer containing a low-energy CF3-decorated surface for continuous pumping recovery of an oil spill from water

In situ X-ray diffraction monitoring of a mechanochemical reaction reveals a unique topology metal-organic framework

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