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1.
Faraday Discuss ; 2020 Nov 26.
Artigo em Inglês | MEDLINE | ID: mdl-33242050

RESUMO

As chemists and materials scientists, it is our duty to synthesize and utilize materials for a multitude of applications that promote the development of society and the well-being of its citizens. Since the inception of metal-organic frameworks (MOFs), researchers have proposed a variety of design strategies to rationally synthesize new MOF materials, studied their porosity and gas sorption performances, and integrated MOFs onto supports and into devices. Efforts have explored the relevance of MOFs for applications including, but not limited to, heterogeneous catalysis, guest delivery, water capture, destruction of nerve agents, gas storage, and separation. Recently, several start-up companies have undertaken MOF commercialization within industrial sectors. Herein, we provide a brief overview of the state of the MOF field from their design and synthesis to their potential applications, and finally, to their commercialization.

2.
J Am Chem Soc ; 2020 Nov 17.
Artigo em Inglês | MEDLINE | ID: mdl-33201702

RESUMO

Various metal oxide clusters upward of 8 atoms (Cu, Cd, Co, Fe, Ga, Mn, Mo, Ni, Sn, W, Zn, In, and Al) were incorporated into the pores of the metal-organic framework (MOF) NU-1000 via atomic layer deposition (ALD) and tested via high-throughput screening for catalytic isomerization and selective hydrogenation of propyne. Cu and Co were found to be the most active for propyne hydrogenation to propylene, and synergistic bimetallic combinations of Co and Zn, along with standalone Zn and Cd, were established as the most active for conversion to the isomerized product, propadiene. The combination of Co and Zn in NU-1000 diminished the propensity for full hydrogenation to propane as well as coking compared to its individual components. This study highlights the potential for high-throughput screening to survey monometallic and bimetallic cluster combinations that best affect the efficient transformation of small molecules, while discerning mechanistic differences in isomerization and hydrogenation by different metals.

3.
J Am Chem Soc ; 142(43): 18576-18582, 2020 Oct 28.
Artigo em Inglês | MEDLINE | ID: mdl-33048545

RESUMO

The encapsulation of enzymes within porous materials has shown great promise, not only in protecting the enzymes from denaturation under nonbiological environments, but also, in some cases, in facilitating their enzymatic reaction rates at favorable reaction conditions. While a number of hypotheses have been developed to explain this phenomenon, the detailed structural changes of the enzymes upon encapsulation within the porous material, which are closely related to their activity, remain largely elusive. Herein, the structural change of cytochrome c (Cyt c) upon encapsulation within a hierarchical metal-organic framework, NU-1000, is investigated through a combination of experimental and computational methods, such as electron paramagnetic resonance, solid-state ultraviolet-visible spectroscopy, and all-atom explicit solvent molecular dynamics simulations. The enhanced catalytic performance of Cyt c after being encapsulated within NU-1000 is supported by the physical and in silico observations of a change around the heme ferric active center.

4.
Artigo em Inglês | MEDLINE | ID: mdl-33030884

RESUMO

Ammonia (NH3) exposure has a serious impact on human health because of its toxic and corrosive nature. Therefore, efficient personal protective equipment (PPE) such as masks is necessary to eliminate and mitigate NH3 exposure risks. Because economically and environmentally viable conditions are of interest for large-scale manufacture of PPE, we herein report a benign procedure to synthesize a Zn-azolate metal-organic framework (MOF), MFU-4, for NH3 capture. The surface area and morphology of MFU-4 obtained in alcohol solvents at room temperature is consistent with that of traditionally synthesized MFU-4 in N,N-dimethylformamide at 140 °C. In addition to its large NH3 uptake capacity at 1 bar (17.7 mmol/g), MFU-4 shows outstanding performance in capturing NH3 at low concentration (10.8 mmol/g at 0.05 bar). Furthermore, the mild synthetic conditions implemented make it facile to immobilize MFU-4 onto cotton textile fiber. Enhanced NH3 capture ability of the MFU-4/fiber composite was also attributed to the well-exposed MOF particles. The benign synthetic MFU-4 procedure, high NH3 uptake, and easy integration onto fiber pave the way toward implementation of similar materials in PPE.

5.
J Am Chem Soc ; 142(43): 18554-18564, 2020 Oct 28.
Artigo em Inglês | MEDLINE | ID: mdl-32981316

RESUMO

Designing new materials for the effective detoxification of chemical warfare agents (CWAs) is of current interest given the recent use of CWAs. Although halogenated boron-dipyrromethene derivatives (4,4-difluoro-4-bora-3a,4a-diaza-s-indacene or BDP or BODIPY) at the 2 and 6 positions have been extensively explored as efficient photosensitizers for generating singlet oxygen (1O2) in homogeneous media, their utilization in the design of porous organic polymers (POPs) has remained elusive due to the difficulty of controlling polymerization processes through cross-coupling synthesis pathways. Our approach to overcome these difficulties and prepare halogenated BODIPY-based porous organic polymers (X-BDP-POP where X = Br or I) represents an attractive alternative through post-synthesis modification (PSM) of the parent hydrogenated polymer. Upon synthesis of both the parent polymer, H-BDP-POP, and its post-synthetically modified derivatives, Br-BDP-POP and I-BDP-POP, the BET surface areas of all POPs have been measured and found to be 640, 430, and 400 m2·g-1, respectively. In addition, the insertion of heavy halogen atoms at the 2 and 6 positions of the BODIPY unit leads to the quenching of fluorescence (both polymer and solution-phase monomer forms) and the enhancement of phosphorescence (particularly for the iodo versions of the polymers and monomers), as a result of efficient intersystem crossing. The heterogeneous photocatalytic activities of both the parent POP and its derivatives for the detoxification of the sulfur mustard simulant, 2-chloroethyl ethyl sulfide (CEES), have been examined; the results show a significant enhancement in the generation of singlet oxygen (1O2). Both the bromination and iodination of H-BDP-POP served to shorten by 5-fold of the time needed for the selective and catalytic photo-oxidation of CEES to 2-chloroethyl ethyl sulfoxide (CEESO).

6.
Artigo em Inglês | MEDLINE | ID: mdl-32909742

RESUMO

Constructing flexible metal-organic frameworks (MOFs) with targeted properties is of high interest given their demonstrated potential as smart materials that undergo structural transformations in response to external stimuli. Herein, we report a flexible and interpenetrated indium-based MOF, NU-50, comprising four-connected [In(CO2)4]- nodes and tetracarboxylate pyrene-based ligands assembled in the pts topology. The flexible framework of NU-50 exhibits intricate structural transformations upon exposure to external stimuli, namely, guest solvent molecules and elevated temperatures. The high density of pyrene moieties throughout the interpenetrated framework offers numerous sites for the adsorption of highly conjugated guest molecules such as atrazine via π-π interactions. As a result, NU-50 efficiently removes atrazine from water, achieving a maximum atrazine uptake capacity of 74 mg of atrazine per gram of NU-50. Molecular simulations reveal that the dynamic behavior of NU-50 involves the distortion of metal-ligand bonds, resulting in a narrow pore structure that affords effective adsorption of atrazine molecules in a sandwich-like geometry. Moreover, washing in acetone quickly regenerates the sorbent.

7.
J Am Chem Soc ; 142(41): 17224-17235, 2020 Oct 14.
Artigo em Inglês | MEDLINE | ID: mdl-32946693

RESUMO

Metal-organic frameworks (MOFs) are hybrid materials composed of metal ions and organic linkers featuring high porosity, crystallinity, and chemical tunability at multiple length scales. A recent advancement in transmission electron microscopy (TEM) and its direct application to MOF structure-property relationships have changed how we consider rational MOF design and development. Herein, we provide a perspective on TEM studies of MOFs and highlight the utilization of state-of-the-art TEM technologies to explore dynamic MOF processes and host-guest interactions. Additionally, we provide thoughts on what the future holds for TEM in the study of MOFs.

8.
Chem Soc Rev ; 49(20): 7406-7427, 2020 Oct 19.
Artigo em Inglês | MEDLINE | ID: mdl-32955065

RESUMO

Since the first reports of metal-organic frameworks (MOFs), this unique class of crystalline, porous materials has garnered increasing attention in a wide variety of applications such as gas storage and separation, catalysis, enzyme immobilization, drug delivery, water capture, and sensing. A fundamental feature of MOFs is their porosity which provides space on the micro- and meso-scale for confining and exposing their functionalities. Therefore, designing MOFs with high porosity and developing suitable activation methods for preserving and accessing their pore space have been a common theme in MOF research. Reticular chemistry allows for the facile design of MOFs from highly tunable metal nodes and organic linkers in order to realize different pore structures, topologies, and functionalities. With the hope of shedding light on future research endeavors in MOF porosity, it is worthwhile to examine the development of MOFs, with an emphasis on their porosity and how to properly access their pore space. In this review, we will provide an overview of the historic evolution of porosity and activation of MOFs, followed by a synopsis of the strategies to design and preserve permanent porosity in MOFs.

9.
ACS Appl Mater Interfaces ; 12(37): 41157-41166, 2020 Sep 16.
Artigo em Inglês | MEDLINE | ID: mdl-32852198

RESUMO

Gadolinium(III) nanoconjugate contrast agents (CAs) provide significant advantages over small-molecule complexes for magnetic resonance imaging (MRI), namely increased Gd(III) payload and enhanced proton relaxation efficiency (relaxivity, r1). Previous research has demonstrated that both the structure and surface chemistry of the nanomaterial substantially influence contrast. We hypothesized that inserting Gd(III) complexes in the pores of a metal-organic framework (MOF) might offer a unique strategy to further explore the parameters of nanomaterial structure and composition, which influence relaxivity. Herein, we postsynthetically incorporate Gd(III) complexes into Zr-MOFs using solvent-assisted ligand incorporation (SALI). Through the study of Zr-based MOFs, NU-1000 (nano and micronsize particles) and NU-901, we investigated the impact of particle size and pore shape on proton relaxivity. The SALI-functionalized Gd nano NU-1000 hybrid material displayed the highest loading of the Gd(III) complex (1.9 ± 0.1 complexes per node) and exhibited the most enhanced proton relaxivity (r1 of 26 ± 1 mM-1 s-1 at 1.4 T). Based on nuclear magnetic relaxation dispersion (NMRD) analysis, we can attribute the performance of Gd nano NU-1000 to the nanoscale size of the MOF particles and larger pore size that allows for rapid water exchange. We have demonstrated that SALI is a promising method for incorporating Gd(III) complexes into MOF materials and identified crucial design parameters for the preparation of next generation Gd(III)-functionalized MOF MRI contrast agents.

10.
Science ; 369(6505)2020 08 14.
Artigo em Inglês | MEDLINE | ID: mdl-32792370

RESUMO

Numerous redox transformations that are essential to life are catalyzed by metalloenzymes that feature Earth-abundant metals. In contrast, platinum-group metals have been the cornerstone of many industrial catalytic reactions for decades, providing high activity, thermal stability, and tolerance to chemical poisons. We assert that nature's blueprint provides the fundamental principles for vastly expanding the use of abundant metals in catalysis. We highlight the key physical properties of abundant metals that distinguish them from precious metals, and we look to nature to understand how the inherent attributes of abundant metals can be embraced to produce highly efficient catalysts for reactions crucial to the sustainable production and transformation of fuels and chemicals.

11.
Chem Commun (Camb) ; 56(72): 10409-10418, 2020 Sep 16.
Artigo em Inglês | MEDLINE | ID: mdl-32745156

RESUMO

Synthetic polymers are ubiquitous across both the industrial and consumer segments of the world economy. Catalysts enable rapid, efficient, selective, and even stereoselective, formation of desired polymers from any of a host of candidate monomers. While numerous molecular catalysts have been shown to be effective for these reactions, separation of the catalysts from reaction products is typically difficult - a potentially problematic complication that suggests instead the use of heterogeneous catalysts. Many of the most effective heterogeneous catalysts, however, comprise supported collections of reaction centres that are decidedly nonuniform in their composition, siting, and activity. Nonuniformity complicates atomic-scale evaluation of the basis for catalytic activity and thus impedes scientific hypothesis-driven understanding and development of superior catalysts. In view of the fundamental desirability of structural and chemical uniformity at the meso, nano, and even atomic scale, crystallographically well-defined, high-porosity metal-organic frameworks (MOFs) have attracted attention as model catalysts and/or catalyst-supports for a wide variety of chemical transformations. In the realm of synthetic polymers, catalyst-functionalized MOFs have been studied for reactions ranging from coordination-mediated polymerization of ethylene to visible-light initiated radical polymerizations. Nevertheless, many polymerization reactions remain to be explored - and, no doubt, will be explored, given the remarkable structural and compositional diversity of attainable MOFs. Noteworthy emerging studies include work directed toward more sophisticated catalytic schemes such as polymer templating using MOF pore architectures and tandem copolymerizations using MOF-supported reaction centres. Finally, it is appropriate to recognize that MOFs themselves are synthetic polymers - albeit, uncoventional ones.

12.
J Am Chem Soc ; 142(31): 13299-13304, 2020 Aug 05.
Artigo em Inglês | MEDLINE | ID: mdl-32678589

RESUMO

A thorium-organic framework (TOF-16) containing hexameric secondary building units connected by functionalized binaphthol linkers was synthesized, characterized, and irradiated to probe its radiation resistance. Radiation stability was examined using γ-rays and 5 MeV He2+ ions to simulate α particles. γ-irradiation of TOF-16 to an unprecedented 4 MGy dose resulted in no apparent bulk structural damage visible by X-ray diffraction. To further probe radiation stability, we conducted the first He2+ ion irradiation study of a metal-organic framework (MOF). Diffraction data indicate onset of crystallinity loss upon approximately 15 MGy of irradiation and total loss of crystallinity upon exposure to approximately 25 MGy of He2+ ion irradiation. The high radiation resistance observed suggests MOFs can withstand radiation exposure at doses found in nuclear waste streams and highlights the need for a systematic approach to understand and eventually design frameworks with exceptional radiation resistance.

13.
J Am Chem Soc ; 142(28): 12357-12366, 2020 Jul 15.
Artigo em Inglês | MEDLINE | ID: mdl-32614581

RESUMO

The expansion of manufacturing and commercial agriculture alongside rapid globalization have resulted in the widespread contamination of freshwater supplies with chemical toxins including persistent organic pollutants. Effective mitigation of such pollution is paramount to the safeguarding of human health, animal and aquatic life, and the environment. Currently, adsorption is the most economically viable water purification strategy. Owing to their crystallinity and modular nature, metal-organic frameworks (MOFs) are an excellent platform material for systematically investigating the physical and chemical properties which govern adsorption processes. X-ray diffraction techniques provide atomically precise descriptions of toxin-MOF interactions, while liquid-phase adsorption isotherms readily allow for the determination of uptake capacity and kinetics; however, determination of the thermodynamics of toxin-MOF interactions in aqueous media remains tedious. Herein, we add isothermal titration calorimetry (ITC) to our arsenal of techniques for characterizing adsorption mechanisms in MOFs. With this method, we are able to directly quantify the full thermodynamic profile of a chemical process (Ka, ΔG, ΔH, TΔS), providing critical details to support the rational design of next-generation sorbents. We demonstrate the suitability of ITC through our exploration of the parameter space of organophosphorus agrochemical adsorption in zirconium-based MOFs.

14.
Inorg Chem ; 2020 Jun 02.
Artigo em Inglês | MEDLINE | ID: mdl-32484338

RESUMO

When photoactivated, the uranyl ion is a powerful oxidant capable of abstracting hydrogen atoms from nonactivated C-H bonds. However, the highly reactive singly reduced [UVO2]+ intermediate is unstable with respect to disproportionation to the uranyl dication and insoluble tetravalent uranium phases, which limits the usage of uranyl ions as robust photocatalysts. Herein, we demonstrate that photoactivated uranyl ions can be stabilized by immobilizing and separating them spatially in a uranyl-organic framework heterogeneous catalyst, NU-1301. The visible-light-photoactivated uranyl ions in NU-1301 exhibited longer-lived U(V) and radicals than those in homogeneous counterparts, as evidenced by X-ray photoelectron spectroscopy and time-dependent electron paramagnetic resonance, leading to higher turnovers and enhanced stability for the fluorination of nonactivated alkanes.

15.
Artigo em Inglês | MEDLINE | ID: mdl-32543827

RESUMO

Four-carbon olefins, such as 1-butene and 1,3-butadiene, are important chemical feedstocks for the production of adhesives and synthetic rubber. These compounds are found in the C4 fraction of "green oil" products that can arise during the hydrogenation of acetylene. Here, we demonstrate that control of the catalyst structure increases the yield and productivity of these important olefins with a family of catalyst materials comprising Cu nanoparticles (CuNPs) bound within the pores of Zr-based metal-organic frameworks. Using carbon monoxide as a probe molecule, we characterize the surfaces of these catalytic CuNPs with diffuse reflectance infrared Fourier transform spectroscopy, revealing that the electronic structure of the CuNP surfaces is size-dependent. Furthermore, we find that as the CuNP diameter decreases, the selectivity for C4 products increases and that lowering the stoichiometric ratio of H2/acetylene improves the selectivity and productivity of the catalyst.

16.
Nat Commun ; 11(1): 2495, 2020 05 19.
Artigo em Inglês | MEDLINE | ID: mdl-32427872

RESUMO

Colloidal crystal engineering with nucleic acid-modified nanoparticles is a powerful way for preparing 3D superlattices, which may be useful in many areas, including catalysis, sensing, and photonics. To date, the building blocks studied have been primarily based upon metals, metal oxides, chalcogenide semiconductors, and proteins. Here, we show that metal-organic framework nanoparticles (MOF NPs) densely functionalized with oligonucleotides can be programmed to crystallize into a diverse set of superlattices with well-defined crystal symmetries and compositions. Electron microscopy and small-angle X-ray scattering characterization confirm the formation of single-component MOF superlattices, binary MOF-Au single crystals, and two-dimensional MOF nanorod assemblies. Importantly, DNA-modified porphyrinic MOF nanorods (PCN-222) were assembled into 2D superlattices and found to be catalytically active for the photooxidation of 2-chloroethyl ethyl sulfide (CEES, a chemical warfare simulant of mustard gas). Taken together, these new materials and methods provide access to colloidal crystals that incorporate particles with the well-established designer properties of MOFs and, therefore, increase the scope of possibilities for colloidal crystal engineering with DNA.


Assuntos
Coloides/química , DNA/química , Estruturas Metalorgânicas/química , Nanopartículas/química , Cristalização , DNA/genética , Engenharia/métodos , Microscopia Eletrônica de Transmissão e Varredura/métodos , Nanopartículas/ultraestrutura , Nanotubos/química , Nanotubos/ultraestrutura , Tamanho da Partícula , Espalhamento a Baixo Ângulo , Prata/química , Difração de Raios X
17.
Acc Chem Res ; 53(6): 1187-1195, 2020 06 16.
Artigo em Inglês | MEDLINE | ID: mdl-32401008

RESUMO

Metal-organic frameworks (MOFs) are a class of crystalline porous materials characterized by inorganic nodes and multitopic organic linkers. Because of their molecular-scale porosity and periodic intraframework chemical functionality, MOFs are attractive scaffolds for supporting and/or organizing catalysts, photocatalysts, chemical-sensing elements, small enzymes, and numerous other functional-property-imparting, nanometer-scale objects. Notably, these objects can be installed after the synthesis of the MOF, eliminating the need for chemical and thermal compatibility of the objects with the synthesis milieu. Thus, postsynthetically functionalized MOFs can present three-dimensional arrays of high-density, yet well-separated, active sites. Depending on the application and corresponding morphological requirements, MOF materials can be prepared in thin-film form, pelletized form, isolated single-crystal form, polycrystalline powder form, mixed-matrix membrane form, or other forms. For certain applications, most obviously catalytic hydrolysis and electro- or photocatalytic water splitting, but also many others, an additional requirement is water stability. MOFs featuring hexa-zirconium(IV)-oxy nodes satisfy this requirement. For applications involving electrocatalysis, charge storage, photoelectrochemical energy conversion, and chemiresistive sensing, a further requirement is electrical conductivity, as embodied in electron or hole transport. As most MOFs, under most conditions, are electrically insulating, imparting controllable charge-transport behavior is both a chemically intriguing and chemically compelling challenge.Herein, we describe three strategies to render zirconium-based metal-organic frameworks (MOFs) tunably electrically conductive and, therefore, capable of transporting charge on the few nanometers (i.e., several molecular units) to few micrometers (i.e., typical dimensions for MOF microcrystallites) scale. The first strategy centers on redox-hopping between periodically arranged, chemically equivalent sites, essentially repetitive electron (or hole) self-exchange. Zirconium nodes are electrically insulating, but they can function as grafting sites for (a) redox-active inorganic clusters or (b) molecular redox couples. Alternatively, charge hopping based on linker redox properties can be exploited. Marcus's theory of electron transfer has proven useful for understanding/predicting trends in redox-hopping based conductivity, most notably, in accounting for variations as great as 3000-fold depending on the direction of charge propagation through structurally anisotropic MOFs. In MOF environments, propagation of electronic charge via redox hopping is necessarily accompanied by movement of charge-compensating ions. Consequently, rates of redox hopping can depend on both the identity and concentration of ions permeating the MOF. In the context of electrocatalysis, an important goal is to transport electronic charge fast enough to match or exceed the inherent activity of MOF-based or MOF-immobilized catalysts.Bandlike electronic conductivity is the focus of an alternative strategy: one based on the introduction of molecular guests capable of forming donor-acceptor charge transfer complexes with the host framework. Theory again can be applied predictively to alter conductivity. A third strategy similarly emphasizes electronic conductivity, but it makes use of added bridges in the form of molecular oligomers or inorganic clusters that can then be linked to span the length of a MOF crystallite. For all strategies, retention of molecular-scale porosity is emphasized, as this property is key to many applications. Finally, while our focus is on Zr-MOFs, the described approaches clearly are extendable to other MOF compositions, as has already been demonstrated, in part, in studies by others.

18.
Artigo em Inglês | MEDLINE | ID: mdl-32469503

RESUMO

Covalent organic frameworks (COFs), materials constructed from organic building blocks joined by robust covalent bonds, have emerged as attractive materials in the context of electrochemical applications due to their high, intrinsic porosities and crystalline frameworks, as well as their ability to be tuned across two- and three-dimensions by the judicious selection of building blocks. Due to the recent and rapid development of this field, we have summarized COFs employed for electrochemical applications, such as batteries and capacitors, water splitting, solar cells, and sensors, with an emphasis on the structural design and resulting performance of the targeted electrochemical system. Overall, we anticipate this review will stimulate the design and synthesis of the next generation of COFs for use in electrochemical applications and beyond.

19.
Inorg Chem ; 2020 May 28.
Artigo em Inglês | MEDLINE | ID: mdl-32463656

RESUMO

Manganese complexes have attracted significant interest in chemical industries and academic research for their application as catalysts owing to their ability to attain a variety of oxidation states. Generally, sterically bulky ligands are required to isolate molecular homogeneous catalysts in order to prevent decomposition. Herein, we capitalize on the catalytic properties of Mn and circumvent the instability of these complexes through incorporation of Mn-atoms into porous crystalline frameworks, such as metal-organic frameworks (MOFs). MOFs are able to enhance the stability of these catalysts while also providing accessibility to the Mn sites for enhanced reactivity. We solvothermally synthesized two trinuclear Mn-based MOFs, namely [Mn3O(BDC)3(H2O)3]n (Mn-MIL-88, where H2BDC = benzene-1,4-dicarboxylic acid) and [Mn3O(BDC-Me4)3(H2O)3]n (Mn-MIL-88-Me4, where H2BDC-Me4 = 2,3,5,6-tetramethylterephthalic acid). Through comprehensive single-crystal X-ray diffraction, spectroscopic, and magnetic studies, we revealed that both MOFs are in a Mn(II/III) mixed-valence state instead of the commonly observed Mn(III) oxidation state. Furthermore, the use of a methylated linker (BDC-Me4) allowed access to permanent porosity in Mn-MIL-88-Me4, which is an analogue of the flexible MIL-88 family, yielding a catalyst for alcohol oxidation.

20.
J Am Chem Soc ; 142(20): 9363-9371, 2020 May 20.
Artigo em Inglês | MEDLINE | ID: mdl-32337982

RESUMO

We report the synthesis and characterization of the first plutonium metal-organic framework (MOF). Pu-UiO-66 expands the established UiO-66 series, which includes transition metal, lanthanide, and early actinide elements in the hexanuclear nodes. The thermal stability and porosity of Pu-UiO-66 were experimentally determined, and multifaceted computational methods were used to corroborate experimental values, examine inherent defects in the framework, decipher spectroscopic signatures, and elucidate the electronic structure. The crystallization of a plutonium chain side product provides direct evidence of the competition that occurs between modulator and linker in MOF syntheses. Ultimately, the synthesis of Pu-UiO-66 demonstrates adept control of Pu(IV) coordination under hydrolysis-prone conditions, provides an opportunity to extend trends across isostructural UiO-66 frameworks, and serves as the foundation for future plutonium MOF chemistry.

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