Water-Stable Metal–Organic Frameworks for Fast and High Dichromate Trapping via Single-Crystal-to-Single-Crystal Ion Exchange

Fu, Hong-Ru; Xu, Zhong-Xuan; Zhang, Jian

doi:10.1021/cm503767r

Cited by 301 publications

(134 citation statements)

References 60 publications

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“…Ion-exchange reactions were extensively investigated and identified in nanometric materials such as chalcogenides [10][11][12] and metal organic frameworks. 13,14 All-inorganic perovskite CsPbX 3 (X = Cl, Br, I) nanocrystals have shown very swift halide exchange, simply by mixing two compositions in solution. 15 These reactions average the halide content in a matter of minutes and give path for bright emitters that are tunable across the visible spectrum.…”

Section: Introductionmentioning

confidence: 99%

First evidence of macroscale single crystal ion exchange found in lead halide perovskites

Efrati

Aharon

Wierzbowska

et al. 2020

EcoMat

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Ion exchange is classified as a reaction that may be performed among nanocrystals. Here, we discovered that methylammonium lead bromide macroscale perovskite single crystals may exchange ions with the environment while maintaining their original morphology. Iodide replaced bromide and was detected even in the very center of a previously pure macroscale MAPbBr3 single crystal. Additionally, the entrance of chloride into the crystal is energetically favorable and most bromides were exchanged, yet kinetic factors hindered Cs+ entry and Pb2+ by Sn2+ substitution. Furthermore, grinding different single crystals together revealed swift I/Br exchange. Clear differences in comparison with nanomaterials, along with density functional theory calculations, shed light on the nature of ion‐exchange reactions in perovskite single crystals. This work provides first evidence of these halide exchange reactions in macroscale perovskite single crystals. These results offer a new perspective on ion‐exchange reaction and pave a path toward synthesis of inhomogeneous single crystals.

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Section: Introductionmentioning

confidence: 99%

First evidence of macroscale single crystal ion exchange found in lead halide perovskites

Efrati

Aharon

Wierzbowska

et al. 2020

EcoMat

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“…Emerging as a new class of functional materials, metal organic frameworks (MOFs), [28][29][30][31][32][33] which feature tailorable structures, exceptional properties, [34][35][36][37][38][39][40][41] have been proposed to be promising materials to meet the dual challenge of CO 2 capture and conversion for the following reasons: (a) the porous MOFs can significantly absorb CO 2 , 42-45 (b) the well ordered porous structures can enrich substrates and facilitate the accessibility of substrates to active sites, (c) the metal ions can serve as Lewis acid sites to efficiently activate epoxide, [46][47][48][49] …”

Section: Introductionmentioning

confidence: 99%

3d-4f Heterometal–Organic Frameworks for Efficient Capture and Conversion of CO₂

Qiao

Cheng

et al. 2017

Crystal Growth & Design

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Two novel three-dimensional 3d-4f heterometallic-organic frameworks {[TbZn(BPDC) 2 (µ 2 -H 2 O)Cl(H 2 O) 3 ]·5H 2 O·0.5DMA} n (1) and {[TbCo(BPDC) 2 (µ 2 -H 2 O)Cl(H 2 O) 3 ]·8H 2 O·0.5DMA} n (2) have been synthesized and structurally characterized. Theyare isostructural and exhibit irregular one-dimensional channels with large potential pore volume.Importantly, both of them demonstrate excellent catalytic activity for the chemical fixation of CO 2 into cyclic carbonates under mild conditions. Moreover, the catalytic recycling of compound 1 as a representative example was explored, it can be easily separated and reused for at least four times without significant reduction in catalytic ability.

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“…[2] Recent advances in MOFs have opened opportunities for developing P-MOFs. PC refers to proactive blocking of metal coordination sites to preclude their occupation by neutralizing ligands such as OH À .…”

mentioning

confidence: 99%

“…[2] Recent advances in MOFs have opened opportunities for developing P-MOFs. [1] In nature,C PMs (for example,z eolites) usually have an anionic framework.…”

mentioning

confidence: 99%

Framework Cationization by Preemptive Coordination of Open Metal Sites for Anion‐Exchange Encapsulation of Nucleotides and Coenzymes

et al. 2016

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Cationic frameworks can selectively trap anions through ion exchange,a nd have applications in ion chromatography and drug delivery.However,cationic frameworks are muchr arer than anionic or neutral ones.H erein, we propose ac oncept, preemptive coordination (PC), for targeting positively charged metal-organic frameworks (P-MOFs). PC refers to proactive blocking of metal coordination sites to preclude their occupation by neutralizing ligands such as OH À . We use 20 MOFs to showt hat this PC concept is an effective approach for developing P-MOFs whose high stability, porosity,and anion-exchange capability allowimmobilization of anionic nucleotides and coenzymes,i na ddition to chargeand size-selective capture or separation of organic dyes.T he CO 2 and C 2 H 2 uptake capacity of 117.9 cm 3 g À1 and 148.5 cm 3 g À1 ,respectively,at273 Kand 1atm, is exceptionally high among cationic framework materials.Crystalline porous materials (CPMs) with exchangeable ions are useful for many ion-exchange applications,s uch as pollutant extraction. [1] In nature,C PMs (for example,z eolites) usually have an anionic framework. Cationic framework materials with anion exchange capability are desired for av ariety of applications,s uch as removal of toxic ClO 4 À and AsO 4 3À ,s eparation of nucleotides and amino acids,o r immobilization of anionic pharmaceuticals. [2] Recent advances in MOFs have opened opportunities for developing P-MOFs. [3] In fact, cationic frameworks were among the earliest MOFs to be studied. [4] Examples include those formed by Cu + (or Ag + )and neutral linkers,such as 4,4'bipyridine.H owever,t hese P-MOFs have limited structural variety and low stability.O ne promising method for creating stable P-MOFs is to use clusters. [5] But not all cluster types are suitable,because of the extra attached negative ligands owing to the increased node connectivity,a swell as the trapping of simple anions,such as O 2À ,can make the overall charge of the cluster neutral or negative.Itisthe ratio between neutral and negative ligand groups that plays apivotal role in the overall charge of acluster.Synthetic strategies capable of controlling this ratio are thus desirable.An analysis shows that both tetrameric [Zn 4 O(RCOO) 6 ] and dimeric M 2 (RCOO) 4 (solvent) 2 clusters usually form neutral MOFs. [6] In comparison, trigonal planar trimers could give ap ositive cluster,s uch as [M 3 O(RCOO) 6 L 3 ] + , when all of the Mi ons are trivalent and all of the Ld onor groups are neutral. [7] There are,h owever, two pitfalls that could neutralize trimers:t he inclusion of M 2+ or the occupation of one Ls ite by an anionic ligand (such as OH À ). [8,9] To overcome the neutralizing effect of M 2+ ,t he simplest solution is to employ metal ions (such as In 3+ )t hat are unlikely to exist as M 2+ .H owever,i ti sa dvantageous to use transition metal ions because of their desirable properties, such as low cost, low toxicity,a nd high stability for applications in aqueous environments.P revious studies on trimers with ions such as Co...

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Water-Stable Metal–Organic Frameworks for Fast and High Dichromate Trapping via Single-Crystal-to-Single-Crystal Ion Exchange

Cited by 301 publications

References 60 publications

First evidence of macroscale single crystal ion exchange found in lead halide perovskites

First evidence of macroscale single crystal ion exchange found in lead halide perovskites

3d-4f Heterometal–Organic Frameworks for Efficient Capture and Conversion of CO₂

Framework Cationization by Preemptive Coordination of Open Metal Sites for Anion‐Exchange Encapsulation of Nucleotides and Coenzymes

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Water-Stable Metal–Organic Frameworks for Fast and High Dichromate Trapping via Single-Crystal-to-Single-Crystal Ion Exchange

Cited by 301 publications

References 60 publications

First evidence of macroscale single crystal ion exchange found in lead halide perovskites

First evidence of macroscale single crystal ion exchange found in lead halide perovskites

3d-4f Heterometal–Organic Frameworks for Efficient Capture and Conversion of CO2

Framework Cationization by Preemptive Coordination of Open Metal Sites for Anion‐Exchange Encapsulation of Nucleotides and Coenzymes

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3d-4f Heterometal–Organic Frameworks for Efficient Capture and Conversion of CO₂