Selective CO<sub>2</sub> Capture and High Proton Conductivity of a Functional Star‐of‐David Catenane Metal–Organic Framework

Huang, Yiding; Wu, Shu Qi; Deng, Wei Hua; Xu, Gang; Hu, Fa Lu; Hill, Jonathan P.; Wei, Wei; Su, Shengqun; Shrestha, Lok Kumar; Sato, Osamu; Wu, Ming Yan; Hong, Min-Chun; Ariga, Katsuhiko

doi:10.1002/adma.201703301

Cited by 41 publications

(6 citation statements)

References 53 publications

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“…The proton conductivity increased from 3.47 × 10 –3 S cm –1 at 30 °C to a maximum value of 1.33 × 10 –2 S cm –1 at 70 °C (Table S3). Remarkably, the room-temperature proton conductivity (3.47 × 10 –3 S cm –1 at 30 °C and 100% RH) and the best conductivity (1.33 × 10 –2 S cm –1 at 70 °C and 100% RH) of 1 surpassed most of the previously reported water-assisted proton-conducting MOF materials. − To understand further the proton transport mechanism, we evaluated the activation energy by fitting the temperature-variable proton conductance with Arrhenius equation σ T = A exp( E a / k B T ), where σ, E a , k B , and A represent the proton conductivity, activation energy, Boltzmann constant, and pre-exponential factor, respectively. The E a of 1 was 0.34 (Figure d), indicating that the proton conduction of 1 follows a Grotthuss mechanism (hydrogen bond mediated, generally E a < 0.4 eV) rather than a vehicle mechanism (transfer of H 3 O + molecular, generally E a > 0.5 eV). , …”

Section: Resultsmentioning

confidence: 99%

Ultra-Stable Metal–Organic Framework with Concurrent High Proton Conductivity and Fluorescence Sensing for Nitrobenzene

Liao

Dong

et al. 2021

Chem. Mater.

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Luminescent metal−organic frameworks (MOFs) coupled with proton conduction offer wide applications in clean energy and luminescence sensors. High stability and remarkable proton conductivity and sensing are requisites for practical applications. Specifically, high thermal and chemical stabilities under harsh conditions are important but challenging to achieve. Herein, an ultra-stable Cu(I)-tetrazolate MOF, NaCu 3 (mtz) 4 (1, mtz = 5-methyltetrazolate), was prepared. It possesses a 3D framework with 1D channels and exhibits outstanding thermal and chemical stabilities under various conditions, including water, organic solvents, and acidic and basic solutions of wide pH range. The compound exhibits strong green emissions, which can be ascribed to metal-toligand charge transfer, and selective fluorescence sensing for pollutant nitrobenzene. Moreover, compound 1 presents a high proton conductivity of over 10 −2 S cm −1 at 70 °C and 100% relative humidity. In 1, abundant uncoordinated nitrogen atoms on the pore walls act as H-bonding acceptors to achieve its high proton conductivity under waterassisted conditions. The compound is an unprecedented water-dependent proton conductor of the tetrazole-based MOF, providing a new avenue to design robust and high-performance proton-conductive MOFs.

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Section: Resultsmentioning

confidence: 99%

Ultra-Stable Metal–Organic Framework with Concurrent High Proton Conductivity and Fluorescence Sensing for Nitrobenzene

Liao

Dong

et al. 2021

Chem. Mater.

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“…The use of solid based adsorption processes has been considered as an alternative as it can offer ease of operation with much less health hazard, and the regeneration of adsorbent is inexpensive and reasonably quick. An array of porous materials has been tried as adsorbents for CO 2 capture including zeolites, metal organic frameworks (MOFs), − amine-modified porous organic polymers, mesoporous carbon nitrides, porous carbons, and solid amine-based adsorbents . For industrial scale application, the selection of an adsorbent is strongly influenced not only by its ability to capture a large quantity of CO 2 but also the cost involved in the synthesis of adsorbent, the ease of availability of the raw materials, and the operational costs.…”

Section: Introductionmentioning

confidence: 99%

High-Performance Biomass-Derived Activated Porous Biocarbons for Combined Pre- and Post-Combustion CO₂ Capture

Singh

Lakhi

Ramadass

et al. 2019

ACS Sustainable Chem. Eng.

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This paper demonstrates the synthesis of highly efficient activated porous biocarbons through chemical activation of Lotus seed for pre- and postcombustion CO2 capture. The activation was performed at three different temperatures using four different KOH/biomass impregnation ratios. The synthesized materials are ultramicroporous and display bimodal porosity which can be easily controlled by varying the experimental conditions. The specific surface area can be tuned from 1079 m2 g–1 to 2230 m2 g–1 by adjusting the amount of activating agent and the carbonization temperature. The optimized material with the highest surface area (2230 m2 g–1) and pore volume (0.96 cm3 g–1) showed a simultaneous high promise for both low pressure (6.8 mmol g–1 at 1 bar/0 °C) and high pressure (26.4 mmol g–1 at 30 bar/0 °C) CO2 capture, which is extremely difficult to achieve for any CO2 sorbent and has never been reported before. This exceptional performance is attributed to ultramicroporosity, high surface area, and surface-oxygenated functional groups. Heat of adsorption (30.4 kJ mol–1) value suggests that adsorption is physical in nature and accounts for easier material regeneration. These multiple merits underline the importance of synthesized materials in the field of CO2 capture and potential for various other environmental applications.

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“…Inspired by such a unique hexagonal structure, the so-called “Star of David” shaped molecules are of special attention in supramolecular chemistry. Although a number of such hexagonal metallo-architectures with organic linkers were reported, no nanosized metal aggregate shaped like a “Star of David” has been reported . Fascinatingly, the center of this molecular hexagon is hollow and the 3D packing of 1 is porous (Figure S9).…”

Section: Resultsmentioning

confidence: 99%

The Gigantic {Ni₃₆Gd₁₀₂} Hexagon: A Sulfate-Templated “Star-of-David” for Photocatalytic CO₂ Reduction and Magnetic Cooling

et al. 2020

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Gigantic coordination molecules assembled from a large number of metal ions and organic ligands are structurally and functionally challenging to characterize. Here we show that a heterometallic cluster [Ni36Gd102(OH)132(mmt)18(dmpa)18(H2dmpa)24(CH3COO)84(SO4)18(NO3)18(H2O)30]·Br6(NO3)6·(H2O) x ·(CH3OH) y , (1, x ≈ 130, y ≈ 60), shaped like a “Star of David”, can be synthesized using a “mixed-ligand” and “sulfate-template” strategy. In terms of metal nuclearity number, 1 is the second largest 3d–4f cluster to date. In the solid state, 1 is porous after removing the lattice guests. The N2 adsoption experiment reveals that the BET and Langmuir surface areas are 299.8 and 412.0 cm2 g–1, respectively. CO2 adsorption at 298 K gives the amount of 45 cm3 g–1 for 1. More importantly, 1 is soluble in common organic solvents and exhibits high solution stability revealed by high resolution MALDI-TOF mass spectroscopy, small-angle X-ray scattering (SAXS), and low-dose transmission electron microscopy. The solubility and the potential open metal sites owing to the labile coordinating components prompted us to investigate the photocatalytic properties of 1, which displays high selectivity and efficiency for reduction of CO2 to CO with turnover number and turnover frequency of 29700 and 1.2 s–1, respectively. These values are higher than most catalysts working under the same conditions, presumably due to the strong Ni–CO2 binding effect. In addition, the large percentage of Gd(III) in 1 leads to a large magnetic entropy change (41.3 J·kg–1·K–1) at 2.0 K for ΔH = 7 T.

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Selective CO₂ Capture and High Proton Conductivity of a Functional Star‐of‐David Catenane Metal–Organic Framework

Cited by 41 publications

References 53 publications

Ultra-Stable Metal–Organic Framework with Concurrent High Proton Conductivity and Fluorescence Sensing for Nitrobenzene

Ultra-Stable Metal–Organic Framework with Concurrent High Proton Conductivity and Fluorescence Sensing for Nitrobenzene

High-Performance Biomass-Derived Activated Porous Biocarbons for Combined Pre- and Post-Combustion CO₂ Capture

The Gigantic {Ni₃₆Gd₁₀₂} Hexagon: A Sulfate-Templated “Star-of-David” for Photocatalytic CO₂ Reduction and Magnetic Cooling

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Selective CO2 Capture and High Proton Conductivity of a Functional Star‐of‐David Catenane Metal–Organic Framework

Cited by 41 publications

References 53 publications

Ultra-Stable Metal–Organic Framework with Concurrent High Proton Conductivity and Fluorescence Sensing for Nitrobenzene

Ultra-Stable Metal–Organic Framework with Concurrent High Proton Conductivity and Fluorescence Sensing for Nitrobenzene

High-Performance Biomass-Derived Activated Porous Biocarbons for Combined Pre- and Post-Combustion CO2 Capture

The Gigantic {Ni36Gd102} Hexagon: A Sulfate-Templated “Star-of-David” for Photocatalytic CO2 Reduction and Magnetic Cooling

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Product

Resources

About

Selective CO₂ Capture and High Proton Conductivity of a Functional Star‐of‐David Catenane Metal–Organic Framework

High-Performance Biomass-Derived Activated Porous Biocarbons for Combined Pre- and Post-Combustion CO₂ Capture

The Gigantic {Ni₃₆Gd₁₀₂} Hexagon: A Sulfate-Templated “Star-of-David” for Photocatalytic CO₂ Reduction and Magnetic Cooling