Amine-Grafted MIL-101(Cr) via Double-Solvent Incorporation for Synergistic Enhancement of CO<sub>2</sub> Uptake and Selectivity

Zhong, Rui; Yu, Xiaofeng; Meng, Wei; Liu, Jia; Zhi, Chenxu; Zou, Ruqiang

doi:10.1021/acssuschemeng.8b03597

Cited by 52 publications

(21 citation statements)

References 62 publications

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“…S11, the derived Q st value for MIL-101(Cr) (19 kJ mol −1 ) at low surface coverage is quite accordance with the existing literature 48,49 . Upon RHA incorporation, the Q st value was increased slightly for RHA-MIL-101(Cr)-I (20 kJ mol −1 ) and RHA-MIL-101(Cr)-II (30 kJ mol −1 ) at low surface coverage, attributed to the strong electrostatic interaction for CO 2 with narrow pore size distribution 49 . Notably, the Q st value of RHA-MIL-101(Cr) is at par with the several established MOF based composites available in the literature (Table S3).…”

Section: Resultssupporting

confidence: 87%

In situ casting of rice husk ash in metal organic frameworks induces enhanced CO2 capture performance

Panda

Saini

Kumar

et al. 2020

Sci Rep

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Incorporation of rice-husk-ash (RHA), an agricultural waste, in situ during the synthesis of MIL-101(Cr) resulted in a significant improvement in the CO2 adsorption properties over the synthesized RHA-MIL-101(Cr). The newly synthesized RHA-MIL-101(Cr) composite exhibited an enhancement of 14–27% in CO2 adsorption capacity as compared to MIL-101(Cr) at 25 °C and 1 bar. The content of RHA incorporated in RHA-MIL-101(Cr) fine tuned the CO2 capture performance to achieve high working capacity (0.54 mmol g−1), high purity (78%), superior CO2/N2 selectivity (18) and low isosteric heat of adsorption (20–30 kJ mol−1). The observed superior CO2 adsorption performance of RHA-MIL-101(Cr) is attributed to the fine tuning of textural characteristics—enhancement of 12–27% in BET surface area, 12–33% in total pore volume and 18–30% in micropore volume—upon incorporation of RHA in MIL-101(Cr).

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Section: Resultssupporting

confidence: 87%

In situ casting of rice husk ash in metal organic frameworks induces enhanced CO2 capture performance

Panda

Saini

Kumar

et al. 2020

Sci Rep

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“…Except for its distinct merits such as large pore volume, high BET surface area, and excellent stability in water, MIL-101 also contains numerous potential open chromium sites (up to 3.0 mmol/g) (Hwang et al, 2008) with an unoccupied orbital that are expected to anchor amine functionalization via a strong binding interaction with the positive nitrogen atoms. It is also demonstrated that amine-functionalized MIL-101 has high CO 2 capture capacities (Lin et al, 2013; Yan et al, 2013; Hu et al, 2014; Lin J.-L. et al, 2014; Cabello et al, 2015; Darunte et al, 2016; Huang et al, 2016; Emerson et al, 2018; Zhong et al, 2018; Liu et al, 2019). Thus, in our work, MIL-101(Cr) was fabricated and modified with a series of amines to achieve the efficient storage of CO 2 substrate.…”

Section: Introductionmentioning

confidence: 99%

Sequential Co-immobilization of Enzymes in Metal-Organic Frameworks for Efficient Biocatalytic Conversion of Adsorbed CO2 to Formate

Wen

Tan

et al. 2019

Front. Bioeng. Biotechnol.

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The main challenges in multienzymatic cascade reactions for CO2 reduction are the low CO2 solubility in water, the adjustment of substrate channeling, and the regeneration of co-factor. In this study, metal-organic frameworks (MOFs) were prepared as adsorbents for the storage of CO2 and at the same time as solid supports for the sequential co-immobilization of multienzymes via a layer-by-layer self-assembly approach. Amine-functionalized MIL-101(Cr) was synthesized for the adsorption of CO2. Using amine-MIL-101(Cr) as the core, two HKUST-1 layers were then fabricated for the immobilization of three enzymes chosen for the reduction of CO2 to formate. Carbonic anhydrase was encapsulated in the inner HKUST-1 layer and hydrated the released CO2 to HCO3-. Bicarbonate ions then migrated directly to the outer HKUST-1 shell containing formate dehydrogenase and were converted to formate. Glutamate dehydrogenase on the outer MOF layer achieved the regeneration of co-factor. Compared with free enzymes in solution using the bubbled CO2 as substrate, the immobilized enzymes using stored CO2 as substrate exhibited 13.1-times higher of formate production due to the enhanced substrate concentration. The sequential immobilization of enzymes also facilitated the channeling of substrate and eventually enabled higher catalytic efficiency with a co-factor-based formate yield of 179.8%. The immobilized enzymes showed good operational stability and reusability with a cofactor cumulative formate yield of 1077.7% after 10 cycles of reusing.

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“…Further FT‐IR spectra prove the existence of organic molecules in the framework, as the distinct C‐N adsorption peak can be observed (Figure S5, Supporting Information). [ 18 ] Element analyses of C and N were conducted to compare the quantity of different Lewis bases in the framework: The calculated molar ratios of Cr 3+ /Lewis base are 1.23, 1.73, and 3.15 for MIL‐101(Cr)‐imidazole, MIL‐101(Cr)‐DETA, and MIL‐101(Cr)‐PEHA, respectively. From the TGA results (Figure S6, Supporting Information), the weight loss below 100 °C is due to the elimination of free guest molecules, and the coordinated H 2 O molecules on metal clusters in the MOFs will be eliminated only at higher temperature (100–200 °C).…”

Section: Resultsmentioning

confidence: 99%

Molecular‐Scale Interface Engineering of Metal–Organic Frameworks toward Ion Transport Enables High‐Performance Solid Lithium Metal Battery

Wang

Guo

et al. 2020

Adv Funct Materials

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Metal-organic frameworks (MOFs) have drawn considerable interest as solid electrolytes (SEs) by virtue of their talents for rational design as ion channels. The crystal interface plays a significant role in ion transport and is thus of vital importance to the performance of solid batteries, however, interface effects of MOFs in SEs are not yet fully understood, especially at the molecular level, and not engineered as well. In this work, MOFs engineered with diverse molecules (Lewis bases) are designed for an optimized interfaces and the impact of interfaces for ion transport is analyzed by using engineered MOFs as SEs. The results show that the ion conductivity of MOFs decorated with a long chain Lewis base (LCLB) has been greatly improved. The interface resistance of the SEs composed of MOFs with LCLB has decreased markedly. Most importantly, the corresponding Li|SE|LiPO 4 solid-state battery (SSB) shows an improved specific capacity of 47% and longer lifetime at 5 C compared with the SSB without interface engineering. Such results shed new light on the understanding of ion transport at interfaces and suggest the feasibility of interface engineered MOFs as advanced SEs.

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Amine-Grafted MIL-101(Cr) via Double-Solvent Incorporation for Synergistic Enhancement of CO₂ Uptake and Selectivity

Cited by 52 publications

References 62 publications

In situ casting of rice husk ash in metal organic frameworks induces enhanced CO2 capture performance

In situ casting of rice husk ash in metal organic frameworks induces enhanced CO2 capture performance

Sequential Co-immobilization of Enzymes in Metal-Organic Frameworks for Efficient Biocatalytic Conversion of Adsorbed CO2 to Formate

Molecular‐Scale Interface Engineering of Metal–Organic Frameworks toward Ion Transport Enables High‐Performance Solid Lithium Metal Battery

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Amine-Grafted MIL-101(Cr) via Double-Solvent Incorporation for Synergistic Enhancement of CO2 Uptake and Selectivity

Cited by 52 publications

References 62 publications

In situ casting of rice husk ash in metal organic frameworks induces enhanced CO2 capture performance

In situ casting of rice husk ash in metal organic frameworks induces enhanced CO2 capture performance

Sequential Co-immobilization of Enzymes in Metal-Organic Frameworks for Efficient Biocatalytic Conversion of Adsorbed CO2 to Formate

Molecular‐Scale Interface Engineering of Metal–Organic Frameworks toward Ion Transport Enables High‐Performance Solid Lithium Metal Battery

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Amine-Grafted MIL-101(Cr) via Double-Solvent Incorporation for Synergistic Enhancement of CO₂ Uptake and Selectivity