Adsorption technology based on ethane-selective materials is a promising alternative to energy-intensive cryogenic distillation for separating ethane (C2H6) and ethylene (C2H4). We employed pore engineering strategy to tune pore environment of metal-organic framework (MOF) through organic functional groups and boosted the C2H6/C2H4 separation of MOF. Introduction of amino (-NH2) groups into Tb-MOF-76 not only decreased pore sizes but also facilitated multiple guest-host interactions in confined pores. The NH2-functionalized Tb-MOF-76(NH2) has increased C2H6 and C2H4 uptakes and C2H6/C2H4 selectivity. The results of experimental and simulated transient breakthroughs reveal that Tb-MOF-76(NH2) has significantly improved one-step separation performance for  C2H6/C2H4 mixtures with a high C2H4 (>99.95%) productivity of 17.66 L kg-1 compared to 7.53 L kg-1 by Tb-MOF-76, resulting from the suitable pore confinement and accissible -NH2 groups on pore surfaces.

Boosting Ethane/Ethylene Separation by MOFs through the Amino-Functionalization of Pores.

One-step C2H4 purification from ternary C2H6/C2H4/C2H2 mixtures by a single adsorbent is of great industrial significance, but few adsorbents achieved this separation. Herein, we report a robust metal-organic framework (MOF) that possesses the methyl-decorated nonpolar pores and shows one-step C2H4 purification (purity > 99.9%) from binary C2H6/C2H4 mixtures and ternary C2H6/C2H4/C2H2 mixtures. The methyl groups in pores provide a suitable pore environment to simultaneously enhance the adsorption capacity for C2H2 and C2H6 compared to C2H4. Simulations revealed the multiple interactions between C2H6 or C2H2 molecules and the pore walls, while the interactions with C2H4 molecules are weak and also unfavorable due to the repulsion from methyl groups in pores. The MOF displays high C2H6 and C2H2 uptakes and benchmark C2H6/C2H4 selectivity (2.2), surpassing all of the reported MOFs for one-step C2H4 purification from ternary C2H6/C2H4/C2H2 mixtures.

One-step C2H4 Purification from Ternary C2H6/C2H4/C2H2 Mixtures by a Robust Metal-Organic Framework with Customized Pore Environment.

Because C 2 H 4 plays an essential role in the chemical industry, economical and energy-efficient separation of ethylene (C 2 H 4 ) from ethane (C 2 H 6 ) is extremely important. With the exception of energy-extensive cryogenic distillation, there are few one-step methods to obtain polymer-grade (≥ 99.95% pure) C 2 H 4 from C 2 H 4 /C 2 H 6 mixtures. Here we report a highly stable metal-organic-framework FJI-H11-Me(des) (FJI-H = Hong's group in Fujian Institute of Research on the Structure of Matter), which features one-dimensional hexagonal nonpolar pore surfaces constructed by aromatic rings and alkyl groups. This FJI-H11-Me(des) adsorbs C 2 H 6 rather than C 2 H 4 between 273 and 303 K. Practical breakthrough experiments with C 2 H 4 containing 1% C 2 H 6 have shown that FJI-H11-Me(des) can realize the acquisition in one-step of polymer-grade, 99.95% pure C 2 H 4 under various conditions including different gas flow rates, temperatures and relative humidities.

A Metal-Organic Framework with Nonpolar Pore Surfaces for the One-step Acquisition of C2H4 from a C2H4 and C2H6 Mixture.

Hydrogen-bonded organic frameworks (HOFs) show great potential in energy-saving C2H6/C2H4 separation, but there are few examples of one-step acquisition of C2H4 from C2H6/C2H4 because it is still difficult to achieve the reverse-order adsorption of C2H6 and C2H4. In this work, we boost the C2H6/C2H4 separation performance in two graphene-sheet-like HOFs by tuning pore polarization. Upon heating, an in situ solid phase transformation can be observed from HOF-NBDA(DMA) (DMA = dimethylamine cation) to HOF-NBDA, accompanied with transformation of the electronegative skeleton into neutral one. As a result, the pore surface of HOF-NBDA has become nonpolar, which is beneficial to selectively adsorbing C2H6. The difference in the capacities for C2H6 and C2H4 is 23.4 cm3∙g-1 for HOF-NBDA, and the C2H6/C2H4 uptake ratio is 136%, which are much higher than those for HOF-NBDA(DMA) (5.0 cm3∙g-1 and 108% respectively). Practical breakthrough experiments demonstrate HOF-NBDA could produce polymer-grade C2H4 from C2H6/C2H4 (1/99, v/v) mixture with a high productivity of 29.2 L∙kg-1 at 298 K, which is about five times as high as HOF-NBDA(DMA) (5.4 L∙kg-1). In addition, in situ breakthrough experiments and theoretical calculations indicate the pore surface of HOF-NBDA is beneficial to preferentially capture C2H6 and thus boosts selective separation of C2H6/C2H4.

Tuning Pore Polarization to Boost Ethane/Ethylene Separation Performance in Hydrogen-Bonded Organic Frameworks.

Developing efficient and sensitive MOF-based luminescence sensors for bioactive molecule detection is of great significance and remains a challenge. Benefiting from favorable chemical and thermal stability, as well as excellent luminescence performance, a porous Zn(II)Ho(III) heterometallic-organic framework (ZnHoMOF) was selected here as a bifunctional luminescence sensor for the early diagnosis of a toluene exposure biomarker of hippuric acid (HA) through "turn-on" luminescence enhancing response and the daily monitoring of NFT/NFZ antibiotics through "turn-off" quenching effects in aqueous media with high sensitivity, acceptable selectivity, good anti-interference, exceptional recyclability performance, and low detection limits (LODs) of 0.7 ppm for HA, 0.04 ppm for NFT, and 0.05 ppm for NFZ. Moreover, the developed sensor was employed to quantify HA in diluted urine samples and NFT/NFZ in natural river water with satisfactory results. In addition, the sensing mechanisms of ZnHoMOF as a dual-response chemosensor in efficient detection of HA and NFT/NFZ antibiotics were conducted from the view of photo-induced electron transfer (PET), as well as inner filter effects (IFEs), with the help of time-dependent density functional theory (TD-DFT) and spectral overlap experiments.

Heterometallic ZnHoMOF as a Dual-Responsive Luminescence Sensor for Efficient Detection of Hippuric Acid Biomarker and Nitrofuran Antibiotics.

A robust ethane-selective metal-organic framework with nonpolar pore surface for efficient C2H6/C2H4 separation

A new metal–organic framework based on rare [Zn4F4] cores for efficient separation of C2H2

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A robust ethane-selective metal-organic framework with nonpolar pore surface for efficient C2H6/C2H4 separation

A new metal–organic framework based on rare [Zn4F4] cores for efficient separation of C2H2