Efficient C2H2/CO2 Separation in Ultramicroporous Metal–Organic Frameworks with Record C2H2 Storage Density DOI
Wei Gong, Hui Cui, Yi Xie

и другие.

Journal of the American Chemical Society, Год журнала: 2021, Номер 143(36), С. 14869 - 14876

Опубликована: Авг. 31, 2021

Physical separation of C2H2 from CO2 on metal–organic frameworks (MOFs) has received substantial research interest due to the advantages simplicity, security, and energy efficiency. However, that exhibit very close physical properties makes their exceptionally challenging. Previous work appeared mostly focused introducing open metal sites aims enhance affinity at desired sites, whereas reticular manipulation organic components rarely been investigated. In this work, by reticulating preselected amino hydroxy functionalities into isostructural ultramicroporous chiral MOFs—Ni2(l-asp)2(bpy) (MOF-NH2) Ni2(l-mal)2(bpy) (MOF-OH)—we targeted efficient uptake C2H2/CO2 separation, which outperforms most benchmark materials. Explicitly, MOF-OH adsorbs amount with record storage density 0.81 g mL–1 ambient conditions, even exceeds solid 189 K. addition, gave IAST selectivity 25 toward equimolar mixture C2H2/CO2, is nearly twice higher than MOF-NH2. Notably, adsorption enthalpies for zero converge in both MOFs are remarkably low (17.5 kJ mol–1 16.7 MOF-NH2), our knowledge lowest among rigid sorbents. The efficiencies validated multicycle breakthrough experiments. DFT calculations provide molecular-level insight over adsorption/separation mechanism. Moreover, can survive boiling water least 1 week be easily scaled up kilograms eco-friendly economically, crucial potential industrial implementation.

Язык: Английский

Energy-efficient separation alternatives: metal–organic frameworks and membranes for hydrocarbon separation DOI
Lifeng Yang,

Siheng Qian,

Xiaobing Wang

и другие.

Chemical Society Reviews, Год журнала: 2020, Номер 49(15), С. 5359 - 5406

Опубликована: Янв. 1, 2020

The diversity of metal–organic frameworks enables the design highly efficient adsorbents and membranes towards hydrocarbon separations for energy consumption mitigation.

Язык: Английский

Процитировано

547

Mixed Metal–Organic Framework with Multiple Binding Sites for Efficient C2H2/CO2Separation DOI
Junkuo Gao, Xuefeng Qian, Rui‐Biao Lin

и другие.

Angewandte Chemie International Edition, Год журнала: 2020, Номер 59(11), С. 4396 - 4400

Опубликована: Янв. 13, 2020

The separation of C

Язык: Английский

Процитировано

379

Ethylene/ethane separation in a stable hydrogen-bonded organic framework through a gating mechanism DOI

Yisi Yang,

Libo Li, Rui‐Biao Lin

и другие.

Nature Chemistry, Год журнала: 2021, Номер 13(10), С. 933 - 939

Опубликована: Июль 8, 2021

Язык: Английский

Процитировано

371

Cage-Interconnected Metal–Organic Framework with Tailored Apertures for Efficient C2H6/C2H4 Separation under Humid Conditions DOI
Heng Zeng, Xiao‐Jing Xie, Mo Xie

и другие.

Journal of the American Chemical Society, Год журнала: 2019, Номер 141(51), С. 20390 - 20396

Опубликована: Ноя. 29, 2019

Metal-organic frameworks (MOFs) with open metal sites (OMSs) have been shown to preferentially adsorb unsaturated hydrocarbons such as C2H4 due the formation of π-complexation. However, adsorption capacity and selectivity might well be dampened under humid conditions because OMSs could easily poisoned in presence water vapor. C2H6-selective adsorbents less hydrophilic environments, on other hand, not only effectively minimize impact humidity separation but also directly produce high-purity from C2H6/C2H4 mixtures. Here, we report a MOF (JNU-2) underlying rare xae topology. Its cage-like cavities are interconnected through apertures limiting diameter ca. 3.7 Å, which is domain kinetic diameters C2H6 molecules. Molecular modeling studies suggest four oxygen atoms aperture poised interact multiple C-H···O hydrogen bonding, rendering JNU-2 an enhanced selectivity. Indeed, experimental results reveal that takes up great amount comparable top-performing MOFs displays excellent even conditions; moreover, it can regenerated at room temperature owing its moderate enthalpy. This work successfully demonstrated strategy balancing for by designing materials tailored apertures. The function screening selectivity, while internal provide space large adsorption.

Язык: Английский

Процитировано

268

Selective capture of carbon dioxide from hydrocarbons using a metal-organic framework DOI Creative Commons
Omid T. Qazvini, Ravichandar Babarao, Shane G. Telfer

и другие.

Nature Communications, Год журнала: 2021, Номер 12(1)

Опубликована: Янв. 8, 2021

Abstract Efficient and sustainable methods for carbon dioxide capture are highly sought after. Mature technologies involve chemical reactions that absorb CO 2, but they have many drawbacks. Energy-efficient alternatives may be realised by porous physisorbents with void spaces complementary in size electrostatic potential to molecular 2 . Here, we present a robust, recyclable inexpensive adsorbent termed MUF-16. This metal-organic framework captures high affinity its one-dimensional channels, as determined adsorption isotherms, X-ray crystallography density-functional theory calculations. Its low other competing gases delivers selectivity the of over methane, acetylene, ethylene, ethane, propylene propane. For equimolar mixtures /CH 4 /C H , is 6690 510, respectively. Breakthrough gas separations under dynamic conditions benefit from short time lags elution weakly-adsorbed component deliver high-purity hydrocarbon products, including pure methane acetylene.

Язык: Английский

Процитировано

268

Pore-Space-Partition-Enabled Exceptional Ethane Uptake and Ethane-Selective Ethane–Ethylene Separation DOI
Huajun Yang, Yanxiang Wang, Rajamani Krishna

и другие.

Journal of the American Chemical Society, Год журнала: 2020, Номер 142(5), С. 2222 - 2227

Опубликована: Янв. 27, 2020

An ideal material for C2H6/C2H4 separation would simultaneously have the highest C2H6 uptake capacity and selectivity. But such is elusive. A benchmark ethane-selective peroxo-functionalized MOF-74-Fe that exhibits best known performance due to its high selectivity (4.4), although moderate (74.3 cm3/g). Here, we report a family of pore-space-partitioned crystalline porous materials (CPMs) with exceptional potential (i.e., C2H4 recovered from mixture) despite their (up 1.75). The ethane as 166.8 cm3/g at 1 atm 298 K, more than twice peroxo-MOF-74-Fe, has been achieved even though isosteric heat adsorption (21.9–30.4 kJ/mol) these CPMs low about one-third peroxo-MOF-74-Fe (66.8 kJ/mol). While overall potentials not yet surpassed robust exhibit outstanding properties including thermal stability 450 °C) aqueous stability, regeneration energy, degree chemical geometrical tunability within same isoreticular framework.

Язык: Английский

Процитировано

258

A robust Th-azole framework for highly efficient purification of C2H4 from a C2H4/C2H2/C2H6 mixture DOI Creative Commons

Zhenzhen Xu,

Xiao‐Hong Xiong, Jian‐Bo Xiong

и другие.

Nature Communications, Год журнала: 2020, Номер 11(1)

Опубликована: Июнь 22, 2020

Abstract Separation of C 2 H 4 from /C 6 mixture with high working capacity is still a challenging task. Herein, we deliberately design Th-metal-organic framework (MOF) for highly efficient separation binary and ternary mixture. The synthesized MOF Azole-Th-1 shows UiO-66-type structure fcu topology built on Th secondary building unit tetrazole-based linker. Such noticeable structure, connected by N,O-donor ligand chemical stability. At 100 kPa 298 K performs excellent (purity > 99.9%) not only (1:9, v/v) but also (9:1:90, v/v/v), the corresponding can reach up to 1.13 1.34 mmol g −1 , respectively. mechanism, as unveiled density functional theory calculation, due stronger van der Waals interaction between ethane skeleton.

Язык: Английский

Процитировано

253

Designer Metal–Organic Frameworks for Size‐Exclusion‐Based Hydrocarbon Separations: Progress and Challenges DOI
Hao Wang, Yunling Liu, Jing Li

и другие.

Advanced Materials, Год журнала: 2020, Номер 32(44)

Опубликована: Июль 9, 2020

Abstract The separation of hydrocarbons is primary importance in the petrochemical industry but remains a challenging process. Hydrocarbon separations have traditionally relied predominantly on costly and energy‐intensive heat‐driven procedures such as low‐temperature distillations. Adsorptive based porous solids represents an alternative technology that potentially more energy efficient for some hydrocarbons. Great efforts been made recently not only development adsorbents with optimal performance also toward subsequent implementation adsorption‐based technology. Emerging relatively new class multifunctional materials, metal–organic frameworks (MOFs) hold substantial promise highly This because their exceptional intrinsic porosity tunability, which enables size‐exclusion‐based render highest possible selectivity. In this review, recent advances MOFs selected groups are reviewed, including methane/C 2 hydrocarbons, normal alkanes, alkane isomers, alkane/alkene/alkyne C 8 alkylaromatics, particular focus size‐exclusion mechanism. Insights into tailor‐made structures, material design strategies, structure–property relationships will be elucidated. addition, existing challenges future directions important research field discussed.

Язык: Английский

Процитировано

252

Selective Ethane/Ethylene Separation in a Robust Microporous Hydrogen-Bonded Organic Framework DOI
Xu Zhang, Libo Li, Jia‐Xin Wang

и другие.

Journal of the American Chemical Society, Год журнала: 2019, Номер 142(1), С. 633 - 640

Опубликована: Дек. 14, 2019

The separation of ethane (C2H6) from ethylene (C2H4) is prime importance in the production polymer-grade C2H4 for industrial manufacturing. It very challenging and still remains unexploited to fully realize efficient C2H6/C2H4 emerging hydrogen-bonded organic frameworks (HOFs) due weak nature hydrogen bonds. We herein report benchmark example a novel ultrarobust HOF adsorbent (termed as HOF-76a) with Brunauer–Emmett–Teller surface area exceeding 1100 m2 g–1, exhibiting preferential binding C2H6 over thus highly selective C2H6/C2H4. Theoretical calculations indicate key role nonpolar suitable triangular channel-like pores HOF-76a sterically "match" better nonplanar molecule than planar C2H4, affording overall stronger multipoint van der Waals interactions C2H6. exceptional performance was clearly demonstrated by gas adsorption isotherms, ideal adsorbed solution theory calculations, simulated experimental breakthrough curves. Breakthrough experiments on reveal that can be straightforwardly produced 50/50 (v/v) mixtures during first cycle high productivity 7.2 L/kg at 298 K 1.01 bar 18.8 5.0 bar, respectively.

Язык: Английский

Процитировано

248

An Ultramicroporous Metal–Organic Framework for High Sieving Separation of Propylene from Propane DOI
Bin Liang, Xin Zhang, Yi Xie

и другие.

Journal of the American Chemical Society, Год журнала: 2020, Номер 142(41), С. 17795 - 17801

Опубликована: Сен. 29, 2020

Highly selective adsorptive separation of olefin/paraffin through porous materials can produce high purity olefins in a much more energy-efficient way than the traditional cryogenic distillation. Here we report an ultramicroporous cobalt gallate metal-organic framework (Co-gallate) for highly sieving propylene/propane at ambient conditions. This material possesses optimal pore structure exact confinement propylene molecules while excluding slightly large propane molecules, as clearly demonstrated neutron diffraction crystal Co-gallate⊃0.38C

Язык: Английский

Процитировано

242