CoNi Alloy Nanoparticles Embedded in Metal–Organic Framework‐Derived Carbon for the Highly Efficient Separation of Xenon and Krypton via a Charge‐Transfer Effect

Chen, Fuqiang; Ding, Jiaqi; Guo, Kaiqing; Yang, Liting; Zhang, Zhiguo; Yang, Qiwei; Yang, Yiwen; Bao, Zongbi; He, Yi; Ren, Qilong

doi:10.1002/anie.202011778

Cited by 64 publications

(42 citation statements)

References 58 publications

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“…Because of the potential of the C 2 H 6 /C 2 H 4 separation, we aimed to look at even more challenging separations, such as xenon/krypton (Xe/Kr), which have small differences in chemical and physical properties. Due to the lack of dipole or quadruple moments, Xe and Kr cannot interact with porous adsorbents via intermolecular interactions, such as π–π stacking, hydrogen bonding, and dipole–dipole interactions . As a result of their similar properties (kinetic diameter: 4.0 Å for Xe and 3.7 Å for Kr; polarizability: 4.04 × 10 25 cm 3 for Xe vs. 2.48 × 10 25 cm 3 ), it remains a great challenge to achieve the efficient separation of Xe and Kr.…”

Section: Results and Discissionmentioning

confidence: 99%

“…Due to the lack of dipole or quadruple moments, Xe and Kr cannot interact with porous adsorbents via intermolecular interactions, such as π−π stacking, hydrogen bonding, and dipole−dipole interactions. 49 As a result of their similar properties (kinetic diameter: 4.0 Å for Xe and 3.7 Å for Kr; polarizability: 4.04 × 10 25 cm 3 for Xe vs. 2.48 × 10 25 cm 3 ), 47 it remains a great challenge to achieve the efficient separation of Xe and Kr. A recent work demonstrated that by utilizing the difference in gate-opening pressures, flexible NbOFFIVE-2−Cu-I (ZU-62) allows for more promise in effectively separating Xe from Kr.…”

Section: ■ Introductionmentioning

confidence: 99%

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Tuning the Structural Flexibility for Multi-Responsive Gas Sorption in Isonicotinate-Based Metal–Organic Frameworks

Chen

Idrees²,

Son³

et al. 2021

ACS Appl. Mater. Interfaces

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Flexible metal–organic frameworks (MOFs) are of high interest as smart programmable materials for gas sorption due to their unique structural changes triggered by external stimuli. Owing to this property, which leads to opportunities such as maximizing deliverable gas capacity, flexible MOFs sometimes offer more advantages in sorption applications compared to their more rigid counterparts. Herein, we elucidate the effect of transition metal identity of a series of isonicotinate-based flexible MOFs, M(4-PyC)2 [MMg, Mn, and Cu; 4-PyC = 4-pyridine carboxylic acid] on the structural dynamic response to different gases (C2H4, C2H6, Xe, Kr, and SO2). Isotherms at different temperatures show that C2H4, C2H6, and Xe can form sufficiently strong interactions with both Mg(4-PyC)2 and Mn(4-PyC)2 frameworks resulting in gate-opening behavior due to the rotation of the linker’s pyridine ring, while Kr cannot induce this phenomenon for the two MOFs under the measured conditions. In contrast, the gate-opening behavior occurs for Cu(4-PyC)2 solely in the presence of C2H4, and no other measured gas, due to the open metal sites of Cu centers. In comparison, SO2, a strong polar molecule, triggers the gate-opening effect in all three MOFs. Interestingly, a shape memory effect is observed for Cu(4-PyC)2 during the second SO2 sorption cycle. When comparing the different gate-opening pressures of each gas, we observed that the structural flexibility of the three frameworks is highly sensitive to the chemical hardness of the Lewis acidic metal ions (Mg2+ > Mn2+ > Cu2+). As a result, the gate opening behavior is observed at lower pressures for the MOFs containing weaker M–N bonds (harder metal ions), with the exception of Cu(4-PyC)2 toward C2H4. These observations reveal that different transition metals can be used to finely control the structural flexibility of the frameworks.

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Section: Results and Discissionmentioning

confidence: 99%

Section: ■ Introductionmentioning

confidence: 99%

Tuning the Structural Flexibility for Multi-Responsive Gas Sorption in Isonicotinate-Based Metal–Organic Frameworks

Chen

Idrees²,

Son³

et al. 2021

ACS Appl. Mater. Interfaces

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show abstract

“…Moreover, strong affinities toward gas molecules can be attributed to the strongly polarized pore channels of zeolites that make regeneration a harsh process [20]. By contrast, porous carbons are considered promising adsorbents for applications in harsh industrial conditions because of their robust stability, low fabrication cost, and water resistance [3,[38][39][40].…”

Section: Introductionmentioning

confidence: 99%

Extraction of propane and ethane from natural gas on ultramicroporous carbon adsorbent with record selectivity

et al. 2022

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The separation of light hydrocarbon mixtures and the extraction of C 3 H 8 and C 2 H 6 from natural gas are of significant importance in natural gas purification and upgrading. Microporous carbon adsorbents are promising in light hydrocarbon separation. However, the fabrication of uniform ultramicropores to boost separation selectivity remains challenging. Herein, we fabricated a series of poly(vinylidene chloride)-resin-derived ultramicroporous carbon adsorbents with a relatively uniform pore size (5.2-5.3 Å) by activator-free pyrolysis. The optimal C-PVDC-800 exhibited record-high ideal adsorption solution theory (IAST) selectivity for C 3 H 8 /CH 4 (3387) and C 2 H 6 /CH 4 (75) and Henry's selectivity for C 3 H 8 /CH 4 (369) among all reported adsorbents under ambient conditions, combined with ultrahigh uptake of C 3 H 8 (3.9 mmol g −1 , 0.05 bar) and C 2 H 6 (2.67 mmol g −1 , 0.10 bar) at low partial pressures and 298 K. More importantly, fast gas adsorption kinetics favorable for fixed-bed adsorption applications was realized. Breakthrough experiments and cycling tests further confirm the superb separation performance of the extraction of C 3 H 8 and C 2 H 6 from natural gas.

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“…Chen et al obtained highly efficient Xe/Kr separation adsorbents using MOFs as precursors. The existence of the NiCo alloy in NiCo@C-700 provided higher charge-transfer performance . Non-noble Ni-based catalysts, for instance, Ni/Al 2 O 3 , Ni–MoO x /C, and Ni/boehmite, showed high conversion of LA to yield GVL but poor stability in consecutive catalytic runs due to the Ni leaching during the reaction process .…”

Section: Introductionmentioning

confidence: 99%

“…The existence of the NiCo alloy in NiCo@C-700 provided higher charge-transfer performance. 31 Non-noble Ni-based catalysts, for instance, Ni/ Al 2 O 3 , Ni−MoO x /C, and Ni/boehmite, showed high conversion of LA to yield GVL but poor stability in consecutive catalytic runs due to the Ni leaching during the reaction process. 4 A series of Cu-based catalysts such as Cu−Cr, Cu− Fe, Cu/ZrO 2 , and Cu/SiO 2 showed excellent activity for acquiring GVL from LA; however, severe catalytic conditions for pursuing high LA conversion was needed.…”

Section: ■ Introductionmentioning

confidence: 99%

Bimetallic NiCu Alloy Catalysts for Hydrogenation of Levulinic Acid

Zhang

et al. 2021

ACS Appl. Nano Mater.

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Upgrading of the biomass-derived levulinic acid (LA) with the activation of carbonyl functional groups is a pivotal reaction in converting biomass into high-value-added products. Herein, we reported a modified strategy to synthesize highly dispersed noble-metal-free bimetallic NiCu alloy nanoparticles (NPs) from metal−organic frameworks for the selective hydrogenation of LA, in which the ligand effect between Ni and Cu plays a crucial role under relatively mild conditions. Among the tested catalysts, the catalyst with a Ni/Cu ratio of 1:2 presented the best catalytic performance in comparison with the homometallic Ni/Cu and bimetallic catalysts with different ratios; an outstanding yield of 93.9% was obtained for γ-valerolactone (GVL). Both experimental studies and characterization analyses verified that the ligand effect is responsible for the excellent catalytic performance. A possible reaction pathway for the samples in the LA hydrogenation process is proposed; after dissociation of adsorbed H 2 on the NiCu alloy surface, reactant LA is adsorbed and activated by NPs with the formation of intermediate, and through a self-condensation reaction to form products. The straightforward synthesis, superior performance, and high stability make these noble-metal-free bimetallic NiCu nanoparticles very attractive for the transformation of various biomass-derived sources into valuable products.

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CoNi Alloy Nanoparticles Embedded in Metal–Organic Framework‐Derived Carbon for the Highly Efficient Separation of Xenon and Krypton via a Charge‐Transfer Effect

Cited by 64 publications

References 58 publications

Tuning the Structural Flexibility for Multi-Responsive Gas Sorption in Isonicotinate-Based Metal–Organic Frameworks

Tuning the Structural Flexibility for Multi-Responsive Gas Sorption in Isonicotinate-Based Metal–Organic Frameworks

Extraction of propane and ethane from natural gas on ultramicroporous carbon adsorbent with record selectivity

Bimetallic NiCu Alloy Catalysts for Hydrogenation of Levulinic Acid

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