Modulating the D‐π‐A Interactions in Metal‐Covalent Organic Frameworks for Efficient Electroreduction of CO2 into Formate DOI
Kai Cui, Zhao Zhang,

Congxu Wang

и другие.

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(32)

Опубликована: Май 23, 2024

Abstract Crystalline porous framework materials have attracted tremendous interest in electrocatalytic CO 2 reduction owing to their ordered structures and high specific surface areas as well rich designability, however, still suffer from a lack of accuracy regulating the binding strength between catalytic sites intermediates, which is crucial for optimizing activity expanding product types. Herein, we report three new kinds vinylene‐linked metal‐covalent organic frameworks (TMT‐CH 3 ‐MCOF, TMP‐CH ‐MCOF TMP‐MCOF) with continuously tunable D‐π‐A interactions by adjusting structure monomers at molecular level realizing efficient electroreduction formate first time. Interestingly, compared TMT‐CH TMP‐MCOF, exhibited highest HCOO − Faradaic efficiency (FE HCOO‐ ) 95.6 % −1.0 V vs RHE displayed FE above 90 voltage range −1.2 vs. RHE, one among various reported electrocatalysts. Theoretical calculations further reveal that unique moderate suitable ability towards reaction intermediate, beneficial formation *HCOO desorption *HCOOH, thus effectively promoting formate.

Язык: Английский

Fluorinated MOF‐Based Hexafluoropropylene Nanotrap for Highly Efficient Purification of Octafluoropropane Electronic Specialty Gas DOI
Mingze Zheng, Wenjuan Xue, Tongan Yan

и другие.

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(15)

Опубликована: Фев. 16, 2024

Abstract High‐purity octafluoropropane (C 3 F 8 ) electronic specialty gas is a key chemical raw material in semiconductor and integrated circuit manufacturing industry, while selective removal of hexafluoropropylene 6 impurity for C purification essential but challenging task. Here we report fluorinated cage‐like MOF Zn‐bzc‐CF (bzc=5‐(trifluoromethyl)‐1H‐pyrazole‐4‐carboxylic acid) /C separation. The incorporation −CF groups not only provides suitable pore aperture size highly efficient size‐exclusive separation, also creates hydrophobic microenvironments, endowing Zn‐bz‐CF high stability. Remarkably, exhibits adsorption capacity excluding , achieving ideal molecular‐sieving Breakthrough experiments show that can efficiently separate mixture high‐purity (99.9 %) be obtained.

Язык: Английский

Процитировано

15

Scalable Synthesis of Robust MOF for Challenging Ethylene Purification and Propylene Recovery with Record Productivity DOI

Gang‐Ding Wang,

Yong‐Zhi Li,

Rajamani Krishna

и другие.

Angewandte Chemie, Год журнала: 2024, Номер 136(15)

Опубликована: Фев. 19, 2024

Abstract Ethylene (C 2 H 4 ) purification and propylene 3 6 recovery are highly relevant in polymer synthesis, yet developing physisorbents for these industrial separation faces the challenges of merging easy scalability, economic feasibility, high moisture stability with great efficiency. Herein, we reported a robust scalable MOF (MAC‐4) simultaneous C . Through creating nonpolar pores decorated by accessible N/O sites, MAC‐4 displays top‐tier uptakes selectivities over at ambient conditions. Molecular modelling combined infrared spectroscopy revealed that molecules were trapped framework stronger contacts relative to Breakthrough experiments demonstrated exceptional performance binary /C as well ternary mixtures, simultaneously affording record productivities 27.4 36.2 L kg −1 high‐purity (≥99.9 %) (≥99.5 %). was facilely prepared deckgram‐scale under reflux condition within hours, making it smart address challenging gas separations.

Язык: Английский

Процитировано

13

Reverse Separation of Carbon Dioxide and Acetylene in Two Isostructural Copper Pyridine‐Carboxylate Frameworks DOI
Jing‐Hong Li,

You-Wei Gan,

Jun‐Xian Chen

и другие.

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(30)

Опубликована: Май 13, 2024

Separating acetylene from carbon dioxide is important but highly challenging due to their similar molecular shapes and physical properties. Adsorptive separation of can directly produce pure hardly realized because relatively polarizable binds more strongly. Here, we reverse the CO

Язык: Английский

Процитировано

12

In situ generated 2,5-pyrazinedicarboxylate and oxalate ligands leading to a Eu-MOF for selective capture of C2H2 from C2H2/CO2 DOI
Fenglan Liang, De‐Yun Ma, Liang Qin

и другие.

Dalton Transactions, Год журнала: 2024, Номер 53(24), С. 10070 - 10074

Опубликована: Янв. 1, 2024

A new Eu-MOF is prepared, involving in situ generation of oxalate and 2,5-pyrazinedicarboxylate ligands, activated at different temperatures to obtain two MOFs (1a 1b), which 1b able selectively capture C 2 H from /CO .

Язык: Английский

Процитировано

12

Constructing local nanomolecular trap in a scalable, low-cost, and ultramicroporous metal–organic framework for efficient capture of greenhouse gases SF6 and CO2 DOI
Shiming Li, Qiang Zhang,

Hong-Chan Jiang

и другие.

Chemical Engineering Journal, Год журнала: 2024, Номер 496, С. 154026 - 154026

Опубликована: Июль 20, 2024

Язык: Английский

Процитировано

12

Metal Hydrogen-Bonded Organic Frameworks as Open Lewis Acid Catalysts for Two Types of CO2 Transformations DOI
Hua Liu, Zhi-Wei Zheng, Xiang‐Yu Zhang

и другие.

Inorganic Chemistry, Год журнала: 2024, Номер 63(25), С. 11554 - 11565

Опубликована: Май 30, 2024

Efficient and multiple CO2 utilization into high-value-added chemicals holds significant importance in carbon neutrality industry production. However, most catalysis systems generally exhibit only one type of transformation with the efficiency to be improved. The restricted abundance active catalytic sites or an inefficient rate these results constraint. Consequently, we designed constructed two metal hydrogen-bonded organic frameworks (M-HOFs) {[M3(L3–)2(H2O)10]·2H2O}n (M = Co (1), Ni (2); L 1-(4-carboxyphenyl)-1H-pyrazole-3,5-dicarboxylic acid) this research. 1 2 are well-characterized, both show excellent stability. networks connected by hydrogen bonds enhance structural flexibility create accessible Lewis acidic sites, promoting interactions between substrates centers. This enhancement facilitates efficient for types transformations, encompassing cycloaddition reactions epoxides aziridines afford cyclic carbonates oxazolidinones. activities (TON/TOF) superior compared those other catalysts. These heterogeneous catalysts still exhibited high performance after being reused several times. Mechanistic studies indicated intense substrates, demonstrating reason catalysis. marks first instance on M-HOFs efficiently catalyzing conversions, finding important significance catalyst design utilization.

Язык: Английский

Процитировано

11

Boosting Acetylene Packing Density within an Isoreticular Metal–Organic Framework for Efficient C2H2/CO2 Separation DOI Creative Commons

Shan‐Qing Yang,

Bo Xing,

Lulu Wang

и другие.

Chem & Bio Engineering, Год журнала: 2024, Номер 1(3), С. 245 - 251

Опубликована: Фев. 1, 2024

Porous solid adsorbents for C2H2/CO2 separation are generally confronted with poor stability, high cost, or regeneration energy, which largely inhibit their industrial implementation. A desired adsorbent material practical implementation should exhibit a good balance between low scale-up production feasibility, and performance. An effective strategy is herein explored based on reticular chemistry through embedding methyl groups in prototype microporous metal-organic framework (MOF) featuring cost stability to effectively separate an mixture. The anchored the pore surfaces could strongly boost C2H2 packing density specifically enhance performance, as distinctly established by single-component gas sorption isotherms. CAU-10-CH3 exhibits excellent of 486 g L-1 adsorption differences CO2 uptake (147%), outperforming benchmark CAU-10-H (392 53%). highly selective over was achieved lower enthalpy (25.18 kJ mol-1) compared that unfunctionalized CAU-10-H. In addition, dynamic column breakthrough experiments further confirm CAU-10-CH3's efficient performance accomplishes scale-up, separation, establishing its promise This approach facilitate development advanced MOF address challenging processes. Thus, this study paves route implementations materials field.

Язык: Английский

Процитировано

10

Metal–Organic Frameworks Possessing Suitable Pores for Xe/Kr Separation DOI

Dong-Mei Zeng,

Lian Huang,

Xing-Ping Fu

и другие.

Inorganic Chemistry, Год журнала: 2024, Номер 63(11), С. 5151 - 5157

Опубликована: Март 6, 2024

Adsorption separation of the Xe/Kr mixture remains a tough issue since Xe and Kr have an inert nature similar sizes. Here we present chlorinated metal–organic framework (MOF) [JXNU-19(Cl)] its nonchlorinated analogue (JXNU-19) for separation. The two isostructural MOFs constructed from heptanuclear cobalt-hydroxyl clusters bridged by organic ligands are three-dimensional structures. Detailed contrast adsorption properties MOF shows that significantly enhanced uptakes selectivity (17.1) observed JXNU-19 as compared to JXNU-19(Cl). main binding sites in revealed computational simulations far away chlorine sites, suggesting introduction groups results unfavorable optimal pores, high surface area, multiple strong Xe–framework interactions facilitate effective JXNU-19.

Язык: Английский

Процитировано

10

Integration of ordered porous materials for targeted three-component gas separation DOI Creative Commons
Xue Jiang, Yu Wang, Wang Hui

и другие.

Nature Communications, Год журнала: 2025, Номер 16(1)

Опубликована: Янв. 15, 2025

Separation of multi-component mixtures in an energy-efficient manner has important practical impact chemical industry but is highly challenging. Especially, targeted simultaneous removal multiple impurities to purify the desired product one-step separation process extremely difficult task. We introduced a pore integration strategy modularizing ordered structures with specific functions for on-demand assembly deal complex systems, which are unattainable by each individual pore. As proof concept, two ultramicroporous nanocrystals (one C2H2-selective and other CO2-selective) as shell pores were respectively grown on C2H6-selective porous material core Both respective pore-integrated materials show excellent ethylene production performance dynamic breakthrough experiments C2H2/C2H4/C2H6 CO2/C2H4/C2H6 gas mixture, even better than that from traditional tandem-packing processes originated optimized mass/heat transfer. Thermodynamic simulation results explained pre-designed modules can perform target independently materials. Pore offers approach assembling demand achieve mixtures.

Язык: Английский

Процитировано

2

Reversed CO2/C2H2 separation via combined adsorption kinetics and diffusion differences in MOF-polymer mixed matrix membrane DOI
Bin Yu,

Tianhao Lan,

Hui Wang

и другие.

Journal of Membrane Science, Год журнала: 2025, Номер unknown, С. 123827 - 123827

Опубликована: Фев. 1, 2025

Язык: Английский

Процитировано

2