Abnormal CO2 and H2O Diffusion in CALF-20(Zn) Metal–Organic Framework: Fundamental Understanding of CO2 Capture DOI
Yann Magnin, Estelle Dirand, Guillaume Maurin

et al.

ACS Applied Nano Materials, Journal Year: 2023, Volume and Issue: 6(21), P. 19963 - 19971

Published: Oct. 31, 2023

Carbon mitigation is one challenging issue that the world facing. To tackle deleterious impacts of CO2, processes emerged, including chemisorption from amine-based solvents and, more recently, physisorption in nanoporous solids. Physisorption metal–organic frameworks (MOFs) currently attracting considerable attention; however, selection optimum sorbent still challenging. While CO2 adsorption by MOFs has been widely explored a thermodynamics standpoint, dynamical aspects remain less explored. CALF-20(Zn) MOF was recently proposed as promising alternative to commercially used 13X zeolite sorbents; an in-depth understanding nanoscopic mechanisms originating its good performance be achieved. do so, we deliver some insights into and diffusion H2O, mixtures CALF-20 through atomistic simulations. revealed exhibit unconventional guest–host behaviors give rise abnormal guest dynamics. The hydrophobic nature solid leads low water enthalpy at loading, followed continuous increase, driven strong hydrogen bonds, found arrange quasi 1D molecular wires nanoporosity, recalling behavior small-diameter carbon nanotubes. no superdiffusion compared nanotubes, this shown impact guest-loading coefficient profile, with presence minimum correlates inflection point isotherm corresponding H2O formation. Interestingly, coefficients were also same order magnitude, similar nonlinear profiles function loading. We further demonstrated for decreases increasing

Language: Английский

Fluorinated metal–organic frameworks for gas separation DOI
Abtin Ebadi Amooghin, Hamidreza Sanaeepur, Rafael Luque

et al.

Chemical Society Reviews, Journal Year: 2022, Volume and Issue: 51(17), P. 7427 - 7508

Published: Jan. 1, 2022

Fluorinated metal-organic frameworks (F-MOFs) as fast-growing porous materials have revolutionized the field of gas separation due to their tunable pore apertures, appealing chemical features, and excellent stability. A deep understanding structure-performance relationships is critical for synthesis development new F-MOFs. This review has focused on several strategies precise design F-MOFs with structures tuned specific purposes. First, basic principles concepts well structure, modification structure property are studied. Then, applications in adsorption membrane discussed. detailed account capabilities various gases governing provided. In addition, exceptional characteristics highly stable engineered size put into perspective fabricate selective membranes separation. Systematic analysis position revealed that benchmark most challenging separations. The outlook future directions science engineering challenges highlighted tackle issues overcoming trade-off between capacity/permeability selectivity a serious move towards industrialization.

Language: Английский

Citations

166
A rational design of functional porous frameworks for electrocatalytic CO2reduction reaction DOI
Changli Wang,

Zunhang Lv,

Wenxiu Yang

et al.

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 52(4), P. 1382 - 1427

Published: Jan. 1, 2023

Rational design of functional porous frameworks for electrocatalytic CO 2 reduction reaction.

Language: Английский

Citations

140
Merging molecular catalysts and metal–organic frameworks for photocatalytic fuel production DOI
Philip M. Stanley, Johanna Haimerl, Natalia B. Shustova

et al.

Nature Chemistry, Journal Year: 2022, Volume and Issue: 14(12), P. 1342 - 1356

Published: Nov. 28, 2022

Language: Английский

Citations

88
Charge and mass transport mechanisms in two-dimensional covalent organic frameworks (2D COFs) for electrochemical energy storage devices DOI
Hanyin Zhang, Yubo Geng, Jin Huang

et al.

Energy & Environmental Science, Journal Year: 2023, Volume and Issue: 16(3), P. 889 - 951

Published: Jan. 1, 2023

Understanding charge- and mass-transport processes in two-dimensional covalent organic frameworks to design better materials energy storage devices.

Language: Английский

Citations

88
Metal‐Corrole‐Based Porous Organic Polymers for Electrocatalytic Oxygen Reduction and Evolution Reactions DOI
Haitao Lei,

Qingxin Zhang,

Zuozhong Liang

et al.

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(24)

Published: March 31, 2022

Integrating molecular catalysts into designed frameworks often enables improved catalysis. Compared with porphyrin-based frameworks, metal-corrole-based have been rarely developed, although monomeric metal corroles are usually more efficient than porphyrin counterparts for the electrocatalytic oxygen reduction reaction (ORR) and evolution (OER). We herein report on porous organic polymers (POPs) as ORR OER electrocatalysts. M-POPs (M=Mn, Fe, Co, Cu) were synthesized by coupling 10-phenyl-5,15-(4-iodophenyl)corrole tetrakis(4-ethynylphenyl)methane. corrole monomers, displayed significantly enhanced catalytic activity stability. Co-POP outperformed other achieving four-electron a half-wave potential of 0.87 V vs. RHE reaching 10 mA cm-2 current density at 340 mV overpotential. This work is unparalleled to develop explore POPs

Language: Английский

Citations

85
MOFormer: Self-Supervised Transformer Model for Metal–Organic Framework Property Prediction DOI Creative Commons
Zhonglin Cao, Rishikesh Magar, Yuyang Wang

et al.

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(5), P. 2958 - 2967

Published: Jan. 27, 2023

Metal-organic frameworks (MOFs) are materials with a high degree of porosity that can be used for many applications. However, the chemical space MOFs is enormous due to large variety possible combinations building blocks and topology. Discovering optimal specific applications requires an efficient accurate search over countless potential candidates. Previous high-throughput screening methods using computational simulations like DFT time-consuming. Such also require 3D atomic structures MOFs, which adds one extra step when evaluating hypothetical MOFs. In this work, we propose structure-agnostic deep learning method based on Transformer model, named as MOFormer, property predictions MOFormer takes text string representation MOF (MOFid) input, thus circumventing need obtaining structure accelerating process. By comparing other descriptors such Stoichiometric-120 revised autocorrelations, demonstrate achieve state-of-the-art prediction accuracy all benchmarks. Furthermore, introduce self-supervised framework pretrains via maximizing cross-correlation between its representations structure-based crystal graph convolutional neural network (CGCNN) >400k publicly available data. Benchmarks show pretraining improves both models various downstream tasks. revealed more data-efficient quantum-chemical than CGCNN training data limited. Overall, provides novel perspective learning.

Language: Английский

Citations

81
Recent progress in host–guest metal–organic frameworks: Construction and emergent properties DOI

Xiao−Ting Liu,

Binbin Qian,

Da−Shuai Zhang

et al.

Coordination Chemistry Reviews, Journal Year: 2022, Volume and Issue: 476, P. 214921 - 214921

Published: Nov. 16, 2022

Language: Английский

Citations

75
Photochemistry Journey to Multielectron and Multiproton Chemical Transformation DOI
Shu‐Lin Meng, Chen Ye, Xu‐Bing Li

et al.

Journal of the American Chemical Society, Journal Year: 2022, Volume and Issue: 144(36), P. 16219 - 16231

Published: Sept. 2, 2022

The odyssey of photochemistry is accompanied by the journey to manipulate "electrons" and "protons" in time, space, energy. Over past decades, single-electron (1e-) photochemical transformations have brought marvelous achievements. However, as each photon absorption typically generates only one exciton pair, it exponentially challenging accomplish multielectron proton transformations. multistep differences thermodynamics kinetics urgently require us optimize light harvesting, expedite consecutive electron transfer, interaction catalysts with substrates, coordinate transfer furnish selective bond formations. Tandem catalysis enables orchestrating different events catalytic from subpicoseconds seconds, which facilitates redox chemistries brings consecutive, value-added reactivities. Joint efforts molecular material design, mechanistic understanding, theoretical modeling will bring synthetic opportunities for fuels, fertilizers, chemicals enhanced versatility, efficiency, selectivity, scalability, thus taking better advantage photons (i.e., sunlight) our sustainable society.

Language: Английский

Citations

74
Large‐area Free‐standing Metalloporphyrin‐based Covalent Organic Framework Films by Liquid‐air Interfacial Polymerization for Oxygen Electrocatalysis DOI

Jiaqi Tang,

Zuozhong Liang, Haonan Qin

et al.

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 62(1)

Published: Nov. 8, 2022

Synthesizing large-area free-standing covalent organic framework (COF) films is of vital importance for their applications but still a big challenge. Herein, we reported the synthesis large metalloporphyrin-based COF and oxygen electrocatalysis. The reaction meso-benzohydrazide-substituted metal porphyrins with tris-aldehyde linkers afforded at liquid-air interface. These can be scaled up to 3000 cm2 area display great mechanical stability structural integrity. Importantly, Co-porphyrin-based are efficient electrocatalytic O2 reduction evolution reactions. A flexible, all-solid-state Zn-air battery was assembled using showed high performance charge-discharge voltage gap 0.88 V 1 mA cm-2 under bent conditions (0° 180°). This work thus presents strategy synthesize functionalized quality uses in flexible electronics.

Language: Английский

Citations

73
Harvesting Blue Energy Based on Salinity and Temperature Gradient: Challenges, Solutions, and Opportunities DOI
Masoud Rastgar,

Kazem Moradi,

Cassie Burroughs

et al.

Chemical Reviews, Journal Year: 2023, Volume and Issue: 123(16), P. 10156 - 10205

Published: July 31, 2023

Greenhouse gas emissions associated with power generation from fossil fuel combustion account for 25% of global and, thus, contribute greatly to climate change. Renewable energy sources, like wind and solar, have reached a mature stage, costs aligning those fuel-derived but suffer the challenge intermittency due variability sunlight. This study aims explore viability salinity gradient power, or "blue energy", as clean, renewable source uninterrupted, base-load generation. Harnessing river estuaries worldwide could meet substantial portion electricity demand (approximately 7%). Pressure retarded osmosis (PRO) reverse electrodialysis (RED) are more prominent technologies blue harvesting, whereas thermo-osmotic conversion (TOEC) is emerging new promise. review scrutinizes obstacles encountered in developing osmotic using membrane-based methods presents potential solutions overcome challenges practical applications. While certain strategies shown promise addressing some these obstacles, further research still required enhance efficiency feasibility processes, enabling their large-scale implementation harvesting.

Language: Английский

Citations

73