Metal–Organic Framework-Based Hierarchically Porous Materials: Synthesis and Applications

Chemical Reviews, Год журнала: 2021, Номер 121(20), С. 12278 - 12326

Опубликована: Июль 19, 2021

Metal-organic frameworks (MOFs) have been widely recognized as one of the most fascinating classes materials from science and engineering perspectives, benefiting their high porosity well-defined tailored structures components at atomic level. Although intrinsic micropores endow size-selective capability surface area, etc., narrow pores limit applications toward diffusion-control large-size species involved processes. In recent years, construction hierarchically porous MOFs (HP-MOFs), MOF-based composites, derivatives has captured widespread interest to extend conventional materials. this Review, advances in design, synthesis, functional are summarized. Their structural characters various applications, including catalysis, gas storage separation, air filtration, sewage treatment, sensing energy storage, demonstrated with typical reports. The comparison HP-MOFs traditional (e.g., zeolite, silica, carbons, metal oxides, polymers), subsisting challenges, well future directions research field, also indicated.

Язык: Английский

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Single-atom catalysis in advanced oxidation processes for environmental remediation

Chemical Society Reviews, Год журнала: 2021, Номер 50(8), С. 5281 - 5322

Опубликована: Янв. 1, 2021

This review presents the recent advances in synthetic strategies, characterisation, and computations of carbon-based single-atom catalysts, as well their innovative applications mechanisms advanced oxidation technologies.

Язык: Английский

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Bimetallic metal–organic frameworks and MOF-derived composites: Recent progress on electro- and photoelectrocatalytic applications

Coordination Chemistry Reviews, Год журнала: 2021, Номер 451, С. 214264 - 214264

Опубликована: Окт. 25, 2021

Язык: Английский

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Noble-metal single-atoms in thermocatalysis, electrocatalysis, and photocatalysis

Energy & Environmental Science, Год журнала: 2021, Номер 14(5), С. 2954 - 3009

Опубликована: Янв. 1, 2021

This review summarizes the recent advances about noble-metal single-atom catalysts in thermocatalysis, electrocatalysis, and photocatalysis.

Язык: Английский

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Single-Atom (Iron-Based) Catalysts: Synthesis and Applications

Chemical Reviews, Год журнала: 2021, Номер 121(21), С. 13620 - 13697

Опубликована: Окт. 13, 2021

Supported single-metal atom catalysts (SACs) are constituted of isolated active metal centers, which heterogenized on inert supports such as graphene, porous carbon, and oxides. Their thermal stability, electronic properties, catalytic activities can be controlled via interactions between the center neighboring heteroatoms nitrogen, oxygen, sulfur. Due to atomic dispersion amount required for catalysis decreased, thus offering new possibilities control selectivity a given transformation well improve catalyst turnover frequencies numbers. This review aims comprehensively summarize synthesis Fe-SACs with focus anchoring single atoms (SA) carbon/graphene supports. The characterization these advanced materials using various spectroscopic techniques their applications in diverse research areas described. When applicable, mechanistic investigations conducted understand specific behavior Fe-SACs-based highlighted, including use theoretical models.

Язык: Английский

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Synergistic Effect of Atomically Dispersed Ni–Zn Pair Sites for Enhanced CO₂ Electroreduction

Advanced Materials, Год журнала: 2021, Номер 33(41)

Опубликована: Авг. 31, 2021

Abstract Dual‐atom catalysts have the potential to outperform well‐established single‐atom for electrochemical conversion of CO 2 . However, lack understanding regarding mechanism this enhanced catalytic process prevents rational design high‐performance catalysts. Herein, an obvious synergistic effect in atomically dispersed Ni–Zn bimetal sites is observed. In situ characterization combined with density functional theory (DFT) calculations reveals that heteronuclear coordination modifies d‐states metal atom, narrowing gap between d‐band centre (ε d ) Ni (3d) orbitals and Fermi energy level ( E F strengthen electronic interaction at reaction interface, resulting a lower free barrier (Δ G thermodynamic pathway reduced activation as well fortified metal–C bonding kinetic pathway. Consequently, faradaic efficiency >90% obtained across broad window from − 0.5 1.0 V (vs RHE), reaching maximum 99% −0.8 V, superior Ni/Zn single‐metal sites.

Язык: Английский

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Synthesis Strategies, Catalytic Applications, and Performance Regulation of Single‐Atom Catalysts

Advanced Functional Materials, Год журнала: 2021, Номер 31(12)

Опубликована: Янв. 4, 2021

Abstract The recent dramatic increase in research on isolated metal atoms has received extensive scientific interest the new frontier of single‐atom catalysis. As newly advanced materials catalysis, catalysts (SACs) have enormous from perspectives both and industrial applications due to their remarkable activity. In addition, other catalytic properties single atoms, including stability selectivity, can be further improved by tuning electronic/geometric structures modulating metal–support interactions. SACs usually consist dispersed appropriate support materials, which are employed anchor, confine, and/or coordinate with atoms. Therefore, nature sites allows acquiring a maximum atom utilization approaching 100%, is significance, particularly for development noble‐metal‐based catalysts. order systematically understand structure–property relationships underlying mechanisms relationship SACs, representative efforts synthesis strategies, applications, performance regulation discussed here. Typical catalysis processes corresponding electrochemistry, photochemistry, organic synthesis, biomedicine also summarized. Finally, challenges prospects highlighted.

Язык: Английский

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Atomic Fe–N₄/C in Flexible Carbon Fiber Membrane as Binder‐Free Air Cathode for Zn–Air Batteries with Stable Cycling over 1000 h

Advanced Materials, Год журнала: 2021, Номер 34(5)

Опубликована: Ноя. 17, 2021

Noble-metal-free, durable, and high-efficiency electrocatalysts for oxygen reduction evolution reaction (ORR/OER) are vital rechargeable Zn-air batteries (ZABs). Herein, a flexible free-standing carbon fiber membrane immobilized with atomically dispersed Fe-N4 /C catalysts (Fe/SNCFs-NH3 ) is synthesized used as air cathode ZABs. The intertwined fibers hierarchical nanopores facilitate the gas transportation, electrolyte infiltration electron transfer. large specific surface area exposes high concentration of sites embedded in matrix. Modulation local atomic configurations by sulfur doping Fe/SNCFs-NH3 catalyst leads to excellent ORR enhanced OER activities. as-synthesized demonstrates positive half-wave potential 0.89 V small Tafel slope 70.82 mV dec-1 , outperforming commercial Pt/C (0.86 V/94.74 most reported M-Nx (M = Fe, Co, Ni) catalysts. Experimental characterizations theoretical calculations uncover crucial role S regulating liquid-state ZABs deliver peak power density 255.84 mW cm-2 long-term cycle durability over 1000 h. Solid-state ZAB shows stable cycling at various flat/bent/flat states, demonstrating great prospects electronic device applications.

Язык: Английский

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Heterogenisation of polyoxometalates and other metal-based complexes in metal–organic frameworks: from synthesis to characterisation and applications in catalysis

Chemical Society Reviews, Год журнала: 2021, Номер 50(10), С. 6152 - 6220

Опубликована: Янв. 1, 2021

This review provides a thorough overview of composites with molecular catalysts (polyoxometalates, or organometallic coordination complexes) immobilised into MOFs via non-covalent interactions.

Язык: Английский

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Single‐Atom Catalysts: A Sustainable Pathway for the Advanced Catalytic Applications

Small, Год журнала: 2021, Номер 17(16)

Опубликована: Фев. 24, 2021

A heterogeneous catalyst is a backbone of modern sustainable green industries; and understanding the relationship between its structure properties key for advancement. Recently, many upscaling synthesis strategies development variety respectable control atomically precise catalysts are reported explored various important applications in catalysis energy environmental remediation. Precise atomic-scale has allowed to significantly increase activity, selectivity, some cases stability. This approach proved be relevant related technologies such as fuel cell, chemical reactors organic synthesis, Therefore, this review aims critically analyze recent progress on single-atom (SACs) application oxygen reduction reaction, evolution hydrogen and/or electrochemical transformations. Finally, opportunities that may open up future summarized, along with suggesting new possible exploitation SACs.

Язык: Английский

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