Metal-organic framework nanocrystal-derived hollow porous materials: Synthetic strategies and emerging applications

The Innovation, Год журнала: 2022, Номер 3(5), С. 100281 - 100281

Опубликована: Июль 6, 2022

Язык: Английский

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Recent advances on electrocatalytic CO2 reduction to resources: Target products, reaction pathways and typical catalysts

Chemical Engineering Journal, Год журнала: 2022, Номер 453, С. 139663 - 139663

Опубликована: Окт. 8, 2022

Язык: Английский

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Atomically Dispersed Metal‐Based Catalysts for Zn–CO₂Batteries

Small Structures, Год журнала: 2022, Номер 3(12)

Опубликована: Авг. 19, 2022

Rechargeable aqueous Zn–CO 2 batteries show great promise in meeting severe environmental problems and energy crises due to their combination of CO utilization output, as well advantages high theoretical density, abundant raw materials, safety. Developing high‐efficiency stable reduction reaction (CO RR) electrocatalysts is critical importance for the promotion this technology. Atomically dispersed metal‐based catalysts (ADMCs), with extremely atom‐utilization efficiency, tunable coordination environments, superior intrinsic catalytic activity, are emerging promising candidates batteries. Herein, some recent developments atomically summarized, including transition metal non‐transition sites. Moreover, various synthetic strategies, characterization methods, relationship between active site structures RR activity/Zn–CO battery performance introduced. Finally, challenges perspectives also proposed future development ADMCs

Язык: Английский

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Single‐Product Faradaic Efficiency for Electrocatalytic of CO₂ to CO at Current Density Larger than 1.2 A cm⁻² in Neutral Aqueous Solution by a Single‐Atom Nanozyme

Angewandte Chemie International Edition, Год журнала: 2022, Номер 61(44)

Опубликована: Сен. 7, 2022

Electroreduction of CO2 to CO is a promising approach for the cycling use , while it still suffers from impractical current density and durability. Here we report single-atom nanozyme (Ni-N5 -C) that achieves industrial-scale performance -to-CO conversion with Faradaic efficiency (FE) exceeded 97 % over -0.8--2.4 V vs. RHE. The at -2.4 RHE reached maximum 1.23 A cm-2 (turnover frequency 69.7 s-1 ) an FE 99.6 %. No obvious degradation was observed 100 hours continuous operation. Compared planar Ni-N4 site, square-pyramidal Ni-N5 site has increase decrease in dz2${{{\rm d}}_{{z}^{2}}}$ dxz/yz orbital energy levels, respectively, as revealed by functional theory calculations. Thus, catalytic more superior activate molecule reduce barriers well promote desorption, thus boosting kinetic activation process activity.

Язык: Английский

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Carbon Catalysts for Electrochemical CO₂ Reduction toward Multicarbon Products

Advanced Energy Materials, Год журнала: 2022, Номер 12(24)

Опубликована: Май 1, 2022

Abstract Electrochemical CO 2 reduction offers a compelling route to mitigate atmospheric concentration and store intermittent renewable energy in chemical bonds. Beyond C 1 , 2+ feedstocks are more desirable due their higher density significant market need. However, the ‐to‐C suffers from barriers of CC coupling complex reaction pathways. Due remarkable tunability over morphology/pore architecture along with great feasibility functionalization modify electronic geometric structures, carbon materials, serving as active components, supports, promoters, provide exciting opportunities tune both adsorption properties intermediates local environment for reduction, offering effective solutions enable steer evolution. general design principles remain ambiguous, causing an impediment rational catalyst refinement application thrusts. This review clarifies insightful advancing materials. First, current performance status challenges discussed strategies outlined promote Further, correlation between composition, structure, morphology catalysts catalytic behavior is elucidated establish mechanisms critical factors determining performance. Finally, future research directions envisioned inspire revolutionary advancements.

Язык: Английский

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Convergent paired electrosynthesis of dimethyl carbonate from carbon dioxide enabled by designing the superstructure of axial oxygen coordinated nickel single-atom catalysts

Energy & Environmental Science, Год журнала: 2022, Номер 16(2), С. 502 - 512

Опубликована: Дек. 22, 2022

A dual-channel superstructured Ni single-atom catalyst with a unique axial oxygen coordination configuration was controllably constructed and affords preeminent performance for convergent paired electrosynthesis of dimethyl carbonate from CO 2 .

Язык: Английский

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Direct OC-CHO coupling towards highly C2+ products selective electroreduction over stable Cu0/Cu2+ interface

Nature Communications, Год журнала: 2023, Номер 14(1)

Опубликована: Ноя. 24, 2023

Electroreduction of CO2 to valuable multicarbon (C2+) products is a highly attractive way utilize and divert emitted CO2. However, major fraction C2+ selectivity confined less than 90% by the difficulty coupling C-C bonds efficiently. Herein, we identify stable Cu0/Cu2+ interfaces derived from copper phosphate-based (CuPO) electrocatalysts, which can facilitate production with low-energy pathway OC-CHO verified in situ spectra studies theoretical calculations. The CuPO precatalyst shows high Faradaic efficiency (FE) 69.7% towards C2H4 an H-cell, exhibits significant FEC2+ 90.9% under industrially relevant current density (j = -350 mA cm-2) flow cell configuration. interface breaks new ground for structural design electrocatalysts construction synergistic active sites improve activity products.

Язык: Английский

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Atomic Distance Engineering in Metal Catalysts to Regulate Catalytic Performance

Advanced Materials, Год журнала: 2023, Номер 36(3)

Опубликована: Окт. 2, 2023

Abstract It is very important to understand the structure–performance relationship of metal catalysts by adjusting microstructure at atomic scale. The distance has an essential influence on composition environment active atom, which a key factor for design targeted with desired function. In this review, we discuss and summarize strategies changing from three aspects relate their effects reactivity catalysts. First, regulating bond length between coordination atom one single‐atom site catalytic performance are introduced. lengths affected strain effect support high‐shell doping can evolve during reaction. Next, sites discussed. Due space matching adsorption electron transport, be adjusted shortening distance. addition, arrangement spacing surface atoms nanocatalysts studied. Finally, comprehensive summary outlook given.

Язык: Английский

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Recent progress on ZIF-8 based MOF derivatives for electrocatalysis

Coordination Chemistry Reviews, Год журнала: 2023, Номер 499, С. 215492 - 215492

Опубликована: Окт. 27, 2023

Язык: Английский

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Highly Ordered Hierarchical Porous Single‐Atom Fe Catalyst with Promoted Mass Transfer for Efficient Electroreduction of CO₂

Advanced Energy Materials, Год журнала: 2023, Номер 13(37)

Опубликована: Авг. 10, 2023

Abstract Electrocatalysts are crucial to drive the electrochemical carbon dioxide reduction reaction (CO 2 RR) which lower energy barrier, tune intricate pathways and suppress competitive side‐reaction. Beyond efficient active sites advantageous local environment, a rapid mass transfer ability is also for catalyst design. However, it rare that research has been done investigate in detail process CO RR, expose underlying relationship between final performance. Here, single‐atom Fe‐N‐C shown with highly ordered porous substrate containing hierarchical micropores, mesopores, macropores. Such delicate structure significantly facilitates toward isolated Fe sites, achieving excellent RR performance, especially limited region H‐cell maximum partial current density of ‐19 mA cm −2 . Operando impedance spectroscopy relevant distributed relaxation times analysis reveal rapidly decreased resistance increase potential. The Lattice Boltzmann method Discrete Element (LBM‐DEM) simulations further performed exhibit origin enhanced performance from facilitated gas diffusion process.

Язык: Английский

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