Intermetallic Nanocrystals for Fuel-Cells-Based Electrocatalysis

Chemical Reviews, Год журнала: 2023, Номер 123(22), С. 12507 - 12593

Опубликована: Ноя. 1, 2023

Electrocatalysis underpins the renewable electrochemical conversions for sustainability, which further replies on metallic nanocrystals as vital electrocatalysts. Intermetallic have been known to show distinct properties compared their disordered counterparts, and long explored functional improvements. Tremendous progresses made in past few years, with notable trend of more precise engineering down an atomic level investigation transferring into practical membrane electrode assembly (MEA), motivates this timely review. After addressing basic thermodynamic kinetic fundamentals, we discuss classic latest synthetic strategies that enable not only formation intermetallic phase but also rational control other catalysis-determinant structural parameters, such size morphology. We demonstrate emerging nanomaterials potentially advancement energy electrocatalysis. Then, state-of-the-art characterizations representative electrocatalysts emphasis oxygen reduction reaction evaluated a MEA setup. summarize review by laying out existing challenges offering perspective future research directions toward practicing conversions.

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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Photocoupled Electroreduction of CO₂ over Photosensitizer-Decorated Covalent Organic Frameworks

Journal of the American Chemical Society, Год журнала: 2023, Номер 145(36), С. 19856 - 19865

Опубликована: Авг. 31, 2023

Introducing an external visible-light field would be a promising strategy to improve the activity of electrocatalytic CO2 reduction reaction (CO2RR), but it still remains challenge due short excited-state lifetime active sites. Herein, Ru(bpy)3Cl2 struts as powerful photosensitive donors were immobilized into backbones Co-porphyrin-based covalent organic frameworks (named Co-Bpy-COF-Rux, x is molar ratio Ru and Co species, = 1/2 2/3) via coordination bonds, for photo-coupled CO2RR produce CO. The optimal Co-Bpy-COF-Ru1/2 displays high CO Faradaic efficiency 96.7% at -0.7 V vs reversible hydrogen electrode (RHE) partial current density 16.27 mA cm-2 -1.1 RHE under assistance light, both which far surpassing values observed in dark. significantly enhanced mainly attributed incorporation donor with long concomitantly giant built-in electric Co-Bpy-COF-Ru1/2, efficiently accelerate photo-induced electron transfer from cobalt-porphyrin light. Thus, sites have longer lower rate-determining steps' energy occurring during actual process. This first work porphyrin-based COFs CO2RR, opening new frontier construction efficient electrocatalysts.

Язык: Английский

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Recent progress of MOF-functionalized nanocomposites: From structure to properties

Advances in Colloid and Interface Science, Год журнала: 2023, Номер 323, С. 103050 - 103050

Опубликована: Ноя. 10, 2023

Язык: Английский

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Engineering organic polymers as emerging sustainable materials for powerful electrocatalysts

Chemical Society Reviews, Год журнала: 2024, Номер 53(3), С. 1447 - 1494

Опубликована: Янв. 1, 2024

A comprehensive overview on organic polymers as electrocatalysts is summarized. By presenting the engineering strategies, insightful understandings, challenges, and perspectives, we hope this review can provide valuable references for readers.

Язык: Английский

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Ultrafast Synthesis of Graphene‐Embedded Cyclodextrin‐Metal‐Organic Framework for Supramolecular Selective Absorbency and Supercapacitor Performance

Advanced Science, Год журнала: 2023, Номер 10(31)

Опубликована: Авг. 27, 2023

Limited by preparation time and ligand solubility, synthetic protocols for cyclodextrin-based metal-organic framework (CD-MOF), as well subsequent derived materials with improved stability properties, still remains a challenge. Herein, an ultrafast, environmentally friendly, cost-effective microwave method is proposed, which induced graphene oxide (GO) to design CD-MOF/GOs. This applicable technique can control the crystal size of CD-MOFs from macro- nanocrystals. CD-MOF/GOs are investigated new type supramolecular adsorbent. It selectively adsorb dye molecule methylene green (MG) owing synergistic effect between hydrophobic nanocavity CDs, abundant O-containing functional groups GO in composites. Following high temperature calcination, resulting N, S co-doped porous carbons exhibit capacitance 501 F g-1 at 0.5 A , stable cycling 90.1% capacity retention after 5000 cycles. The carbon exhibits good electrochemical performance due its surface containing numerous electrochemically active sites adsorption carbonization. strategy incorporating variety molecules into optimizes properties their materials, furthering development toward fabrication zeitgeisty high-performance energy storage devices.

Язык: Английский

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Electronic Structure Design of Transition Metal-Based Catalysts for Electrochemical Carbon Dioxide Reduction

ACS Nano, Год журнала: 2024, Номер 18(14), С. 9823 - 9851

Опубликована: Март 28, 2024

With the increasingly serious greenhouse effect, electrochemical carbon dioxide reduction reaction (CO2RR) has garnered widespread attention as it is capable of leveraging renewable energy to convert CO2 into value-added chemicals and fuels. However, performance CO2RR can hardly meet expectations because diverse intermediates complicated processes, necessitating exploitation highly efficient catalysts. In recent years, with advanced characterization technologies theoretical simulations, exploration catalytic mechanisms gradually deepened electronic structure catalysts their interactions intermediates, which serve a bridge facilitate deeper comprehension structure-performance relationships. Transition metal-based (TMCs), extensively applied in CO2RR, demonstrate substantial potential for further modulation, given abundance d electrons. Herein, we discuss representative feasible strategies modulate catalysts, including doping, vacancy, alloying, heterostructure, strain, phase engineering. These approaches profoundly alter inherent properties TMCs interaction thereby greatly affecting rate pathway CO2RR. It believed that rational design modulation fundamentally provide viable directions development toward conversion many other small molecules.

Язык: Английский

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Ionic Covalent Organic Frameworks in Adsorption and Catalysis

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(22)

Опубликована: Апрель 2, 2024

The ion extraction and electro/photo catalysis are promising methods to address environmental energy issues. Covalent organic frameworks (COFs) a class of template construct absorbents catalysts because their stable frameworks, high surface areas, controllable pore environments, well-defined catalytic sites. Among them, ionic COFs as unique crystalline porous materials, with charges in the or along walls, have shown different properties resulting performance these applications those from charge-neutral COFs. In this review, current research progress based on for conversion, including cationic/anionic materials is reviewed terms synthesis strategy, modification methods, mechanisms adsorption catalysis, well applications. Finally, we demonstrated challenges future development design strategies

Язык: Английский

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Lignin‐Metal Supramolecular Framework Strategy of Self‐Healing Carbon‐Coated CoRu Alloy Nanocatalyst for Efficient Overall Water Splitting

Advanced Energy Materials, Год журнала: 2024, Номер 14(32)

Опубликована: Июнь 19, 2024

Abstract Common precursors for carbon materials typically include petroleum‐based polymers or MOF materials. However, these often encounter challenges such as metal aggregation, high cost, and metals leaching. In this work, a novel of approach lignin‐metal supramolecular framework complex (MSF@Lignin) is introduced. These complexes are formed through oxidative ammonolysis lignin (OAL) to synthesize nitrogen‐doped carbon‐encapsulated CoRu nanocatalyst (CoRu@OALC) via in situ carbonization. CoRu@OALC exhibited exceptional performance both HER (90 mV) OER (200 at the current density 10 mA cm −2 , with an overall water splitting voltage 1.5 V outstanding stability under density. During pyrolysis process, became encapsulated by lignin‐derived carbon, occurring within temperature range 600–700 °C. catalytic active sites primarily located defects showcasing unique “self‐healing” phenomenon layer. Oxygen‐containing intermediates ( * OH, O, OOH) facilitated reconstruction on layer, while hydrogen‐containing H) contributed reappearance defect‐rich structure.

Язык: Английский

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