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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Atomically dispersed Mn–N_x catalysts derived from Mn‐hexamine coordination frameworks for oxygen reduction reaction

Carbon Energy, Год журнала: 2024, Номер 6(5)

Опубликована: Янв. 10, 2024

Abstract Metal‐organic frameworks recently have been burgeoning and used as precursors to obtain various metal–nitrogen–carbon catalysts for oxygen reduction reaction (ORR). Although rarely studied, Mn–N–C is a promising catalyst ORR due its weak Fenton activity strong graphitization catalysis. Here, we developed facile strategy anchoring the atomically dispersed nitrogen‐coordinated single Mn sites on carbon nanosheets (MnNCS) from an Mn‐hexamine coordination framework. The Mn–N 4 were ultrathin with hierarchically porous structure. optimized MnNCS displayed excellent performance in half‐cells (0.89 V vs. reversible hydrogen electrode (RHE) base 0.76 RHE acid half‐wave potential) Zn–air batteries (233 mW cm −2 peak power density), along significantly enhanced stability. Density functional theory calculations further corroborated that –C 12 site has favorable adsorption of *OH rate‐determining step. These findings demonstrate metal‐hexamine framework can be model system rational design highly active atomic metal energy applications.

Язык: Английский

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Destabilization of Single‐Atom Catalysts: Characterization, Mechanisms, and Regeneration Strategies

Advanced Materials, Год журнала: 2025, Номер unknown

Опубликована: Янв. 19, 2025

Abstract Numerous in situ characterization studies have focused on revealing the catalytic mechanisms of single‐atom catalysts (SACs), providing a theoretical basis for their rational design. Although research is relatively limited, stability SACs under long‐term operating conditions equally important and prerequisite real‐world energy applications, such as fuel cells water electrolyzers. Recently, there has been rise destabilization regeneration SACs; however, timely comprehensive summaries that provide catalysis community with valuable insights directions are still lacking. This review summarizes recent advances strategies SACs, specifically highlighting various state‐of‐the‐art techniques employed studies. The factors induce identified by discussing failure active sites, coordination environments, supports, reaction scenarios. Next, primary introduced, including redispersion, surface poison desorption, exposure subsurface sites. Additionally, advantages limitations both ex discussed. Finally, future proposed, aimed at constructing structure–stability relationships guiding design more stable SACs.

Язык: Английский

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Cyclodextrin‐supported Co(OH)₂ Clusters as Electrocatalysts for Efficient and Selective H₂O₂ Synthesis

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(37)

Опубликована: Июль 5, 2023

Co-based material catalysts have shown attractive application prospects in the 2 e- oxygen reduction reaction (ORR). However, for industrial synthesis of H2 O2 , there is still lack with high production yield rate. Here, novel cyclodextrin-supported Co(OH)2 cluster were prepared via a mild and facile method. The catalyst exhibited remarkable selectivity (94.2 % ~ 98.2 %), good stability (99 activity retention after 35 h), ultra-high rate (5.58 mol gcatalyst-1 h-1 H-type electrolytic cell), demonstrating its promising potential. Density functional theory (DFT) reveals that cyclodextrin-mediated electronic structure optimizes adsorption OOH* intermediates significantly enhances activation energy barrier dissociation, leading to reactivity ORR. This work offers valuable practical strategy design electrocatalysts production.

Язык: Английский

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High‐rate Electrochemical H ₂ O ₂ Production over Multi‐metallic Atom Catalysts Under Acidic‐Neutral Conditions

Carbon Energy, Год журнала: 2023, Номер 6(1)

Опубликована: Март 24, 2023

Abstract Hydrogen peroxide (H 2 O ) production by the electrochemical 2‐electron oxygen reduction reaction (2e − ORR) is a promising alternative to energy‐intensive anthraquinone process, and single‐atom electrocatalysts show unique capability of high selectivity toward 2e ORR against 4e one. The extremely low surface density sites inflexibility in manipulating their geometric/electronic configurations, however, compromise H yield impede further performance enhancement. Herein, we construct family multiatom catalysts (MACs), on which two or three single atoms are closely coordinated form high‐density active that versatile atomic configurations for optimal adsorption essential *OOH species. Among them, Co x –Ni MAC presents excellent electrocatalytic ORR, terms its exceptionally acidic electrolytes (28.96 mol L −1 g cat. h under neutral conditions wide potential region (>80%, 0–0.7 V). Operando X‐ray absorption functional theory analyses jointly unveil trimetallic NiN 8 configuration, efficiently induces an appropriate Ni–d orbital filling modulates adsorption, together boosting capability. This work thus provides new strategy tuning structure other processes.

Язык: Английский

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Engineering Symmetry-Breaking Centers and d-Orbital Modulation in Triatomic Catalysts for Zinc-Air Batteries

ACS Nano, Год журнала: 2024, Номер unknown

Опубликована: Фев. 5, 2024

Unraveling the configuration–activity relationship and synergistic enhancement mechanism (such as real active center, electron spin-state, d-orbital energy level) for triatomic catalysts, well their intrinsically bifunctional oxygen electrocatalysis, is a great challenge. Here we present catalyst (TAC) with trinuclear structure that displays extraordinary electrocatalysis reduction reaction (ORR) evolution (OER), greatly outperforming counterpart of single-atom diatomic catalysts. The aqueous Zn-air battery (ZAB) equipped TAC-based cathode exhibits rechargeable stability ultrarobust cycling performance (1970 h/3940 cycles at 2 mA cm–2, 125 h/250 10 cm–2 negligible voltage decay), quasi-solid-state ZAB outstanding rechargeability low-temperature adaptability (300 h/1800 −60 °C), other state-of-the-art ZABs. experimental theoretical analyses reveal symmetry-breaking CoN4 configuration under incorporation neighboring metal atoms (Fe Cu), which leads to modulation, low-shift d band weakened binding strength intermediates, decreased barrier electrocatalysis. This rational tricoordination design an in-depth analysis indicate hetero-TACs can be promisingly applied in various applications.

Язык: Английский

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MOF-Derived Cobalt Nanoparticles with Dispersed Iron Phthalocyanines as Bifunctional Oxygen Electrocatalysts

ACS Sustainable Chemistry & Engineering, Год журнала: 2024, Номер 12(11), С. 4779 - 4788

Опубликована: Март 7, 2024

Iron phthalocyanine (FePc), characterized by its distinctive Fe–N4 sites, represents a macromolecular catalyst with promising applications in bifunctional oxygen catalysis. However, inherently flat and symmetrical configuration often results relatively weak electrocatalytic performance. In this study, novel approach was employed first anchoring the Co-based zeolitic imidazolate framework onto microsized carbon spheres derived from Zn-based coordination polymer, followed incorporation of dispersed FePc molecules. The resultant catalyst, denoted as FePc-CoNC-CMS, exhibited remarkable reduction reaction/oxygen evolution reaction (ORR/OER) activity an alkaline medium, notably achieving half-wave potential 0.87 V overpotential 313 mV at 10 mA cm–2. Both experimental theoretical investigations revealed that presence on cobalt surface induced significant alterations electron distribution within Fe center, thereby regulating adsorption affinity sites toward oxygen. This structural modification led to outstanding activity. When applied zinc–air batteries, it demonstrated excellent power density 147.6 mW cm–2 satisfactory charge–discharge stability over period 70 h pioneering work integrates metal–organic framework-derived metal–carbon nanomaterials catalysts, offering efficient pathway for multifunctional applications.

Язык: Английский

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Mesoporous high-entropy-alloy electrocatalysts via electrospinning for enhanced alkaline water electrolysis

Fuel, Год журнала: 2025, Номер 391, С. 134800 - 134800

Опубликована: Фев. 21, 2025

Язык: Английский

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Metalation of functionalized benzoquinoline-linked COFs for electrocatalytic oxygen reduction and lithium-sulfur batteries

Journal of Colloid and Interface Science, Год журнала: 2023, Номер 650, С. 1466 - 1475

Опубликована: Июль 17, 2023

Язык: Английский

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Recent progress in functional metal–organic frameworks for bio-medical application

Regenerative Biomaterials, Год журнала: 2023, Номер 11

Опубликована: Дек. 23, 2023

Abstract Metal–organic frameworks (MOFs) have a high specific surface area, adjustable pores and can be used to obtain functional porous materials with diverse well-ordered structures through coordination self-assembly, which has intrigued wide interest in broad range of disciplines. In the arena biomedical engineering, functionalized modification MOFs produced drug carriers excellent dispersion functionalities such as target delivery response release, promising applications bio-detection, disease therapy, tissue healing, other areas. This review summarizes present state research on functionalization by physical binding or chemical cross-linking small molecules, polymers, biomacromolecules, hydrogels evaluates role approach boosting reactivity materials. On this basis, application composites engineering fields delivery, repair, treatment, bio-detection imaging is surveyed, development trend prospects an important new class field are anticipated, may provide some inspiration reference for further MOF bio-medical applications.

Язык: Английский

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