Achieving Near 100% Faradaic Efficiency of Electrocatalytic Nitrate Reduction to Ammonia on Symmetry-Broken Medium-Entropy-Alloy Metallene

ACS Catalysis, Год журнала: 2024, Номер 14(10), С. 7907 - 7916

Опубликована: Май 6, 2024

Electrochemical nitrate reduction (NO3RR) offers an ecofriendly way for ammonia production. However, improving the sluggish kinetics of such a multistep reaction still remains challenging. Herein, asymmetry strategy is proposed to adjust charge distribution active centers on metallene by presenting novel symmetry-broken medium-entropy-alloy (MEA) via heteroatom alloying. Benefiting from maximized exposure well-regulated sites, proof-of-concept PdCuCo MEA delivers near 100% NH3 Faradaic efficiency in both neutral and alkaline electrolytes, along with record-high yield rate over 532.5 mg h–1 mgcat–1. Moreover, it enables 99.7% conversion industrial wastewater level 6200 ppm drinkable water level. Detailed studies further revealed that redistribution induced elemental electronegativity difference metallene, which will weaken N–O bond *NO, thus reducing energy barrier rate-determining step. Meanwhile, competitive HER formation NO2– are also hindered. We believe our this work shed light design efficient NO3RR catalysts more practical

Язык: Английский

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Acidic electroreduction CO2 to formic acid via interfacial modification of Bi nanoparticles at industrial-level current

Nano Research, Год журнала: 2024, Номер 17(7), С. 5817 - 5825

Опубликована: Март 23, 2024

Язык: Английский

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High Fire‐Safety and Multifunctional Eutectogel for Flexible Quasi‐Solid‐State Supercapacitors

Advanced Functional Materials, Год журнала: 2024, Номер unknown

Опубликована: Авг. 10, 2024

Abstract The preparation of high‐performance and fire‐safe electrolytes for flexible quasi‐solid‐state supercapacitors is challenging. In this work, a novel multifunctional deep eutectic solvent gel (DESG) fabricated using acrylic acid urea as hydrogen bond donors choline chloride acceptor. DESG shows high ionic conductivity (0.552 S m −1 ), good electrochemical performance (specific capacitance: 106.8 F g wide operating temperature range (−20–90 °C), being promising candidate solid‐state supercapacitors. Furthermore, it exhibits thermoelectric conversion capability (Seebeck coefficient: 1.56 mV K ideal capacitors fire‐warning sensors. prepared rapidly self‐extinguishes after removal from fire, reaching limiting oxygen index value 38.0% demonstrating its excellent flame retardancy. addition, has self‐healing (healing efficiency 84.3%). work provides new insights into the application fire‐safety eutectogels

Язык: Английский

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Efficient acidic CO2 electroreduction to formic acid by modulating electrode structure at industrial-level current

Chemical Engineering Journal, Год журнала: 2024, Номер 489, С. 151238 - 151238

Опубликована: Апрель 14, 2024

Язык: Английский

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Microenvironment Modulation of Ultrathin Bronze‐Phase TiO₂ Nanosheets for Highly Selective Photocatalytic CO₂ Reduction in Water

Advanced Functional Materials, Год журнала: 2023, Номер 34(9)

Опубликована: Ноя. 21, 2023

Abstract Photocatalytic reduction of CO 2 with H O provides a promising and sustainable pathway to produce valuable chemicals fuels. However, the low efficiency concomitant competition evolution pose serious challenges practical applications. Herein, novel approach is proposed modulate surface microenvironment photocatalysts by utilizing hydrogen peroxide (H ). A bronze‐phase TiO (TB) composed ultrathin nanosheet thickness ∼3 nm fabricated employed as model catalyst for photocatalytic reduction. molecules are presumed be bonded TB form TB‐H (TBHO) active specie. The newly generated TBHO enhances adsorption accelerates mass transfer, weakly acidic serves purpose mediating proton‐coupled electron transfer path. Consequently, nanosheets assisted show an excellent generation rate 29.1 µmol −1 g h (which 11.2‐fold higher than that pure TB) in water, selectivity toward nearly 100%. This work underscores importance tailoring promote while minimizing water.

Язык: Английский

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Single‐atom catalysts for the electrochemical reduction of carbon dioxide into hydrocarbons and oxygenates

Carbon Energy, Год журнала: 2023, Номер 6(3)

Опубликована: Сен. 6, 2023

Abstract The electrochemical reduction of carbon dioxide offers a sound and economically viable technology for the electrification decarbonization chemical fuel industries. In this technology, an electrocatalytic material renewable energy‐generated electricity drive conversion into high‐value chemicals carbon‐neutral fuels. Over past few years, single‐atom catalysts have been intensively studied as they could provide near‐unity atom utilization unique catalytic performance. Single‐atom become one state‐of‐the‐art catalyst materials monoxide. However, it remains challenge to facilitate efficient products beyond review, we summarize present important findings critical insights from studies on reaction hydrocarbons oxygenates using catalysts. It is hoped that review gives thorough recapitulation analysis science behind catalysis more reduced through so can be guide future research development with industry‐ready performance

Язык: Английский

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Electrifying the future: the advances and opportunities of electrocatalytic carbon dioxide reduction in acid

Science China Chemistry, Год журнала: 2023, Номер 66(12), С. 3426 - 3442

Опубликована: Сен. 26, 2023

Язык: Английский

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Covalent Phenanthroline‐Porphyrin Polymer for Aminocarbonylation through Electro/Thermocatalytic Tandem Processes: Extending Chemical Valorization of CO₂

Advanced Functional Materials, Год журнала: 2024, Номер 34(25)

Опубликована: Фев. 4, 2024

Abstract The covalent organic frameworks/polymers configurated with metal‐N 4 conjugated structures offer an exceptional platform for efficient electrochemical CO 2 reduction reaction (eCO RR). However, understanding the impact of structure‐mediated local microenvironment and integrating electroreduction follow‐up utilization toward extending chemical valorization are still far from sufficient. Herein, a set phenanthroline‐porphyrin polymers designed to decode modulation originating built‐in structures, optimized one delivered extraordinary performance eCO RR ≈100% Faradaic efficiency under stabilized ‐electrolysis 70 h. experimental theoretical analyses suggest that regulation Co‐N electronic convoys formation key intermediate * COOH. Furthermore, through CO‐mediated electro/thermocatalytic tandem processes, aminocarbonylation aryl iodides amines high yields has been convincingly implemented over coordinated Pd sites, which is remarkably helpful propel .

Язык: Английский

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Recent advances in pulsed electrochemical techniques: Synthesis of electrode materials and electrocatalytic reactions

Surfaces and Interfaces, Год журнала: 2024, Номер 50, С. 104519 - 104519

Опубликована: Май 22, 2024

Язык: Английский

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Recent Advances in Electrocatalysts for Sustainable Electrosynthesis of Ammonia and Urea from Ambient Nitrite Reduction and C–N Coupling

ACS Materials Letters, Год журнала: 2023, Номер 5(12), С. 3347 - 3363

Опубликована: Ноя. 21, 2023

The global nitrogen cycle has been destroyed by the quickly growing anthropogenic emissions of nitrite-containing pollutants during past decades, which causes numerous unexpected environmental side effects and threatens human health. Compared with conventional nitrite removal methods featuring low efficiency, high cost, secondary pollution, electrocatalytic reduction reaction garnered significant attention offers an appealing solution for recovering balance. Moreover, it takes a step further to convert into recyclable nitrogen-containing fertilizer including ammonia urea. However, materials design mechanistic aspects such emerging complex reactions are yet be explored compared other well-studied primary as oxygen water splitting. To address this challenge, review provides comprehensive account sustainable electrosynthesis urea from ambient C–N coupling. two key reactions, namely production synthesis coreduction carbon dioxide, elaborated in detail, available catalysts focus discussion. current technical barriers potential research prospects domain, exploring excellent electrocatalysts activity selectivity, precisely controlling interfacial microenvironment, understanding in-depth mechanism, highlighted.

Язык: Английский

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