Recent advances in nanostructured heterogeneous catalysts for N-cycle electrocatalysis

Deleted Journal, Год журнала: 2022, Номер 1, С. e9120010 - e9120010

Опубликована: Май 30, 2022

To restore the natural nitrogen cycle (N-cycle), artificial N-cycle electrocatalysis with flexibility, sustainability, and compatibility can convert intermittent renewable energy (e.g., wind) to harmful or value-added chemicals minimal carbon emissions. The background of such N-cycles, as fixation, ammonia oxidation, nitrate reduction, is briefly introduced here. discussion emerging nanostructures in various conversion reactions focused on architecture/compositional design, electrochemical performances, reaction mechanisms, instructive tests. Energy device advancements for achieving more functions well in situ/operando characterizations toward understanding key steps are also highlighted. Furthermore, some recently proposed less discussed C–N coupling summarized. We classify inorganic sources that each other under an applied voltage into three types, namely, abundant nitrogen, toxic (nitrite), oxides, useful compounds ammonia, hydrazine, hydroxylamine, goal providing critical insights strategies facilitate development our circular economy.

Язык: Английский

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Unveiling the Synergy of O‐Vacancy and Heterostructure over MoO_3‐x/MXene for N₂ Electroreduction to NH₃

Advanced Energy Materials, Год журнала: 2021, Номер 12(3)

Опубликована: Дек. 21, 2021

Abstract The electrochemical N 2 reduction reaction (NRR) offers a promising approach for sustainable NH 3 production, and modulating the structural/electronic configurations of catalyst materials with optimized electrocatalytic properties is pivotal achieving high‐efficiency NRR electrocatalysis. Herein, vacancy heterostructure engineering are rationally integrated to explore O‐vacancy‐rich MoO 3‐ x anchored on Ti C T ‐MXene (MoO /MXene) as highly active selective electrocatalyst, an exceptional activity yield 95.8 µg h −1 mg (−0.4 V) Faradaic efficiency 22.3% (−0.3 V). A combination in situ spectroscopy, molecular dynamics simulations density functional theory computations employed unveil synergistic effect O‐vacancies heterostructures NRR, which demonstrates that serve sites chemisorption activation, while MXene substrate can further regulate O‐vacancy break scaling relation effectively stabilize *N /*N H destabilizing *NH /*NH , resulting more binding affinity intermediates toward reduced energy barriers enhanced /MXene.

Язык: Английский

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Ambient Ammonia Synthesis via Electrochemical Reduction of Nitrate Enabled by NiCo₂O₄ Nanowire Array

Small, Год журнала: 2022, Номер 18(13)

Опубликована: Фев. 10, 2022

NiCo2 O4 nanowire array on carbon cloth (NiCo2 /CC) is proposed as a highly active electrocatalyst for ambient nitrate (NO3- ) reduction to ammonia (NH3 ). In 0.1 m NaOH solution with NaNO3 , such /CC achieves high Faradic efficiency of 99.0% and large NH3 yield up 973.2 µmol h-1 cm-2 . The superior catalytic activity comes from its half-metal feature optimized adsorption energy due the existence Ni in crystal structure. A Zn-NO3- battery cathode also shows record-high performance.

Язык: Английский

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Recent Advances in Electrocatalysts for Efficient Nitrate Reduction to Ammonia

Advanced Functional Materials, Год журнала: 2023, Номер 33(43)

Опубликована: Июнь 25, 2023

Abstract Ammonia as an irreplaceable chemical has been widely demanded to keep the sustainable development of modern society. However, its industrial production consumes huge energy and releases extraordinary green‐house gases, leading various environmental issues. To achieve green ammonia is a great challenge that extensively pursued recently. In review, most promising strategy, electrochemical nitrate reduction reaction (e‐NO 3 RR) for purpose comprehensively investigated give full understanding mechanism provide guidance future directions. Particularly, electrocatalysts focused realize high yield rate Faraday efficiency applications. The recent‐developed catalysts, including noble metallic materials, alloys, metal compounds, single‐metal‐atom metal‐free are systematically discussed review effects factors on catalytic performance in e‐NO RR. Accordingly, strategies, defects engineering, coordination environment modulating, surface controlling, hybridization, carefully improve performance, such intrinsic activity selectivity. Finally, perspectives challenges given out. This shall insightful advanced systems efficiently industry.

Язык: Английский

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Lewis Acid Fe‐V Pairs Promote Nitrate Electroreduction to Ammonia

Advanced Functional Materials, Год журнала: 2023, Номер 33(13)

Опубликована: Янв. 18, 2023

Abstract Electrochemical reduction of nitrate to ammonia (NO 3 RR) has been recognized as an appealing approach realize both sustainable NH production and waste removal. Herein, from the perspective Lewis acid‐base interaction, a single‐atom Fe‐doped V 2 O 5 (Fe‐V ) catalyst enriched is designed with acid sites, which present maximum ‐Faradaic efficiency 97.1% corresponding yield 12.5 mg h −1 cm −2 at –0.7 versus RHE. Mechanistic studies based on theoretical calculations operando spectroscopic characterizations identify creation Fe‐V pairs , can synergetically activate NO − promote hydrogenation energetics, restrain hydrogen evolution, leading enhanced RR activity selectivity.

Язык: Английский

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High-efficiency ammonia electrosynthesis via selective reduction of nitrate on ZnCo2O4 nanosheet array

Materials Today Physics, Год журнала: 2022, Номер 23, С. 100619 - 100619

Опубликована: Янв. 26, 2022

Язык: Английский

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Sulfur-deficient Bi2S3−x synergistically coupling Ti3C2Tx-MXene for boosting electrocatalytic N2 reduction

Nano Research, Год журнала: 2022, Номер 15(5), С. 3991 - 3999

Опубликована: Фев. 8, 2022

Язык: Английский

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High-Efficiency Electrochemical Nitrate Reduction to Ammonia on a Co₃O₄ Nanoarray Catalyst with Cobalt Vacancies

ACS Applied Materials & Interfaces, Год журнала: 2022, Номер 14(41), С. 46595 - 46602

Опубликована: Окт. 5, 2022

Electrocatalytic nitrate reduction reaction (NO3RR) affords a bifunctional character in the carbon-free ammonia synthesis and remission of pollution water. Here, we fabricated Co3O4 nanosheet array with cobalt vacancies on carbon cloth (vCo-Co3O4/CC) by situ etching aluminum-doped Co3O4/CC, which exhibits an excellent Faradaic efficiency 97.2% large NH3 yield as high 517.5 μmol h-1 cm-2, better than pristine Co3O4/CC. Theoretical calculative results imply that can tune local electronic environment around Co sites Co3O4, increasing charge reducing electron cloud density sites, is thus conducive to adsorption NO3- for greatly enhanced reduction. Furthermore, vCo-Co3O4 (311) facet presents NO3RR activity low energy barrier about 0.63 eV potential-determining step, much smaller (1.3 eV).

Язык: Английский

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Recent progress and strategies on the design of catalysts for electrochemical ammonia synthesis from nitrate reduction

Inorganic Chemistry Frontiers, Год журнала: 2023, Номер 10(12), С. 3489 - 3514

Опубликована: Янв. 1, 2023

Ammonia (NH3) is an essential raw material in the production of fertilizers and a promising carbon-free energy carrier, however, its synthesis still depends on energy- capital-intensive Haber–Bosch process. Recently, electrochemical N2 reduction reaction has attracted significant interest as emerging method for NH3 under ambient conditions. However, limited solubility aqueous electrolyte strong NN bonds result low yield rate, inferior faradaic efficiency unsatisfactory selectivity, impeding further practical application. Considering high water nitrate (NO3−), NO3− (NO3−RR) become fascinating route achieving sustainable NH3, enormous progress been made this field. As consequence, review discusses mechanism systematically summarizes recent development electrocatalysts NO3−RR, including noble-metal-based materials, single-atom metal catalysts, transition-metal-based catalysts. Diverse design strategies catalysts to boost NO3−RR performance, such defect engineering, rational structure design, strain engineering constructing heterostructures, are discussed. This followed by illustration how robust understanding optimization affords fundamental insights into efficiency, selectivity electrocatalysts. Finally, we conclude with future perspectives critical issues, challenges research directions high-efficiency selective NH3.

Язык: Английский

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ITO@TiO2 nanoarray: An efficient and robust nitrite reduction reaction electrocatalyst toward NH3 production under ambient conditions

eScience, Год журнала: 2022, Номер 2(4), С. 382 - 388

Опубликована: Май 6, 2022

Ambient electrochemical nitrite (NO2-) reduction is viewed as an effective and sustainable approach for simultaneously removing NO2- producing ammonia (NH3). However, the complex multi-electron transfer steps involved in reaction (NO2-RR) lead to sluggish kinetics low product selectivity toward NH3, underscoring need NH3 synthesis electrocatalysts with high activity durability. Herein, we report amorphous indium–tin oxide sputtered on a TiO2 nanobelt array Ti plate ([email protected]2/TP) 3D NH3-producing catalyst NO2-. In 0.5 ​M LiClO4 0.1 NO2-, it shows greatly boosted NO2-RR production, excellent selectivity, achieving large yield of 411.3 ​μmol ​h−1 ​cm−2 Faradaic efficiency 82.6%. It also durability continuous electrolysis. A Zn‐NO2- battery [email protected]2/TP cathode offers 23.1 peak power density 1.22 ​mW ​cm−2.

Язык: Английский

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