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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Electrochemical Nitrate Reduction: Ammonia Synthesis and the Beyond

Advanced Materials, Год журнала: 2023, Номер 36(17)

Опубликована: Июнь 9, 2023

Natural nitrogen cycle has been severely disrupted by anthropogenic activities. The overuse of N-containing fertilizers induces the increase nitrate level in surface and ground waters, substantial emission oxides causes heavy air pollution. Nitrogen gas, as main component air, used for mass ammonia production over a century, providing enough nutrition agriculture to support world population increase. In last decade, researchers have made great efforts develop processes under ambient conditions combat intensive energy consumption high carbon associated with Haber-Bosch process. Among different techniques, electrochemical reduction reaction (NO

Язык: Английский

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Enabled Efficient Ammonia Synthesis and Energy Supply in a Zinc–Nitrate Battery System by Separating Nitrate Reduction Process into Two Stages

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(13)

Опубликована: Фев. 2, 2023

The aqueous electrocatalytic reduction of NO3- into NH3 (NitrRR) presents a sustainable route applicable to production and potentially energy storage. However, the NitrRR involves directly eight-electron transfer process generally required large overpotential (<-0.2 V versus reversible hydrogen electrode (vs. RHE)) reach optimal efficiency. Here, inspired by biological nitrate respiration, was separated two stages along [2+6]-electron pathway alleviate kinetic barrier. system employed Cu nanowire catalyst produces NO2- with current efficiencies 91.5 % 100 %, respectively at lower overpotentials (>+0.1 vs. RHE). high efficiency for such further explored in zinc-nitrate battery. This battery could be specified output voltage 0.70 V, an average density 566.7 Wh L-1 10 mA cm-2 power 14.1 mW , which is well beyond all previously reported similar concepts.

Язык: Английский

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Intermetallic Single-Atom Alloy In–Pd Bimetallene for Neutral Electrosynthesis of Ammonia from Nitrate

Journal of the American Chemical Society, Год журнала: 2023, Номер 145(25), С. 13957 - 13967

Опубликована: Июнь 19, 2023

Harvesting recyclable ammonia (NH3) from the electrocatalytic reduction of nitrate (NO3RR) offers a sustainable strategy to close ecological nitrogen cycle nitration contamination in an energy-efficient and environmentally friendly manner. The emerging intermetallic single-atom alloys (ISAAs) are recognized achieve highest site density single atoms by isolating contiguous metal into sites stabilized another within structure, which holds promise couple catalytic benefits nanocrystals catalysts for promoting NO3RR. Herein, ISAA In-Pd bimetallene, Pd isolated surrounding In atoms, is reported boost neutral NO3RR with NH3 Faradaic efficiency (FE) 87.2%, yield rate 28.06 mg h-1 mgPd-1, exceptional stability increased activity/selectivity over 100 h 20 cycles. structure induces substantially diminished overlap d-orbitals narrowed p-d hybridization In-p Pd-d states around Fermi level, resulting stronger NO3- adsorption depressed energy barrier potential-determining step Further integrating catalyst Zn-NO3- flow battery as cathode delivers power 12.64 mW cm-2 FE 93.4% production.

Язык: Английский

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Emerging Applications, Developments, Prospects, and Challenges of Electrochemical Nitrate‐to‐Ammonia Conversion

Advanced Functional Materials, Год журнала: 2023, Номер 33(29)

Опубликована: Апрель 23, 2023

Abstract Ammonia is not only an important feedstock for chemical industry but also a carbon‐free energy carrier and safe storage media hydrogen. Due to the advantages compared Haber–Bosch process, electrochemical NO 3 − ‐to‐NH conversion via nitrate reduction reaction (NO RR) received attention. Recently, “green hydrogen” generated from water electrolysis shows promise become future limited by safety of transportation. This review proposes can store renewable electric into NH , which potential solution solving puzzle Moreover, theoretical insights RR electrocatalyst design are discussed. Finally, challenges opportunities in this field elucidated. provides novel perspective accelerates development effective electrocatalysts conversion.

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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Electrochemical nitrate reduction in acid enables high-efficiency ammonia synthesis and high-voltage pollutes-based fuel cells

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

Опубликована: Дек. 5, 2023

Abstract Most current research is devoted to electrochemical nitrate reduction reaction for ammonia synthesis under alkaline/neutral media while the investigation of acidic conditions rarely reported. In this work, we demonstrate potential TiO 2 nanosheet with intrinsically poor hydrogen-evolution activity selective and rapid conditions. Hybridized iron phthalocyanine, resulting catalyst displays remarkably improved efficiency toward formation owing enhanced adsorption, suppressed hydrogen evolution lowered energy barrier rate-determining step. Then, an alkaline-acid hybrid Zn-nitrate battery was developed high open-circuit voltage 1.99 V power density 91.4 mW cm –2 . Further, environmental sulfur recovery can be powered by above hydrazine-nitrate fuel cell simultaneously hydrazine/nitrate conversion electricity generation. This work demonstrates attractive electrosynthesis broadens field conversion.

Язык: Английский

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A Zn–nitrite battery as an energy-output electrocatalytic system for high-efficiency ammonia synthesis using carbon-doped cobalt oxide nanotubes

Energy & Environmental Science, Год журнала: 2022, Номер 15(7), С. 3024 - 3032

Опубликована: Янв. 1, 2022

A Zn-NO 2 − battery with C/Co 3 O 4 catalyst cathode is developed as an energy-output electrocatalytic system that can simultaneously convert NO to NH high faradaic efficiency and supply electricity a power density of 6.03 mW cm −2 .

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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Laser-controlled tandem catalytic sites of CuNi alloys with ampere-level electrocatalytic nitrate-to-ammonia reduction activities for Zn–nitrate batteries

Energy & Environmental Science, Год журнала: 2023, Номер 16(7), С. 2991 - 3001

Опубликована: Янв. 1, 2023

Laser-constructed CuNi alloy electrodes with tandem sites of Ni provide H* and Cu for NO 3 − reduction, achieving ampere-level reduction high-performance Zn–NO batteries.

Язык: Английский

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