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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Unveiling Cutting‐Edge Developments in Electrocatalytic Nitrate‐to‐Ammonia Conversion

Advanced Materials, Год журнала: 2024, Номер 36(16)

Опубликована: Янв. 11, 2024

The excessive enrichment of nitrate in the environment can be converted into ammonia (NH

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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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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Piezocatalytic Techniques in Environmental Remediation

Angewandte Chemie International Edition, Год журнала: 2022, Номер 62(5)

Опубликована: Ноя. 1, 2022

Abstract As a consequence of rapid industrialization throughout the world, various environmental pollutants have begun to accumulate in water, air, and soil. This endangers ecological environment earth, remediation has become an immediate priority. Among techniques, piezocatalytic which uniquely take advantage piezoelectric effect, attracted much attention. Piezoelectric effects allow pollutant degradation directly, while also enhancing photocatalysis by reducing recombination photogenerated carriers. In this Review, we provide comprehensive summary recent developments techniques for remediation. The origin effect as well classification materials their application are systematically summarized. We analyze potential underlying mechanisms. Finally, urgent problems future development discussed.

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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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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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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Iron Nanoparticles Protected by Chainmail‐structured Graphene for Durable Electrocatalytic Nitrate Reduction to Nitrogen

Angewandte Chemie International Edition, Год журнала: 2022, Номер 62(5)

Опубликована: Дек. 5, 2022

Abstract The electrochemical nitrate reduction reaction (NO 3 RR) is an appealing technology for regulating the nitrogen cycle. Metallic iron one of well‐known electrocatalysts NO RR, but it suffers from poor durability due to leaching and oxidation during electrocatalytic process. In this work, a graphene‐nanochainmail‐protected nanoparticle (Fe@Gnc) electrocatalyst reported. It displays superior removal efficiency high selectivity. Notably, catalyst delivers exceptional stability durability, with rate selectivity remained ≈96 % that first time after up 40 cycles (24 h cycle). As expected, conductive graphene nanochainmail provides robust protection internal active sites, allowing Fe@Gnc maintain its long‐lasting catalytic activity. This research proposes workable solution scientific challenge lasting ability iron‐based in large‐scale industrialization.

Язык: Английский

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