Unraveling the Role of Intrinsic Carbon Defects for the Heterogeneous Reduction of NO with NH 3 DOI

Ruyi Zhao,

Chuanjin Zhao,

Hai Zhang

et al.

Combustion Science and Technology, Journal Year: 2024, Volume and Issue: unknown, P. 1 - 17

Published: Aug. 27, 2024

This study investigates the impact of intrinsic carbon defects on reduction nitrogen oxides (NOx) during coal combustion, with a focus synergistic effect ammonia (NH3) and pulverized coal. Two representative computational models containing are described, their influence NH3 NO is studied. Stable species transition states present in pathways calculated using B3LYP/6-31 G(d). Results indicate that exposed edge atoms exhibit higher charge density distribution, affecting adsorption reduction. The maximum energy barriers for both do not exceed 45 kcal/mol, achievable practical combustion systems. paper also calculates heterogeneous process model without (Char model), aim observing specific effects processes migration H/O atoms, recombination N formation desorption N2 molecules. Furthermore, analyses demonstrated an increase rate defective surfaces comparison to Char/NH/NO system, indicating have contributory catalytic activity. With regard magnitude reaction increasing temperature, presence base serves reinforce role temperature rate-determining step. Overall, this provides insights into carbon-based catalysis offers implications oxide emission control strategies.

Language: Английский

Interfacial Electronic Interactions Promoted Activation for Nitrate Electroreduction to Ammonia over Ag‐modified Co3O4 DOI Open Access

Zhenhai Fan,

Chunmei Cao,

Xingchuan Yang

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(44)

Published: Aug. 7, 2024

Abstract Electrocatalytic nitrate (NO 3 − ) reduction to ammonia (NRA) offers a promising pathway for synthesis. The interfacial electronic interactions (IEIs) can regulate the physicochemical capabilities of catalysts in electrochemical applications, while impact IEIs on electrocatalytic NRA remains largely unexplored current literature. In this study, high‐efficiency electrode Ag‐modified Co O 4 (Ag 1.5 Co/CC) is prepared neutral media, exhibiting an impressive conversion rate 96.86 %, Faradaic efficiency 96.11 and selectivity ~100 %. Notably, intrinsic activity Ag Co/CC ~81 times that nanoparticles (Ag/CC). Multiple characterizations theoretical computations confirm presence between , which stabilize CoO 6 octahedrons within significantly promote adsorption reactants as well intermediates 2 NO), suppressing Heyrovsky step, thereby improving electroreduction efficiency. Furthermore, our findings reveal synergistic effect different active sites enables tandem catalysis NRA: NO predominantly occurs at tends hydrogenate sites. This study valuable insights development high‐performance electrocatalysts.

Language: Английский

Citations

15
Deciphering Indirect Nitrite Reduction to Ammonia in High‐Entropy Electrocatalysts Using In Situ Raman and X‐ray Absorption Spectroscopies DOI
Talshyn Begildayeva,

Jayaraman Theerthagiri,

Wanwisa Limphirat

et al.

Small, Journal Year: 2024, Volume and Issue: 20(29)

Published: April 11, 2024

This research adopts a new method combining calcination and pulsed laser irradiation in liquids to induce controlled phase transformation of Fe, Co, Ni, Cu, Mn transition-metal-based high-entropy Prussian blue analogs into single-phase spinel oxide face-centered cubic alloy (HEA). The synthesized HEA, characterized by its highly conductive nature reactive surface, demonstrates exceptional performance capturing low-level nitrite (NO

Language: Английский

Citations

8
Mitigating Intraphase Catalytic‐Domain Transfer via CO2 Laser for Enhanced Nitrate‐to‐Ammonia Electroconversion and Zn‐Nitrate Battery Behavior DOI

Yeryeong Lee,

Jayaraman Theerthagiri,

Nuttapon Yodsin

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(47)

Published: Aug. 13, 2024

Abstract Developing sustainable energy solutions is critical for addressing the dual challenges of demand and environmental impact. In this study, a zinc‐nitrate (Zn−NO 3 − ) battery system was designed simultaneous production ammonia (NH via electrocatalytic NO reduction reaction (NO RR) electricity generation. Continuous wave CO 2 laser irradiation yielded precisely controlled CoFe O 4 @nitrogen‐doped carbon (CoFe @NC) hollow nanocubes from Prussian blue analogs (CoFe‐PBA) as integral electrocatalyst RR in 1.0 M KOH, achieving remarkable NH + rate 10.9 mg h −1 cm −2 at −0.47 V versus Reversible Hydrogen Electrode with exceptional stability. situ ex methods revealed that @NC surface transformed into high‐valent Fe/CoOOH active species, optimizing adsorption (*NO *NO species) intermediates. Furthermore, density functional theory calculations validated possible pathway on starting conversion to intermediates, followed by *NO. Subsequent protonation forms *NH leading formation final protonation. The Zn−NO utilizing cathode exhibits functionality generating stable open‐circuit voltage 1.38 Zn/Zn 2+ producing . This study highlights innovative use transform cost‐effective catalysts hierarchical structures RR‐to‐NH conversion, positioning promising technology industrial applications.

Language: Английский

Citations

5
Intraphase Switching of Hollow CoCuFe Nanocubes for Efficient Electrochemical Nitrite Reduction to Ammonia DOI
Ahreum Min,

Jueun Park,

Talshyn Begildayeva

et al.

ACS Applied Materials & Interfaces, Journal Year: 2024, Volume and Issue: 16(40), P. 53718 - 53728

Published: Aug. 22, 2024

This study addresses the urgent need to focus on nitrite reduction reaction (NO

Language: Английский

Citations

4
Laser‐Regulated CoFeRu‐LDH Nanostructures: Nitrite‐to‐Ammonia Production in Zn–Nitrite Battery and Oxygen Evolution in Water Electrolysis DOI

Sieon Jung,

Raja Arumugam Senthil, Cheol Joo Moon

et al.

Small, Journal Year: 2025, Volume and Issue: unknown

Published: May 2, 2025

Abstract Herein, the design and synthesis of Ru‐doped CoFe‐layered double hydroxide (CoFeRu─LDH) nanostructures is presented via an innovative yet straightforward pulsed laser method. The CoFeRu─LDH catalyst demonstrates outstanding electrocatalytic performance, achieving a high NH 4 + Faradaic efficiency (FE) 89.65% at −0.7 V versus reversible hydrogen electrode for nitrite reduction reaction (NO 2 − RR) low overpotential 297 mV 10 mA cm −2 oxygen evolution (OER). Comprehensive in situ ex analyses reveal electrochemically energetic species formed on surface during NO RR OER. Theoretical studies confirm that Ru doping plays imperative role tuning electronic structure CoFeRu─LDH, lowering its barriers, thereby remarkably enhancing OER performance. Specifically, galvanic Zn–nitrite battery using as cathode efficiently converts to with FE 96.8% while concurrently generating electricity power density 4.14 . Furthermore, pairing anode Pt/C water electrolysis enables H production cell voltage 1.57 This study presents new pathway designing versatile, high‐performance electrocatalysts sustainable energy conversion carbon‐free 3 fuels.

Language: Английский

Citations

0
Interfacial Electronic Interactions Promoted Activation for Nitrate Electroreduction to Ammonia over Ag‐modified Co3O4 DOI

Zhenhai Fan,

Chunmei Cao,

Xingchuan Yang

et al.

Angewandte Chemie, Journal Year: 2024, Volume and Issue: 136(44)

Published: Aug. 7, 2024

Abstract Electrocatalytic nitrate (NO 3 − ) reduction to ammonia (NRA) offers a promising pathway for synthesis. The interfacial electronic interactions (IEIs) can regulate the physicochemical capabilities of catalysts in electrochemical applications, while impact IEIs on electrocatalytic NRA remains largely unexplored current literature. In this study, high‐efficiency electrode Ag‐modified Co O 4 (Ag 1.5 Co/CC) is prepared neutral media, exhibiting an impressive conversion rate 96.86 %, Faradaic efficiency 96.11 and selectivity ~100 %. Notably, intrinsic activity Ag Co/CC ~81 times that nanoparticles (Ag/CC). Multiple characterizations theoretical computations confirm presence between , which stabilize CoO 6 octahedrons within significantly promote adsorption reactants as well intermediates 2 NO), suppressing Heyrovsky step, thereby improving electroreduction efficiency. Furthermore, our findings reveal synergistic effect different active sites enables tandem catalysis NRA: NO predominantly occurs at tends hydrogenate sites. This study valuable insights development high‐performance electrocatalysts.

Language: Английский

Citations

3
FeTiO3/TiO2 heterojunction for the electrocatalytic and photo-assisted electrocatalytic reduction of nitric oxide into ammonia DOI
Dongcai Shen, Lei Chen, Bao-Jing Li

et al.

Ceramics International, Journal Year: 2024, Volume and Issue: 50(21), P. 41603 - 41613

Published: Aug. 3, 2024

Language: Английский

Citations

2
Mitigating Intraphase Catalytic‐Domain Transfer via CO2 Laser for Enhanced Nitrate‐to‐Ammonia Electroconversion and Zn‐Nitrate Battery Behavior DOI

Yeryeong Lee,

Jayaraman Theerthagiri,

Nuttapon Yodsin

et al.

Angewandte Chemie, Journal Year: 2024, Volume and Issue: 136(47)

Published: Aug. 13, 2024

Abstract Developing sustainable energy solutions is critical for addressing the dual challenges of demand and environmental impact. In this study, a zinc‐nitrate (Zn−NO 3 − ) battery system was designed simultaneous production ammonia (NH via electrocatalytic NO reduction reaction (NO RR) electricity generation. Continuous wave CO 2 laser irradiation yielded precisely controlled CoFe O 4 @nitrogen‐doped carbon (CoFe @NC) hollow nanocubes from Prussian blue analogs (CoFe‐PBA) as integral electrocatalyst RR in 1.0 M KOH, achieving remarkable NH + rate 10.9 mg h −1 cm −2 at −0.47 V versus Reversible Hydrogen Electrode with exceptional stability. situ ex methods revealed that @NC surface transformed into high‐valent Fe/CoOOH active species, optimizing adsorption (*NO *NO species) intermediates. Furthermore, density functional theory calculations validated possible pathway on starting conversion to intermediates, followed by *NO. Subsequent protonation forms *NH leading formation final protonation. The Zn−NO utilizing cathode exhibits functionality generating stable open‐circuit voltage 1.38 Zn/Zn 2+ producing . This study highlights innovative use transform cost‐effective catalysts hierarchical structures RR‐to‐NH conversion, positioning promising technology industrial applications.

Language: Английский

Citations

0
Unraveling the Role of Intrinsic Carbon Defects for the Heterogeneous Reduction of NO with NH 3 DOI

Ruyi Zhao,

Chuanjin Zhao,

Hai Zhang

et al.

Combustion Science and Technology, Journal Year: 2024, Volume and Issue: unknown, P. 1 - 17

Published: Aug. 27, 2024

This study investigates the impact of intrinsic carbon defects on reduction nitrogen oxides (NOx) during coal combustion, with a focus synergistic effect ammonia (NH3) and pulverized coal. Two representative computational models containing are described, their influence NH3 NO is studied. Stable species transition states present in pathways calculated using B3LYP/6-31 G(d). Results indicate that exposed edge atoms exhibit higher charge density distribution, affecting adsorption reduction. The maximum energy barriers for both do not exceed 45 kcal/mol, achievable practical combustion systems. paper also calculates heterogeneous process model without (Char model), aim observing specific effects processes migration H/O atoms, recombination N formation desorption N2 molecules. Furthermore, analyses demonstrated an increase rate defective surfaces comparison to Char/NH/NO system, indicating have contributory catalytic activity. With regard magnitude reaction increasing temperature, presence base serves reinforce role temperature rate-determining step. Overall, this provides insights into carbon-based catalysis offers implications oxide emission control strategies.

Language: Английский

Citations

0