High-entropy FeCoNiCuRu solid solutions triggered cocktail effect to achieve fine-tuning adsorption energy for boosting nitrate electroreduction to ammonia DOI

Tianfang Yang,

Jinrui Huang, Shixiang Hu

et al.

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 500, P. 157426 - 157426

Published: Nov. 1, 2024

Language: Английский

Metal/covalent-organic framework-based electrocatalysts for electrochemical reduction of nitrate to ammonia DOI Creative Commons
Tarekegn Heliso Dolla, Boying Zhang, Thabo Matthews

et al.

Coordination Chemistry Reviews, Journal Year: 2024, Volume and Issue: 518, P. 216061 - 216061

Published: July 8, 2024

The pervasive contamination of industrial, domestic, and agricultural wastewater with nitrate poses profound ecological public health risks. Traditional methods for remediating nitrate-laden water face formidable challenges due to its high solubility stability. However, a promising solution emerges in the form electrochemical reduction (eNO3RR), offering both efficient removal valuable ammonia generation sustainable manner. This review explores burgeoning field eNO3RR, focusing on recent advancements utilizing porous crystalline framework materials − metal–organic frameworks (MOFs) covalent-organic (COFs) as novel class electrocatalysts. These innovative exhibit unique properties such adjustable porosity, diverse structures, tunable pore sizes, well-defined active sites, making them ideal candidates enhancing efficiency selectivity under ambient conditions. By dissecting structure–activity relationship inherent MOF/COF-based electrocatalysts, this aims provide comprehensive understanding their role driving conversion NO3− NH3. Moreover, it identifies current proposes future prospects leveraging these advanced pollutants, glimpse into greener more effective approach remediation resource recovery.

Language: Английский

Citations

10

The Impact of Clean Grid Transition on Wastewater Sector Greenhouse Gas Emissions DOI

Xiatong Li,

Cuihong Song, Sahar H. El Abbadi

et al.

Environmental Science & Technology Letters, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 8, 2025

This study examines the spatial and temporal impacts of U.S. clean energy grid transition on related greenhouse gas (GHG) emissions from wastewater treatment industry. By analyzing data 17,156 water resource recovery facilities (WRRFs) state-specific decarbonization scenarios, results project a 60% reduction in Scope 2 by 2050, driven national shift to renewable energy. However, regional disparities are prominent, with northeastern western states achieving most significant reductions, while Ohio Valley Rockies likely experience higher due reliance fossil fuels. offers first assessment WRRFs highlights need for targeted, region-specific strategies across different emission scopes. research provides insights policymakers stakeholders sector, emphasizing critical role GHG goals.

Language: Английский

Citations

1

Understanding Free-Energy Landscapes in Electrocatalysis: A Case Study on Nitrate Reduction over Au(111) DOI Creative Commons
Ebrahim Tayyebi, Kai S. Exner

ACS electrochemistry., Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 25, 2025

Free-energy landscapes are essential tools in electrocatalysis for assessing catalyst activity and selectivity of proton-coupled electron transfer steps. It is a common approach to focus on the thermodynamic part free-energy landscape refer only reaction intermediates, which turn leads results being highly dependent accuracy calculated binding energies adsorbed intermediates. Since evaluation electrocatalytic processes solid surfaces usually requires density functional theory calculations (DFT) with periodic boundary conditions, free energy reference molecules relevant binding-energy determination subject an inherent error. For this purpose, gas-phase error corrections have been introduced recent years, allow correction DFT error, based assessment formation enthalpies, by assigning double or triple bonds molecules. In contribution, we present simple unbiased errors: do not distinguish between bond order but correct all single, double, referring atomization compounds. We employ our nitrate reduction Au(111) as case study, using different levels exchange–correlation functionals generalized gradient meta-generalized approximation. shown that inclusion well solvation ion significantly affects energetics predictions descriptor-based analysis, highlighting importance correcting DFT-based gaining reliable insights into systems.

Language: Английский

Citations

1

Understanding first electron transfer kinetic process of electrochemical nitrate reduction to ammonia on Fe2O3 nanorods array DOI
Tingsong Li, Chun Tang, Heng Guo

et al.

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 485, P. 149560 - 149560

Published: Feb. 20, 2024

Language: Английский

Citations

5

Exergy and environmental footprint analysis for a green ammonia production process DOI

Zhaohui Gu,

Zhiqiang Liu, Sheng Yang

et al.

Journal of Cleaner Production, Journal Year: 2024, Volume and Issue: 455, P. 142357 - 142357

Published: April 26, 2024

Language: Английский

Citations

5

Manipulating Superexchange Interaction of Ru–O–Fe Sites for Enhanced Electrocatalytic Nitrate-to-Ammonia Selectivity DOI

Mengyang Xia,

Chao Zhao, Hang Xiao

et al.

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(16), P. 12152 - 12162

Published: July 30, 2024

Fe-based catalysts are promising for electrochemical nitrate reduction, but their selectivity is limited by the multielectron/proton transfer reaction steps. Here, we propose optimizing eg-orbital electron occupancy regulating superexchange interaction of Fe site to improve NH3 production performance. Our experimental and theoretical prediction results confirmed that Ru–O–Fe sites in double perovskite iron oxides (LaFe0.9Ru0.1O3) have more significant interactions, mainly manifested O-anion-mediated from Ru cations. alters Fe's spin configuration through orbital hybridization, transitioning a high-spin (HS, eg ≈ 2) an intermediate-spin state (eg 1). This transition promotes NO3– adsorption lowers hydrogenation energy barrier *NO intermediate. Consequently, LaFe0.9Ru0.1O3 could efficiently convert NH3, achieving rates 0.75 mmol·h–1·cm–2 with Faraday efficiency 98.5%. Remarkably, was as high 90.7%, which represents almost best catalyst date.

Language: Английский

Citations

4

Ruthenium Anchored Laser‐Induced Graphene as Binder‐Free and Free‐Standing Electrode for Selective Electrosynthesis of Ammonia from Nitrate DOI Creative Commons

Zekun Geng,

Zhiliang Feng,

Haoran Kong

et al.

Advanced Science, Journal Year: 2024, Volume and Issue: 11(39)

Published: Aug. 13, 2024

Developing effective electrocatalysts for the nitrate reduction reaction (NO

Language: Английский

Citations

4

Pulsed Electrolysis in Membrane Electrode Assembly Architecture for Enhanced Electrochemical Nitrate Reduction Reaction to Ammonia DOI
Ramireddy Boppella,

Maryam Ahmadi,

B Arndt

et al.

ACS Catalysis, Journal Year: 2024, Volume and Issue: unknown, P. 18223 - 18236

Published: Nov. 26, 2024

Electrochemical nitrate reduction reaction (NO3–RR) to ammonia offers a promising solution environmental and energy challenges, converting ubiquitous pollutant in aquatic environments into carbon-free carrier essential chemical feedstock. While considerable research has focused on electrocatalyst development, relatively less attention been given device engineering electroanalytical techniques that play crucial roles enhancing the performance of electrocatalytic NO3–RR, especially at such low concentrations. Here, CuxRuy alloy catalysts were synthesized, their was investigated by using various H-type membrane-electrode-assembly (MEA) configurations. The results revealed poor NO3–RR NO3– concentrations (0.01 M) H cells due mass transfer loss, promoting competing hydrogen evolution reaction. Pulsed electrolysis leveraged as an effective strategy enhance yield rate (3-fold) Faradaic efficiency (FE) (2-fold) compared potentiostatic (i.e., constant voltage) condition concentrations, primarily impacting local microenvironment. Additionally, MEA cell constructed with anionic bipolar membranes, comparative study conducted examining voltage, selectivity, efficiency. findings exhibited membrane type significantly influences voltage system Notably, CuRu catalyst anion exchange achieved FE exceeding 90% 200 mA cm–2 highest NH3 5.74 ± 0.27 mmol h–1 stability over 100 h assessed 600 cm–2. insights gained from this work could inform rational design electrochemical enhanced catalytic

Language: Английский

Citations

4

Alloy Catalysts for Electrochemical Nitrate Reduction to Ammonia DOI Creative Commons
Rong Zhang, Xintao Ma, Shaoce Zhang

et al.

ChemElectroChem, Journal Year: 2025, Volume and Issue: 12(4)

Published: Jan. 31, 2025

Abstract Electrochemical nitrate reduction reaction (NO 3 − RR) represents a promising ammonia (NH ) production approach and has garnered significant attention in recent years. Owing to the highly tunable electronic structures physicochemical properties, alloy materials have emerged as efficient catalysts for electrochemical NO RR. This review systematically examines advancements including binary alloys multi‐metal RR, comprehensively analyzing their structure, catalytic activity, mechanisms In addition, relationship between catalysts′ composition, active sites, activity are described, aiming elucidate underlying principles high guide rational design of future catalysts. Finally, this addresses challenges proposes directions research development.

Language: Английский

Citations

0

Synthesis of Bimetallic (Iron–Cobalt) Single Atom Catalysts for Electrochemical Detection of Nitrites DOI Creative Commons
Guillermo Tostado-Blázquez, Messaoud Harfouche, Jose L. Cerrillo

et al.

Advanced Materials Technologies, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 8, 2025

Abstract Nitrite (NO 2 − ) is responsible for several physiological processes but can be harmful in excess. With rising exposure from food preservatives, fertilizers, and pollutants, accurate nitrite assessment crucial health environmental safety. Different methods have been employed its determination, with electrochemical sensors showcasing great promise. Single atom catalysts (SACs) are a class of nanomaterials that consists isolated catalytic metal atoms anchored on conductive supports, which exhibit unique electronic properties promise this application. The performance these materials enhanced even more by incorporating secondary the catalyst structure. This leads to creation surface‐active sites enables facilitation multi‐step reactions. Herein, bimetallic single (FeCoSAN) synthesized through step laser assisted solid‐process anchoring iron cobalt while simultaneously creating laser‐scribed graphene (LSG) support. presence Fe Co verified high‐angle annular dark‐field scanning transmission electron microscopy (HAADF‐STEM) X‐ray absorption spectroscopy (XANES EXAFS). Through testing, system demonstrated excellent capabilities determination NO , achieving up 100% efficiency, comparison bare LSG, detection limit 2.42 µ m sensitivity value 515.07 µA −1 cm −2 over linear range 5.0 1666 . highlights their potential vivo point‐of‐care sensing applications.

Language: Английский

Citations

0