Selective Electrocatalytic Oxidation of Nitrogen to Nitric Acid Using Manganese Phthalocyanine

ACS Applied Materials & Interfaces, Год журнала: 2023, Номер 15(29), С. 34642 - 34650

Опубликована: Июль 14, 2023

Ammonia is produced through the energy-intensive Haber-Bosch process, which undergoes catalytic oxidation for production of commercial nitric acid by senescent Ostwald process. The two industrial processes demand process sustainability. Hence, single-step electrocatalysis offers a promising approach toward more environmentally friendly solution. Herein, we report 10-electron pathway associated one-step electrochemical dinitrogen reaction (N2OR) to manganese phthalocyanine (MnPc) hollow nano-structures under ambient conditions. catalyst delivers yield 513.2 μmol h-1 gcat-1 with 33.9% Faradaic efficiency @ 2.1 V versus reversible hydrogen electrode. excellent N2OR performances are achieved due specific-selectivity, presence greater number exposed active sites, recyclability, and long period stability. extended X-ray absorption fine structure confirms that Mn atoms coordinated pyrrolic pyridinic nitrogen via Mn-N4 coordination. Density functional theory-based theoretical calculations confirm site MnPc main center N2OR, suppresses oxygen evolution reaction. This work provides new arena about successful example one step utilizing site-based metal electrocatalyst development carbon-neutral sustainable society.

Язык: Английский

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Efficient nitrite-to-ammonia electroreduction over Zr-Ni frustrated Lewis acid-base pairs

Science China Chemistry, Год журнала: 2024, Номер 67(5), С. 1707 - 1714

Опубликована: Апрель 17, 2024

Язык: Английский

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Electrocatalysts with atomic-level site for nitrate reduction to ammonia

Journal of Energy Chemistry, Год журнала: 2024, Номер 96, С. 642 - 668

Опубликована: Май 27, 2024

Язык: Английский

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Understanding Potential Losses and pH Distribution in the Electrochemical Nitrate Reduction Reaction to Ammonia

Industrial & Engineering Chemistry Research, Год журнала: 2024, Номер 63(21), С. 9315 - 9328

Опубликована: Март 26, 2024

Electrochemical nitrate reduction reaction (NO3–RR) to ammonia is a promising route eliminate one of the major pollutants in surface water and groundwater. When powered by renewable electricity, electrolysis provides sustainable method generate from ions, facilitating transition linear circular economy. Optimizing physical chemical properties cells crucial making this process economically viable for widespread implementation. Here, we explore how choice current density, conductivity, pH, interelectrode distance, membrane, catalyst, buffer solution affect removal performance efficiency. We developed modeling framework investigate cell characteristics fluid dynamics during electrochemical NO3–RR using both laminar bubbly flows. To obtain more precise results, employed flow model (i.e., multiphase fluid) take into account gas production near electrode affects liquid velocity, pH distribution, and, ultimately, potential losses. exploit mass transfer theory include density effect on migration diffusion. In absence solution, Nernstian loss became significant portion polarization loss, which increased with density. identified positive membrane energy efficiency as being at smaller distances. This study insights origin losses enabling optimization fuel synthesis.

Язык: Английский

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Green synthesis of chitosan/glutamic acid/agarose/Ag nanocomposite hydrogel as a new platform for colorimetric detection of Cu ions and reduction of 4-nitrophenol

International Journal of Biological Macromolecules, Год журнала: 2024, Номер 259, С. 129394 - 129394

Опубликована: Янв. 11, 2024

Язык: Английский

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Investigation of catalytic methane oxidation over Ag/Co2MO (M = Co, Ni, Cu) catalysts with varying interfacial electron transfer

Journal of Colloid and Interface Science, Год журнала: 2024, Номер 668, С. 412 - 425

Опубликована: Апрель 24, 2024

Язык: Английский

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Boosting Synergistic Catalysis C–N Coupling via Stabilizing Close Zn/Ti Bimetallic Sites for Electrocatalytic Urea Synthesis from CO₂ and Nitrite

ACS Catalysis, Год журнала: 2025, Номер unknown, С. 2703 - 2714

Опубликована: Янв. 30, 2025

Electrocatalytic urea synthesis is significantly limited by the low efficiency of C–N bond coupling between CO2 and nitrite. Here, we designed a Zn Ti bimetallic active site catalyst anchoring TiO2 on surface ZnO developed new NF@CoMn2O4@ZnO-TiO2 electrocatalyst with high resistance to deactivation. The Co3+/Mn3+-Mn4+ solid oxide pairs in maintain their stability extracting accumulated electrons around Zn2+ Ti4+ through strong electronic interactions. sites can efficiently catalyze reduction *CO, while NO2– *NH2 intermediate product. proximity shortens distance *CO intermediates, facilitating efficient electrocatalytic urea. DFT calculations indicate that ΔG required for adsorbed short-range CoMn2O4@ZnO-TiO2 lower compared CoMn2O4@ZnO ZnO. This results remarkably Faradaic 61.18% at −0.6 V vs RHE NF@CoMn2O4@ZnO-TiO2. work provides pathway achieving synergistic catalysis reactions different metal catalytic sites.

Язык: Английский

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Core–shell heterojunction engineering of Co₃O₄/NiFe LDH nanosheets as bifunctional electrocatalysts for efficient reduction of nitrite to ammonia

Inorganic Chemistry Frontiers, Год журнала: 2023, Номер 10(15), С. 4510 - 4518

Опубликована: Янв. 1, 2023

Core–shell Co 3 O 4 /NiFe LDH heterostructured nanosheets serve as remarkable NO 2 − RR and OER bifunctional electrocatalysts for high-efficiency low-cost ammonia production.

Язык: Английский

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High-Performance Electrocatalytic Reduction of Nitrite to Ammonia under Ambient Conditions on a FeP@TiO₂ Nanoribbon Array

Inorganic Chemistry, Год журнала: 2023, Номер 62(32), С. 12644 - 12649

Опубликована: Авг. 3, 2023

Electrochemical nitrite (NO2–) reduction is recognized as a promising strategy for synthesizing valuable ammonia (NH3) and degrading NO2– pollutants in wastewater. The six-electron process the reaction complex necessitates highly selective stable electrocatalyst efficient conversion of to NH3. Herein, FeP nanoparticle-decorated TiO2 nanoribbon array on titanium plate (FeP@TiO2/TP) proposed an catalyst NH3 production under ambient conditions. In 0.1 M NaOH with NO2–, such FeP@TiO2/TP affords large yield 346.6 μmol h–1 cm–2 high Faradaic efficiency 97.1%. Additionally, it demonstrates excellent stability durability during long-term cycling tests electrolysis experiments.

Язык: Английский

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Recent Advances in Electrocatalysts for Sustainable Electrosynthesis of Ammonia and Urea from Ambient Nitrite Reduction and C–N Coupling

ACS Materials Letters, Год журнала: 2023, Номер 5(12), С. 3347 - 3363

Опубликована: Ноя. 21, 2023

The global nitrogen cycle has been destroyed by the quickly growing anthropogenic emissions of nitrite-containing pollutants during past decades, which causes numerous unexpected environmental side effects and threatens human health. Compared with conventional nitrite removal methods featuring low efficiency, high cost, secondary pollution, electrocatalytic reduction reaction garnered significant attention offers an appealing solution for recovering balance. Moreover, it takes a step further to convert into recyclable nitrogen-containing fertilizer including ammonia urea. However, materials design mechanistic aspects such emerging complex reactions are yet be explored compared other well-studied primary as oxygen water splitting. To address this challenge, review provides comprehensive account sustainable electrosynthesis urea from ambient C–N coupling. two key reactions, namely production synthesis coreduction carbon dioxide, elaborated in detail, available catalysts focus discussion. current technical barriers potential research prospects domain, exploring excellent electrocatalysts activity selectivity, precisely controlling interfacial microenvironment, understanding in-depth mechanism, highlighted.

Язык: Английский

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