Selective Electrocatalytic Oxidation of Nitrogen to Nitric Acid Using Manganese Phthalocyanine

ACS Applied Materials & Interfaces, Journal Year: 2023, Volume and Issue: 15(29), P. 34642 - 34650

Published: July 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.

Language: Английский

---

Electrocatalysts with atomic-level site for nitrate reduction to ammonia

Journal of Energy Chemistry, Journal Year: 2024, Volume and Issue: 96, P. 642 - 668

Published: May 27, 2024

Language: Английский

---

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

Science China Chemistry, Journal Year: 2024, Volume and Issue: 67(5), P. 1707 - 1714

Published: April 17, 2024

Language: Английский

---

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

Industrial & Engineering Chemistry Research, Journal Year: 2024, Volume and Issue: 63(21), P. 9315 - 9328

Published: March 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.

Language: Английский

---

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

Journal of Colloid and Interface Science, Journal Year: 2024, Volume and Issue: 668, P. 412 - 425

Published: April 24, 2024

Language: Английский

---

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, Journal Year: 2024, Volume and Issue: 259, P. 129394 - 129394

Published: Jan. 11, 2024

Language: Английский

---

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

Inorganic Chemistry Frontiers, Journal Year: 2023, Volume and Issue: 10(15), P. 4510 - 4518

Published: Jan. 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.

Language: Английский

---

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

Inorganic Chemistry, Journal Year: 2023, Volume and Issue: 62(32), P. 12644 - 12649

Published: Aug. 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.

Language: Английский

---

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

ACS Materials Letters, Journal Year: 2023, Volume and Issue: 5(12), P. 3347 - 3363

Published: Nov. 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.

Language: Английский

---

Silver Nanowires‐Based Flexible Gold Electrode Overcoming Interior Impedance of Nanomaterial Electrodes

Small, Journal Year: 2024, Volume and Issue: 20(25)

Published: Jan. 9, 2024

Abstract In the development of nanomaterial electrodes for improved electrocatalytic activity, much attention is paid to compositions, lattice, and surface morphologies. this study, a new concept enhance activity proposed by reducing impedance inside electrodes. Gold nanodendrites (AuNDs) are grown along silver nanowires (AgNWs) on flexible polydimethylsiloxane (PDMS) support. The AuNDs/AgNWs/PDMS electrode affords an oxidative peak current density 50 mA cm −2 ethanol electrooxidation, value ≈20 times higher than those in literature do. Electrochemical spectroscopy (EIS) demonstrates significant contribution AgNWs reduce impedance. densities electrooxidation decreased 7.5‐fold when electrolytically corroded. By situ surface‐enhanced Raman (SERS) functional theory (DFT) simulation, it validated that favors production acetic acid with undetectable CO, resulting more complete oxidation long‐term stability, while corrosion greatly decreases production. This novel strategy fabricating using as charge transfer conduit may stimulate insights into design

Language: Английский

---