Advances in ammonia electrosynthesis from ambient nitrate/nitrite reduction

Chem, Journal Year: 2023, Volume and Issue: 9(7), P. 1768 - 1827

Published: June 21, 2023

Language: Английский

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Electrochemical Nitrate Reduction: Ammonia Synthesis and the Beyond

Advanced Materials, Journal Year: 2023, Volume and Issue: 36(17)

Published: June 9, 2023

Natural nitrogen cycle has been severely disrupted by anthropogenic activities. The overuse of N-containing fertilizers induces the increase nitrate level in surface and ground waters, substantial emission oxides causes heavy air pollution. Nitrogen gas, as main component air, used for mass ammonia production over a century, providing enough nutrition agriculture to support world population increase. In last decade, researchers have made great efforts develop processes under ambient conditions combat intensive energy consumption high carbon associated with Haber-Bosch process. Among different techniques, electrochemical reduction reaction (NO

Language: 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, Journal Year: 2023, Volume and Issue: 16(7), P. 2991 - 3001

Published: Jan. 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.

Language: Английский

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Oxygen‐Bridged Copper–Iron Atomic Pair as Dual‐Metal Active Sites for Boosting Electrocatalytic NO Reduction

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(39)

Published: June 12, 2023

Electrocatalytic reduction of nitric oxide (NO) to ammonia (NH3 ) is a promising approach NH3 synthesis. However, due the lack efficient electrocatalysts, performance electrocatalytic NO reaction (NORR) far from satisfactory. Herein, it reported that an atomic copper-iron dual-site electrocatalyst bridged by axial oxygen atom (OFeN6 Cu) anchored on nitrogen-doped carbon (CuFe DS/NC) for NORR. The CuFe DS/NC can significantly enhance synthesis (Faraday efficiency, 90%; yield rate, 112.52 µmol cm-2 h-1 at -0.6 V versus RHE, which dramatically higher than corresponding Cu single-atom, Fe single-atom and all NORR catalysts in literature so far. Moreover, assembled proof-of-concept Zn-NO battery using as cathode outputs power density 2.30 mW 45.52 µg mgcat-1 . theoretical calculation result indicates bimetallic sites promote changing rate-determining step accelerating protonation process. This work provides flexible strategy sustainable

Language: Английский

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Oxygen Vacancies‐Rich Metal Oxide for Electrocatalytic Nitrogen Cycle

Advanced Energy Materials, Journal Year: 2023, Volume and Issue: 14(1)

Published: Nov. 13, 2023

Abstract The development of industry and agriculture has been accompanied by an artificially imbalanced nitrogen cycle, which threatens human health ecological environments. Electrocatalytic systems have emerged as a sustainable way converting nitrogen‐containing molecules into high value‐added chemicals. However, the construction high‐performance electrocatalysts remains challenging. oxygen vacancy engineering strategy promoted more research efforts to explore structure‐activity relationship between catalytic activity vacancies. This review systematically summarizes recent vacancies‐rich metal oxides for electro‐catalyzing cycling systems, involving electrocatalytic nitrate reduction reaction, nitric oxide C─N coupling, urea oxidation reaction. First, methods characterization vacancies are summarized. Then, effect on is discussed in terms regulating electronic structures electrocatalysts, improving electroconductivity catalysts, lowing energy barrier, strengthening adsorption activation intermediate species. Finally, future directions cycle anticipated.

Language: Английский

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Constructing FeNiPt@C Trifunctional Catalyst by High Spin‐Induced Water Oxidation Activity for Zn‐Air Battery and Anion Exchange Membrane Water Electrolyzer

Advanced Science, Journal Year: 2024, Volume and Issue: 11(19)

Published: March 14, 2024

Abstract Developing cost‐efficient trifunctional catalysts capable of facilitating hydrogen evolution reaction (HER), oxygen (OER), and reduction (ORR) activity is essential for the progression energy devices. Engineering these to optimize their active sites integrate them into a cohesive system presents significant challenge. This study introduces nanoflower (NFs)‐like carbon‐encapsulated FeNiPt nanoalloy catalyst (FeNiPt@C NFs), synthesized by substituting Co 2+ ions with high‐spin Fe in Hofmann‐type metal‐organic framework, followed carbonization pickling processes. The FeNiPt@C NFs catalyst, characterized its nitrogen‐doped metal alloy structure phase‐segregated slight surface oxidization, exhibits excellent catalytic performance. evidenced activities HER (−25 mV at 10 mA cm −2 ), ORR (half‐wave potential 0.93 V), OER (294 enhanced water oxidation attributed state element. Consequently, Zn‐air battery anion exchange membrane electrolyzer assembled demonstrate remarkable power density (168 mW ) industrial‐scale current (698 1.85 respectively. innovative integration multifunctional paves way advancement sustainable systems.

Language: Английский

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Electrocatalytic Synthesis of Pyridine Oximes using in Situ Generated NH₂OH from NO species on Nanofiber Membranes Derived from NH₂‐MIL‐53(Al)

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(45)

Published: Sept. 20, 2023

Pyridine oximes produced from aldehyde or ketone with hydroxylamine (NH2 OH) have been widely applied in pharmaceutics, enzymatic and sterilization. However, the important raw material NH2 OH exhibits corrosive unstable properties, leading to substantial energy consumption during storage transportation. Herein, this work presents a novel method for directly synthesizing highly valuable pyridine using situ generated electrocatalytic NO reduction well-design nanofiber membranes (Al-NFM) derived -MIL-53(Al). Particularly, 2-pyridinealdoxime, precursor of antidote pralidoxime (2-PAM) nerve agents suffering scarcity high cost, was achieved Faraday efficiency up 49.8 % yield 92.1 %, attributing selectivity production on Al-NFM, further easily reacted iodomethane produce 2-PAM. This study proposes creative approach, having wide universality other range functional groups, which not only facilitates conversion exhaust gas (NO) waste water (NO2- ) into chemicals especially utilization through electrochemistry, but also holds significant potential synthesis neuro detoxifying drugs humanity security.

Language: Английский

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Atomically Dispersed W₁–O₃ Bonded on Pd Metallene for Cascade NO Electroreduction to NH₃

ACS Catalysis, Journal Year: 2023, Volume and Issue: 13(14), P. 9550 - 9557

Published: July 5, 2023

Electrocatalytic NO reduction to NH3 (NORR) offers a prospective method for removing hazardous and producing valuable simultaneously. Herein, we demonstrate that atomically dispersed W on Pd metallene (W1Pd) can be an efficient robust NORR catalyst. Atomic coordination characterizations unravel single atoms exist as W1–O3 moieties bonded metallene. In situ spectroscopic measurements theoretical calculations reveal the synergistic cascade effect of promote energetics W1Pd, in which activation hydrogenation occur W1–O3, while dissociates H2O donates protons required NH3. Consequently, W1Pd exhibits yield rate 758.5 μmol h–1 cm–2 with NH3-Faradaic efficiency 91.3% flow cell (272.1 93.7% H-type cells), ranking almost highest performance among all reported catalysts.

Language: Английский

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Breaking the Scaling Relationship in C−N Coupling via the Doping Effects for Efficient Urea Electrosynthesis

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(24)

Published: April 10, 2024

Abstract Electrochemical C−N coupling reaction based on carbon dioxide and nitrate have been emerged as a new “green synthetic strategy” for the synthesis of urea, but catalytic efficiency is seriously restricted by inherent scaling relations adsorption energies active sites, improvement activity frequently accompanied decrease in selectivity. Herein, doping engineering strategy was proposed to break relationship intermediate binding minimize kinetic barrier coupling. A thus designed SrCo 0.39 Ru 0.61 O 3−δ catalyst achieves urea yield rate 1522 μg h −1 mg cat. faradic 34.1 % at −0.7 V versus reversible hydrogen electrode. series characterizations revealed that Co not only induces lattice distortion also creates rich oxygen vacancies (O ) SrRuO 3 . The weaken *CO *NH 2 intermediates sites respectively, strain effects over Co−Ru dual promoting occurrence two monomers instead selective hydrogenating form by‐products. This work presents an insight into molecular reactions towards via

Language: Английский

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Screening of Intermetallic Compounds Based on Intermediate Adsorption Equilibrium for Electrocatalytic Nitrate Reduction to Ammonia

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(29), P. 20069 - 20079

Published: July 10, 2024

Electrocatalytic nitrate (NO

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