Thermally Enhanced Relay Electrocatalysis of Nitrate-to-Ammonia Reduction over Single-Atom-Alloy Oxides

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(11), P. 7779 - 7790

Published: March 11, 2024

The electrochemical nitrate reduction reaction (NO3RR) holds promise for converting nitrogenous pollutants to valuable ammonia products. However, conventional electrocatalysis faces challenges in effectively driving the complex eight-electron and nine-proton transfer process of NO3RR while also competing with hydrogen evolution reaction. In this study, we present thermally enhanced nitrate-to-ammonia conversion over nickel-modified copper oxide single-atom alloy nanowires. catalyst demonstrates improved production performance a Faradaic efficiency approximately 80% yield rate 9.7 mg h–1 cm–2 at +0.1 V versus reversible electrode elevated cell temperatures. addition, system displays impressive stability, interference resistance, favorable energy consumption greenhouse gas emissions simulated industrial wastewater treatment. Complementary situ analyses confirm that significantly superior relay active species formed Ni sites facilitates thermal-field-coupled Cu surface-adsorbed *NOx hydrogenation. Theoretical calculations further support thermodynamic kinetic feasibility catalysis mechanism Ni1Cu model catalyst. This study introduces conceptual thermal-electrochemistry approach synergistic regulation catalytic processes, highlighting potential multifield-coupled advance sustainable-energy-powered chemical synthesis technologies.

Language: Английский

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Atomic-level design of metalloenzyme-like active pockets in metal–organic frameworks for bioinspired catalysis

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 53(1), P. 137 - 162

Published: Nov. 29, 2023

Natural metalloenzymes with astonishing reaction activity and specificity underpin essential life transformations. Nevertheless, enzymes only operate under mild conditions to keep sophisticated structures active, limiting their potential applications. Artificial that recapitulate the catalytic of can not circumvent enzymatic fragility but also bring versatile functions into practice. Among them, metal-organic frameworks (MOFs) featuring diverse site-isolated metal sites supramolecular have emerged as promising candidates for move toward unparalleled properties behaviour enzymes. In this review, we systematically summarize significant advances in MOF-based metalloenzyme mimics a special emphasis on active pocket engineering at atomic level, including primary secondary coordination spheres. Then, deep understanding mechanisms advanced applications are discussed. Finally, perspective emerging frontier research is provided advance bioinspired catalysis.

Language: Английский

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Defect-enabling zirconium-based metal–organic frameworks for energy and environmental remediation applications

Chemical Society Reviews, Journal Year: 2024, Volume and Issue: 53(12), P. 6244 - 6294

Published: Jan. 1, 2024

This review highlights the promising prospects of defective zirconium-based MOFs in addressing challenging energy- and environment-related problems, positioning them as versatile tools toward a cleaner more sustainable future.

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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Electrocatalytic upgrading of nitrogenous wastes into value-added chemicals: A review

Materials Today, Journal Year: 2024, Volume and Issue: 73, P. 208 - 259

Published: Feb. 7, 2024

Language: Английский

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Optimizing Intermediate Adsorption over PdM (M=Fe, Co, Ni, Cu) Bimetallene for Boosted Nitrate Electroreduction to Ammonia

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(18)

Published: March 7, 2024

Electrochemical reduction of nitrate to ammonia (NO

Language: Английский

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Critical review in electrocatalytic nitrate reduction to ammonia towards a sustainable nitrogen utilization

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 483, P. 148952 - 148952

Published: Jan. 22, 2024

Language: Английский

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Synergism of electrostatic attraction and tandem catalytic effect enabled efficient electrosynthesis of ammonia from a wide-range of nitrate concentrations

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 485, P. 149769 - 149769

Published: Feb. 16, 2024

Language: Английский

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Comprehensive understanding of the thriving electrocatalytic nitrate/nitrite reduction to ammonia under ambient conditions

Journal of Energy Chemistry, Journal Year: 2024, Volume and Issue: 92, P. 459 - 483

Published: Jan. 4, 2024

Language: Английский

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The synergistic catalysis effect on electrochemical nitrate reduction at the dual-function active sites of the heterostructure

Energy & Environmental Science, Journal Year: 2024, Volume and Issue: 17(13), P. 4582 - 4593

Published: Jan. 1, 2024

The synergistic catalysis effect based on CoP and Cu 3 P dual-function active sites is proposed to understand the mechanism of hydrogen (*H) adsorbed intermediates (*NO x ) during water-splitting nitrate reduction.

Language: Английский

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