Designing a Built-In Electric Field for Efficient Energy Electrocatalysis

ACS Nano, Journal Year: 2022, Volume and Issue: 16(12), P. 19959 - 19979

Published: Dec. 15, 2022

To utilize intermittent renewable energy as well achieve the goals of peak carbon dioxide emissions and neutrality, various electrocatalytic devices have been developed. However, reactions, e.g., hydrogen evolution reaction/oxygen reaction in overall water splitting, polysulfide conversion lithium–sulfur batteries, formation/decomposition lithium peroxide lithium–oxygen nitrate reduction to degrade sewage, suffer from sluggish kinetics caused by multielectron transfer processes. Owing merits accelerated charge transport, optimized adsorption/desorption intermediates, raised conductivity, regulation microenvironment, ease combine with geometric characteristics, built-in electric field (BIEF) is expected overcome above problems. Here, we give a Review about very recent progress BIEF for efficient electrocatalysis. First, construction strategies characterization methods (qualitative quantitative analysis) are summarized. Then, up-to-date overviews engineering electrocatalysis, attention on electron structure optimization microenvironment modulation, analyzed discussed detail. In end, challenges perspectives proposed. This gives deep understanding design electrocatalysts next-generation storage devices.

Language: Английский

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Recent progress and strategies on the design of catalysts for electrochemical ammonia synthesis from nitrate reduction

Inorganic Chemistry Frontiers, Journal Year: 2023, Volume and Issue: 10(12), P. 3489 - 3514

Published: Jan. 1, 2023

Ammonia (NH3) is an essential raw material in the production of fertilizers and a promising carbon-free energy carrier, however, its synthesis still depends on energy- capital-intensive Haber–Bosch process. Recently, electrochemical N2 reduction reaction has attracted significant interest as emerging method for NH3 under ambient conditions. However, limited solubility aqueous electrolyte strong NN bonds result low yield rate, inferior faradaic efficiency unsatisfactory selectivity, impeding further practical application. Considering high water nitrate (NO3−), NO3− (NO3−RR) become fascinating route achieving sustainable NH3, enormous progress been made this field. As consequence, review discusses mechanism systematically summarizes recent development electrocatalysts NO3−RR, including noble-metal-based materials, single-atom metal catalysts, transition-metal-based catalysts. Diverse design strategies catalysts to boost NO3−RR performance, such defect engineering, rational structure design, strain engineering constructing heterostructures, are discussed. This followed by illustration how robust understanding optimization affords fundamental insights into efficiency, selectivity electrocatalysts. Finally, we conclude with future perspectives critical issues, challenges research directions high-efficiency selective NH3.

Language: Английский

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V-doped TiO2 nanobelt array for high-efficiency electrocatalytic nitrite reduction to ammonia

Materials Today Physics, Journal Year: 2022, Volume and Issue: 30, P. 100944 - 100944

Published: Dec. 5, 2022

Language: Английский

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Intensified Kirkendall effect assisted construction of double-shell hollow Cu-doped CoP nanoparticles anchored by carbon arrays for water splitting

Applied Catalysis B Environment and Energy, Journal Year: 2022, Volume and Issue: 325, P. 122295 - 122295

Published: Dec. 14, 2022

Language: Английский

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Recent Advance in Heterogenous Electrocatalysts for Highly Selective Nitrite Reduction to Ammonia Under Ambient Condition

Small Structures, Journal Year: 2023, Volume and Issue: 4(11)

Published: July 23, 2023

Industrial ammonia production mainly relies on the conventional Haber–Bosch process accompanied by high energy consumption and plentiful carbon dioxide emissions, which triggered recent interest to explore more energy‐efficient environmentally benign alternatives. Very recently, electrochemical nitrite reduction in an aqueous medium promises new opportunities for advanced, energy‐efficient, sustainable at ambient conditions. The formation rate Faradic efficiency are strongly associated with adopted electrocatalysts; therefore, striving high‐efficient electrocatalysts is key via reaction. Herein, a critical overview of advances reaction presented, highlighting latest innovative heterogenous including noble metal catalysts, transition‐metal‐based their compounds. Meanwhile, possible pathway electroreduction ammonia, detection, catalytic activity descriptor briefly summarized. Finally, perspective research challenges that convert outlined, increasing contributions route realizing neutral footprint.

Language: Английский

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Sustainable Ammonia Electrosynthesis from Nitrate Wastewater Coupled to Electrocatalytic Upcycling of Polyethylene Terephthalate Plastic Waste

ACS Nano, Journal Year: 2023, Volume and Issue: 17(13), P. 12422 - 12432

Published: June 26, 2023

Integrating the nitrate reduction reaction (NO3RR) with polyethylene terephthalate (PET) hydrolysate oxidation to construct nitrate/PET coelectrolysis system holds a great promise of realizing simultaneous upcycling wastewater and PET plastic waste, which, however, is still an almost untouched research area. Herein, we develop ultralow content Ru-incorporated Co-based metal-organic frameworks as bifunctional precatalyst, which can be in situ reconstructed Ru-Co(OH)2 at cathode Ru-CoOOH anode under electrocatalytic environments, function real active catalysts for NO3RR oxidation, respectively. With two-electrode system, current density 50 mA cm-2 achieved cell voltage only 1.53 V, production ammonia formate lower energy consumption. This study provides concept construction systems waste.

Language: Английский

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Tandem Electrocatalytic Reduction of Nitrite to Ammonia on Rhodium–Copper Single Atom Alloys

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(36)

Published: April 23, 2024

Abstract Electrocatalytic reduction of NO 2 − to NH 3 (NO RR) presents a fascinating approach for simultaneously migrating pollutants and producing valuable . In this study, single‐atom Rh‐alloyed copper (CuRh 1 ) is explored as highly active selective catalyst toward the RR. Combined theoretical calculations in situ FTIR/EPR spectroscopic experiments uncover synergistic effect Rh Cu promote RR energetics CuRh through tandem catalysis pathway, which activates preliminary adsorption hydrogenation → *NO *NOOH *NO), while generated on then transferred substrate promotes rate‐determining step *NHO synthesis. As result, equipped flow cell an unprecedented yield rate 2191.6 µmol h −1 cm −2 ‐Faradaic efficiency 98.9% at high current density 322.5 mA , well long‐term stability 100 electrolysis.

Language: Английский

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Highly Efficient Electroenzymatic Cascade Reduction Reaction For The Conversion of Nitrite to Ammonia

Advanced Energy Materials, Journal Year: 2023, Volume and Issue: 13(20)

Published: April 6, 2023

Abstract The electrochemical nitrite reduction reaction provides an alternative approach to offer sustainable ammonia source routes for repairing imbalances in the global nitrogen cycle. In this work, electrocatalysis is combined with enzymatic catalysis provide efficient and clean process recoverable production. NO 2 − reduced NH 3 by electroenzymatic cascade on a bioconjugate, which 1‐butyl‐3‐methylimidazolium bromide (IL BMB ) modified chloroperoxidase (CPO) fixed polyethyleneimine (PEI) multi‐walled carbon nanotubes (MWCNT) from bioconjugate (CPO‐IL /MWCNT‐PEI). 15 N 14 isotope labeling reveal that species derived reduction. Density functional theory calculations identify Fe II heme center of CPO serve as key active site amino groups MWCNT‐PEI not only bridge covalently immobilize but also enrich ion at electrode/solution interface through electrostatic interactions. low energy barrier adsorption free intermediate result high Faradaic efficiency (96.4%), yield (112.7 mg h −1 ), selectivity pH 5.0 solution. highly ensurespromising applications conversion .

Language: Английский

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p-d hybridized In-Co dual sites promote nitrite electroreduction to ammonia at high current density

Nano Energy, Journal Year: 2024, Volume and Issue: 125, P. 109594 - 109594

Published: April 6, 2024

Language: Английский

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Molten salts etching strategy construct alloy/MXene heterostructures for efficient ammonia synthesis and energy supply via Zn-nitrite battery

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 348, P. 123862 - 123862

Published: April 24, 2024

Language: Английский

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