Electrochemical C–N coupling of CO₂and nitrogenous small molecules for the electrosynthesis of organonitrogen compounds

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 52(6), P. 2193 - 2237

Published: Jan. 1, 2023

Electrochemical C–N coupling reaction by renewable electricity for the electrosynthesis of organonitrogen compounds with abundant CO 2 and nitrogenous small molecules as carbon nitrogen sources, respectively, is a promising sustainable synthetic strategy.

Language: Английский

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Engineering photocatalytic ammonia synthesis

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 52(20), P. 6938 - 6956

Published: Jan. 1, 2023

This review is organized based on an engineering perspective, including materials engineering, structure and reaction spanning photocatalyst preparation to photocatalytic process intensification.

Language: Английский

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Inter‐Metal Interaction of Dual‐Atom Catalysts in Heterogeneous Catalysis

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(42)

Published: June 14, 2023

Dual-atom catalysts (DACs) have been a new frontier in heterogeneous catalysis due to their unique intrinsic properties. The synergy between dual atoms provides flexible active sites, promising enhance performance and even catalyze more complex reactions. However, precisely regulating site structure uncovering dual-atom metal interaction remain grand challenges. In this review, we clarify the significance of inter-metal DACs based on understanding center structures. Three diatomic configurations are elaborated, including isolated single-atom, N/O-bridged dual-atom, direct dual-metal bonding interaction. Subsequently, up-to-date progress oxidation reactions, hydrogenation/dehydrogenation electrocatalytic photocatalytic reactions summarized. structure-activity relationship catalytic is then discussed at an atomic level. Finally, challenges future directions engineer discussed. This review will offer prospects for rational design efficient toward catalysis.

Language: Английский

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Complementary Design in Multicomponent Electrocatalysts for Electrochemical Nitrogen Reduction: Beyond the Leverage in Activity and Selectivity

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(15)

Published: Jan. 24, 2023

Electrochemical nitrogen reduction reaction (eNRR) is promising in place of the Haber-Bosch process for artificial N2 fixation. However, high activity and selectivity eNRR are challenging to achieve simultaneously due scaling relations. Such "leverage" between has severely restricted eNRR. To overcome this bottleneck, complementary design electronic structures multicomponent electrocatalysts been recently pursued, aiming maximize advantages each component optimize multistep reactions, which stood at cutting edge aspect. Here, we present a minireview design, performance, mechanism with structures. We particularly emphasize interactions elements from d-, p-, s-blocks, essential understanding how these beyond selectivity.

Language: Английский

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Cobaloximes: selective nitrite reduction catalysts for tandem ammonia synthesis

Energy & Environmental Science, Journal Year: 2023, Volume and Issue: 16(4), P. 1590 - 1596

Published: Jan. 1, 2023

Herein, we demonstrate cobaloximes as a bioinspired molecular platform for exclusive ammonia synthesis via electrocatalytic NO 2 − reduction (eNO RR), which attained 98.5% faradaic efficiency (FE) under close-to-neutral conditions.

Language: Английский

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Improving Electrocatalytic Nitrogen Reduction Selectivity and Yield by Suppressing Hydrogen Evolution Reaction via Electronic Metal–Support Interaction

Advanced Energy Materials, Journal Year: 2023, Volume and Issue: 13(21)

Published: April 9, 2023

Abstract The electrochemical nitrogen reduction reaction (NRR) has the potential to replace Haber–Bosch process for ammonia synthesis under ambient conditions. However, selectivity and yield of NRR are impractical, owing preferential binding electrocatalyst H consequential coverage active sites. In this study, VO 2 , with N strongly adsorbed over atoms, is used as a support provide source avoid hydrogen evolution reaction. Mo, high activity, introduced site promote NRR. Meanwhile, electronic metal–support interaction between Mo creates electron‐deficient sites, which weakens adsorption lowers energy barrier first step, protonation, thereby kinetically enhancing activity. average NH 3 Mo/VO 190.1 µg mg cat. −1 h Faradaic efficiency 32.4% at −0.5 V versus reversible electrode, 10.8 2.8 times greater than that respectively.

Language: Английский

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Targeted Modulation of Competitive Active Sites toward Nitrogen Fixation via Sulfur Vacancy Engineering Over MoS₂

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(36)

Published: May 12, 2023

Electrocatalytic nitrogen reduction reaction (NRR) offers an environmentally benign and sustainable alternative for NH3 synthesis. However, developing NRR electrocatalysts with both high activity selectivity remains a significant challenge. Guided by the density functional theory (DFT) calculations further verified experiment, modulated MoS2 well-controlled S vacancies (MoS2-Vs) is prepared as excellent electrocatalyst NRR, where of mightily rely on S-vacancy concentration. The optimized catalyst (MoS2-7H) in suitable concentration (17.5%) empowered (NH3 yield rate: 66.74 µg h−1 mg−1 at −0.6 V) (Faradic efficiency (FE): 14.68% −0.5 V). Further mechanistic study reveals that performance powerfully concentration-dependent since its enhanced due to S-vacancy-strengthened N2 adsorption reduced energy barrier. Simultaneously, synchronously improved steadily inversely suppressed hydrogen evolution through limiting H2 desorption kinetics, which sets it markedly apart from other reported defective MoS2-based catalysts.

Language: Английский

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NH₃ Electrosynthesis from N₂ Molecules: Progresses, Challenges, and Future Perspectives

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(10), P. 6409 - 6421

Published: Feb. 27, 2024

Green ammonia (NH3), made by using renewable electricity to split nearly limitless nitrogen (N2) molecules, is a vital platform molecule and an ideal fuel drive the sustainable development of human society without carbon dioxide emission. The NH3 electrosynthesis field currently faces dilemma low yield rate efficiency; however, decoupling overlapping issues this area providing guidelines for its directions are not trivial because it involves complex reaction process multidisciplinary entries (for example, electrochemistry, catalysis, interfaces, processes, etc.). In Perspective, we introduce classification scheme based on process, namely, direct (N2 reduction reaction) indirect (Li-mediated/plasma-enabled electrosynthesis). This categorization allows us finely decouple complicated pathways identify specific rate-determining steps/bottleneck each synthesis approach such as N2 activation, H2 evolution side reaction, solid-electrolyte interphase engineering, plasma etc. We then present detailed overview latest progresses solving these core in terms whole electrochemical system covering electrocatalysts, electrodes, electrolytes, electrolyzers, Finally, discuss research focuses promising strategies future with multiscale perspective atomistic mechanisms, nanoscale microscale electrodes/interfaces, macroscale electrolyzers/processes. It expected that Perspective will provide readers in-depth understanding bottleneck insightful guidance designing efficient systems.

Language: Английский

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Seawater electrolysis for fuels and chemicals production: fundamentals, achievements, and perspectives

Chemical Society Reviews, Journal Year: 2024, Volume and Issue: 53(14), P. 7455 - 7488

Published: Jan. 1, 2024

Seawater electrolysis for the production of fuels and chemicals involved in onshore offshore plants powered by renewable energies offers a promising avenue unique advantages energy environmental sustainability. Nevertheless, seawater presents long-term challenges issues, such as complex composition, potential side reactions, deposition poisoning microorganisms metal ions, well corrosion, thus hindering rapid development technology. This review focuses on value-added (hydrogen beyond) fine through electrolysis, step towards sustainable carbon neutrality. The principle related are first introduced, redox reaction mechanisms summarized. Strategies operating anodes cathodes including application chloride- impurity-resistant electrocatalysts/membranes reviewed. We comprehensively summarize (hydrogen, monoxide, sulfur, ammonia,

Language: Английский

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Progress in Single/Multi Atoms and 2D‐Nanomaterials for Electro/Photocatalytic Nitrogen Reduction: Experimental, Computational and Machine Leaning Developments

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: 14(28)

Published: Feb. 11, 2024

Abstract The conversion of atmospheric nitrogen (N 2 ) into ammonia (NH 3 ), known as fixation, plays a crucial role in sustaining life on Earth, facing innovation with electrocatalytic and photocatalytic methods. These approaches promise gentler conversions from to ammonia, diverging the energy‐intensive Haber‐Bosch process, which requires complex plant infrastructure. Vitality lies eco‐friendly, cost‐effective, energy‐efficient pathways. challenge is that electrocatalysts photocatalysts for reduction have shown low Faraday efficiency, hampered by hydrogen evolution. This work delves recent strides electro/photo‐catalytic fixation/reduction, deciphering mechanisms, catalysts, prospects. By unveiling core principles steering these processes, it dissects efficiency drivers. Experimental theoretical studies, ranging density functional calculations/simulations machine learning‐based catalyst screening, mark path toward highly efficient including single/multi‐atom catalysts embedded 2D materials. journey explores diverse assessing their performance, spotlighting emerging nanomaterials, heterostructures, co‐catalyst techniques. Perspectives future directions potential applications fixation/reduction are offered, emphasizing sustainable management implications global agriculture environmental sustainability.

Language: Английский

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