Lithium-mediated electrochemical dinitrogen reduction reaction

Iqbal, Muhammad Saqlain; Ruan, Yukun; Iftikhar, Ramsha; Khan, Faiza Zahid; Li, Weixiang; Hao, Leiduan; Robertson, Alex; Percoco, Gianluca; Sun, Zhenyu

doi:10.1039/d3im00006k

Cited by 18 publications

(6 citation statements)

References 87 publications

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“…Electrochemical reduction techniques have gained significant interest as options for nitrogen reduction reaction (NRR) [287][288][289] that proceeds via coupled or sequential proton and electron transfer processes (Table S5). Heterogeneous electrocatalysts typically have two potential pathways: associative and dissociative.…”

Section: Reactionmentioning

confidence: 99%

Emerging two-dimensional materials: Synthesis, physical properties, and application for catalysis in energy conversion and storage

Xu,

Iqbal,

Wang

et al. 2024

TIMS

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<p>Inorganic, organic, and hybrid two-dimensional (2D) materials are being developed for ever-expanding numbers of applications, though energy and catalysis remain the main drivers of their development. We present overviews of bottom-up and top-down synthetic strategies of such materials and examine manufacturing scalability issues. Mechanical, electrical, and thermal properties and their modulation are highlighted because they are fundamental to the above-mentioned drivers. The burgeoning importance of heterostructures in such materials, particularly for catalysis and electrode design and function is stressed. Detailed attention is given to applications of 2D materials to the electrocatalysis reactions: oxygen reduction, oxygen evolution, hydrogen evolution, carbon dioxide reduction, and nitrogen reduction. Water splitting, carbon dioxide reduction, and nitrogen reduction by photocatalysis are also examined. A perspective of expected advances in the expansion of applications and types of 2D materials, with a focus on heterostructure development, is presented in the conclusion.</p>

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Section: Reactionmentioning

confidence: 99%

Emerging two-dimensional materials: Synthesis, physical properties, and application for catalysis in energy conversion and storage

Xu,

Iqbal,

Wang

et al. 2024

TIMS

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“…One of the key issues is overcoming the limitations imposed by scaling relationships. [25][26][27][28] However, the concept of breaking scaling relationships has not been deeply discussed in the development of NRR catalysts thus far. The NRR process involves multiple proton-electron transfer reactions and different intermediates.…”

Section: The Scaling Relationshipsmentioning

confidence: 99%

Emerging two-dimensional materials for the electrocatalytic nitrogen reduction reaction to yield ammonia

Ruan,

He,

Liu

et al. 2023

J. Mater. Chem. A

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“…The Haber-Bosch method of producing ammonia is currently being replaced by new synthetic techniques. Researchers have preferred the environmentally friendly and sustainable process of electrochemical ammonia synthesis, which uses electricity produced from renewable energy sources, water, and electrons as proton donors and catalysts, and oxygen as a byproduct of the anode reaction [23][24][25][26][27][28]. Unfortunately, owing to the high energy barrier for cleaving the N≡N bond (941 kJ mol −1 ), the NH 3 yield rate in NRR is still insufficient to fulfill the demands of industrial production [29][30][31].…”

Section: Introductionmentioning

confidence: 99%

Bimetallic synergistic catalysts based on two-dimensional carbon-rich conjugated frameworks for nitrate electrocatalytic reduction to ammonia: catalyst screening and mechanism insights

Luo,

Guo

2024

Nanotechnology

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The discovery of the "two birds, one stone" electrochemical nitrate reduction reaction (NO3RR) allows for the removal of harmful NO3− pollutants as well as the production of economically beneficial ammonia (NH3). However, current understanding of the catalytic mechanism of NO3RR is not enough, and this research is still challenging. To determine the mechanism needed to create efficient electrocatalysts, we thoroughly examined the catalytic activity of molybdenum-based diatomic catalysts (DACs) anchored on two-dimensional carbon-rich conjugated frameworks (2D CCFs) for NO3RR. Among the 23 candidate materials, after a four-step screening method and detailed mechanism studies, we discovered that NO3RR can efficiently generate NH3 by following the N-end pathway on the MoTi-Pc, MoMn-Pc, and MoNb-Pc, with limiting potential of −0.33 V, −0.13 V, and −0.38 V, respectively. The activity of NO3RR can be attributed to the synergistic effect of the TM1-TM2 dimer d orbital coupling to the anti-bonding orbital of NO3−. Additionally, high hybridization between the Mo-4d, TM-3d(4d), and NO3−-2p orbitals on the MoTMs-Pc DACs can speed up the flow of electrons from the Mo-TM dual-site to NO3−. The research presented here paves the way for the reasonable design of effective NO3RR catalysts and offers a theoretical basis for experimental research.

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Lithium-mediated electrochemical dinitrogen reduction reaction

Abstract: The Haber-Bosch process is a well-known approach for NH3 production but faces certain limitations due to higher temperatures and energy-intensive steps. For the sustainable and green NH3 production at ambient...

Cited by 18 publications

References 87 publications

Emerging two-dimensional materials: Synthesis, physical properties, and application for catalysis in energy conversion and storage

Emerging two-dimensional materials: Synthesis, physical properties, and application for catalysis in energy conversion and storage

Emerging two-dimensional materials for the electrocatalytic nitrogen reduction reaction to yield ammonia

Bimetallic synergistic catalysts based on two-dimensional carbon-rich conjugated frameworks for nitrate electrocatalytic reduction to ammonia: catalyst screening and mechanism insights

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