Nitrogen-fixation catalyst based on graphene: every part counts

Le, Yuan-Qi; Gu, Jia; Tian, Wei

doi:10.1039/c4cc01950d

Cited by 106 publications

(80 citation statements)

References 27 publications

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“…Charge population analysis then revealed that the graphene serves as the electron reservoir, while the FeN 3 acts as the active center and the transmitter for electron transfer. Similar computational results have also been reported for Mo/N‐doped graphene catalyst, in which the MoN 3 moiety acts as the active center for N 2 bond breaking and the graphene serves as the electron transmitter and electron reservoir for protonation and reduction (Figure b) …”

Section: Nitrogen Fixation At Atomic‐scale Active Sitessupporting

confidence: 81%

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Nitrogen Reduction to Ammonia on Atomic‐Scale Active Sites under Mild Conditions

et al. 2019

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Ammonia is one of the most important chemicals and energy carriers. Currently, ammonia is industrially produced through the Haber–Bosch process under harsh conditions of high pressure and high temperature, which are energy consuming and environmentally unfriendly. Recently, nitrogen reduction to ammonia under ambient conditions has attracted intensive research interest, in which highly efficient catalysts are of great importance. In this review, recent theoretical and experimental progresses on novel heterogeneous catalysts with low atomicity for the nitrogen reduction reaction (NRR) under ambient conditions are highlighted. Reaction mechanisms for the NRR are first introduced. Then, advances in the synthesis and characterization of catalysts with single atom features are summarized, with a particular focus on the rational design of atomic catalysts for the NRR. Lastly, the critical challenges, possible solutions, and future perspectives in the research on NRR catalysis are presented. This review systematically presents the readers with the latest advances in this field, and more importantly, sheds light on the future development of NRR catalysis with the single atomic feature.

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Section: Nitrogen Fixation At Atomic‐scale Active Sitessupporting

confidence: 81%

Section: Nitrogen Fixation At Atomic‐scale Active Sitesmentioning

confidence: 99%

Nitrogen Reduction to Ammonia on Atomic‐Scale Active Sites under Mild Conditions

et al. 2019

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“…Based on the existing experience, Tian et al explored the possible reaction mechanism of N fixation by SA Mo–N–C catalyst through theoretical calculation, molecular orbital theory and particle analysis. It is found that the enzymatic route is beneficial in energy for the simultaneous bonding of two N atoms to the Mo atom, which is more feasible than the Schrock path ( Figure ) …”

Section: Theoretical Calculations For Nonprecious Metal Single Atomicmentioning

confidence: 99%

Nitrogen‐Doped Porous Carbon Supported Nonprecious Metal Single‐Atom Electrocatalysts: from Synthesis to Application

et al. 2019

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Nonprecious metal single‐atom materials have attracted extensive attention in the field of electrocatalysis due to their low cost, high reactivity, high selectivity, and high atomic utilization. However, the high surface energy of a single atom causes agglomeration during preparation and catalytic measurement, resulting in damage to the catalytic sites. The strong interaction between substrate and monoatoms is the key factor to prevent the aggregation of individual metal atoms, and the geometry and electronic structure of the catalysts can be adjusted to optimize the catalytic activity. Due to the hierarchically pores, high specific surface area, and defect effect, nitrogen‐doped porous carbon (NPC) has been widely studied as an ideal nonprecious metal single‐atom support, which synergistically enhance the electrocatalytic performance toward oxygen reduction reaction, oxygen evolution reaction, hydrogen evolution reaction, carbon dioxide reduction reaction, and nitrogen reduction reaction with non‐noble metal single atoms. This review summarizes the controllable synthesis, characterization, theoretical calculation, and application of M (M = Co, Fe, Ni, Cu, Zn, Mo, etc.) single atoms on nitrogen‐doped porous carbon. Finally, the future development and challenges of nitrogen‐doped porous carbon supported nonprecious metal single‐atom electrocatalysts for practical commercialization are concluded.

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“…Aside from direct utilization as electrocatalysts, carbon materials are extensively used as catalyst support. Experimental evidence has confirmed that defects or doping heteroatoms in carbon materials are necessary for metal loading . Metal‐based catalysts including metals/alloys, metal oxides, nitrides, and chalcogenides are effective in electrocatalysis .…”

Section: Carbon Materialsmentioning

confidence: 99%

Carbon‐Based Substrates for Highly Dispersed Nanoparticle and Even Single‐Atom Electrocatalysts

2019

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In recent decades, electrocatalysis has become an important research hotspot in energy storage and conversion technologies due to the persistently increasing energy and environmental issues. Nanostructured carbon materials with excellent electrical conductivity, competitive activity, and relatively high chemical stability are extensively studied as either electrocatalysts or substrates to support metal‐based catalysts. Especially, when used as supporting substrates for metal‐based catalysts, carbon‐based materials can not only effectively promote the dispersion of metals and even lead to single‐atom catalysts but also lead to prominent synergistic effects for enhanced activity. This review sheds light on state‐of‐the‐art carbon‐based materials employed as supporting substrates for selected electrocatalytic processes involving H2/O2/CO2/N2. By combining experimental explorations with theoretical computations, clear insight is elaborately afforded into the fundamental relationship between electrocatalytic activity and metal–substrate interaction, in order to disclose some clues for electrocatalyst design. Finally, the remaining challenges and perspectives are discussed for the future development of carbon‐supported electrocatalysts.

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Nitrogen-fixation catalyst based on graphene: every part counts

Cited by 106 publications

References 27 publications

Nitrogen Reduction to Ammonia on Atomic‐Scale Active Sites under Mild Conditions

Nitrogen Reduction to Ammonia on Atomic‐Scale Active Sites under Mild Conditions

Nitrogen‐Doped Porous Carbon Supported Nonprecious Metal Single‐Atom Electrocatalysts: from Synthesis to Application

Carbon‐Based Substrates for Highly Dispersed Nanoparticle and Even Single‐Atom Electrocatalysts

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