Catalysts for nitrogen reduction to ammonia

Foster, Shelby L.; Bakovic, Sergio I. Perez; Duda, Royce D.; Maheshwari, Sharad; Milton, Ross D.; Minteer, Shelley D.; Janik, Michael J.; Renner, Julie N.; Greenlee, Lauren F.

doi:10.1038/s41929-018-0092-7

Cited by 1,195 publications

(960 citation statements)

References 104 publications

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“…[8] There are several advantages in electrocatalytic NRR for ammonia synthesis: at first, the required electricity can be supplied by green energy sources, such as solar, tide, wind, etc. [10] Dispersion of metal in the form of single or a few metal atoms as actives sites on a suitable substrate could be an effective strategy to achieve facile ammonia synthesis. [9] Moreover, it has added benefits, such as modularity, scalability, and on-site, on-demand generation, which enables ammonia production in remote areas.…”

mentioning

confidence: 99%

Tuning the Catalytic Preference of Ruthenium Catalysts for Nitrogen Reduction by Atomic Dispersion

White

et al. 2019

Adv Funct Materials

175

121

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Developing cost-effective, high-performance nitrogen reduction reaction (NRR) electrocatalysts is required for the production of green and low-cost ammonia under ambient conditions. Here, a strategy is proposed to adjust the reaction preference of noble metals by tuning the size and local chemical environment of the active sites. This proof-of-concept model is realized by single ruthenium atoms distributed in a matrix of graphitic carbon nitride (Ru SAs/g-C 3 N 4 ). This model is compared, in terms of the NRR activity, to bulk Ru. The as-synthesized Ru SAs/g-C 3 N 4 exhibits excellent catalytic activity and selectivity with an NH 3 yield rate of 23.0 µg mg cat −1 h −1 and a Faradaic efficiency as high as 8.3% at a low overpotential (0.05 V vs the reversible hydrogen electrode), which is far better than that of the bulk Ru counterpart. Moreover, the Ru SAs/g-C 3 N 4 displays a high stability during five recycling tests and a 12 h potentiostatic test. Density functional theory calculations reveal that compared to bulk Ru surfaces, Ru SAs/g-C 3 N 4 has more facile reaction thermodynamics, and the enhanced NRR performance of Ru SAs/g-C 3 N 4 originates from a tuning of the d-electron energies from that of the bulk to a single-atom, causing an up-shift of the d-band center toward the Fermi level.can maximize metal utilization. Since SACs have unique catalytic sites, they usually exhibit a distinct catalytic selectivity as compared to their nanoclusters or nanoparticle counterparts. [2] For example, single atomic Pt immobilized in the surface of Ni nanocrystals shows a higher activity and chemoselectivity toward the hydrogenation of 3-nitrostyrene. [3] Isolated Co single-site catalysts anchored on a N-doped porous carbon nanobelt exhibits an excellent catalytic performance for oxidation of ethylbenzene with 98% conversion and 99% selectivity, whereas the Co nanoparticles are essentially inert. [4] Moreover, atomic Ni-anchored covalent triazine framework has a remarkable selectivity for the conversion of CO 2 to CO, with a Faradaic efficiency (FE) of > 90% over the range of −0.6 to −0.9 V versus the reversible hydrogen electrode (RHE). [5] In view of these reported works, it is evident that the size of metal particles is a key factor in determining their catalytic performance, and decreasing the size offers an intriguing opportunity to alter the activity and selectivity of these metal catalysts. SACs, as the limit of size reduction, hold great potential to achieve high activity and selectivity in catalytic reactions.Recently, the electrocatalytic N 2 reduction reaction (NRR) in aqueous electrolytes for synthesizing ammonia at ambient

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mentioning

confidence: 99%

Tuning the Catalytic Preference of Ruthenium Catalysts for Nitrogen Reduction by Atomic Dispersion

White

et al. 2019

Adv Funct Materials

175

121

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“…Overall, ammonia production from the H–B process is unsustainable and harmful to the environment. Apprehensive of its adverse impact, researchers have continuously experimented with other sustainable approaches to ammonia synthesis, and preferentially those with minimal infrastructural needs and operability under ambient conditions …”

Section: Introductionmentioning

confidence: 99%

“…However, a significant energy input is still required to break the nonpolar NN triple bond for the subsequent hydrogenation. Depending on the manner of energy input and reaction route, the emerging nitrogen fixation methods can be categorized into biochemical, photocatalytic, plasma‐chemical, chemical looping, and electrochemical approaches . Among these alternatives, the electrochemical method that utilizes electricity from renewable solar or wind energy as the energy input is highly desirable for energy conservation efforts in ammonia production .…”

Section: Introductionmentioning

confidence: 99%

“…The overall electrocatalytic system serves as the media for nitrogen dissolution and transport to the electrocatalyst surfaces, as a proton source for dinitrogen hydrogenation, and a key factor for modulation of electrocatalytic activity. Therefore, electrocatalysts in conjunction with a matching electrocatalytic system may markedly lower the activation energy of the NN triple bond, which is the most critical step in electrochemical ammonia synthesis

N_{2} + 3 H_{2} \to 2 {NH}_{3}, {normalΔ}_{f} H_{0} = - 45.9 kJ {mol}^{- 1}

…”

Section: Introductionmentioning

confidence: 99%

“…Further research is necessary to fully address the efficiency bottlenecks in electrocatalytic nitrogen reduction because of insufficient design guiding principles. On the other hand, mechanistic understanding of nitrogen reduction processes continues to be delineated by studying molecular and enzyme catalyzes, affording some activity‐relevant structural information for electrocatalyst design. It is worth noting that the dinitrogen electroreduction processes on heterogeneous electrocatalysts are different to molecular and enzymatic catalyzes, especially in proton‐coupled electron transfer (PCET) processes and electrocatalytic environments.…”

Section: Introductionmentioning

confidence: 99%

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Atomic Modulation, Structural Design, and Systematic Optimization for Efficient Electrochemical Nitrogen Reduction

et al. 2020

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Ammonia (NH3) is a pivotal precursor in fertilizer production and a potential energy carrier. Currently, ammonia production worldwide relies on the traditional Haber–Bosch process, which consumes massive energy and has a large carbon footprint. Recently, electrochemical dinitrogen reduction to ammonia under ambient conditions has attracted considerable interest owing to its advantages of flexibility and environmental friendliness. However, the biggest challenge in dinitrogen electroreduction, i.e., the low efficiency and selectivity caused by poor specificity of electrocatalysts/electrolytic systems, still needs to be overcome. Although substantial progress has been made in recent years, acquiring most available electrocatalysts still relies on low efficiency trial‐and‐error methods. It is thus imperative to establish some critical guiding principles for nitrogen electroreduction toward a rational design and accelerated development of this field. Herein, a basic understanding of dinitrogen electroreduction processes and the inherent relationships between adsorbates and catalysts from fundamental theory are described, followed by an outline of the crucial principles for designing efficient electrocatalysts/electrocatalytic systems derived from a systematic evaluation of the latest significant achievements. Finally, the future research directions and prospects of this field are given, with a special emphasis on the opportunities available by following the guiding principles.

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Push–Pull Activation of N ₂ : Coordination of Lewis Acids to Dinitrogen Complexes

Coffinet

Simonneau

Specklin

2020

Encyclopedia of Inorganic and Bioinorganic Chemistry

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HAL is a multi-disciplinary open access archive for the deposit and dissemination of scientific research documents, whether they are published or not. The documents may come from teaching and research institutions in France or abroad, or from public or private research centers. L'archive ouverte pluridisciplinaire HAL, est destinée au dépôt et à la diffusion de documents scientifiques de niveau recherche, publiés ou non, émanant des établissements d'enseignement et de recherche français ou étrangers, des laboratoires publics ou privés.

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Catalysts for nitrogen reduction to ammonia

Cited by 1,195 publications

References 104 publications

Tuning the Catalytic Preference of Ruthenium Catalysts for Nitrogen Reduction by Atomic Dispersion

Tuning the Catalytic Preference of Ruthenium Catalysts for Nitrogen Reduction by Atomic Dispersion

Atomic Modulation, Structural Design, and Systematic Optimization for Efficient Electrochemical Nitrogen Reduction

Push–Pull Activation of N ₂ : Coordination of Lewis Acids to Dinitrogen Complexes

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Catalysts for nitrogen reduction to ammonia

Cited by 1,195 publications

References 104 publications

Tuning the Catalytic Preference of Ruthenium Catalysts for Nitrogen Reduction by Atomic Dispersion

Tuning the Catalytic Preference of Ruthenium Catalysts for Nitrogen Reduction by Atomic Dispersion

Atomic Modulation, Structural Design, and Systematic Optimization for Efficient Electrochemical Nitrogen Reduction

Push–Pull Activation of N 2 : Coordination of Lewis Acids to Dinitrogen Complexes

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Product

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Push–Pull Activation of N ₂ : Coordination of Lewis Acids to Dinitrogen Complexes