Ternary intermetallic LaCoSi as a catalyst for N2 activation

Gong, Yutong; Wu, Jiazhen; Kitano, Masaaki; Wang, Junjie; Ye, Tian Nan; Jiang, Li; Kobayashi, Yasukazu; Kishida, Kazuhisa; Abe, Hitoshi; Niwa, Yasumasa; Yang, Hainan; Tada, Tomofumi; Hosono, Hideo

doi:10.1038/s41929-017-0022-0

Cited by 245 publications

(209 citation statements)

References 51 publications

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“…Molecular dynamics (MD) simulations suggested a low energy barrier of 2.38 kJ mol −1 for approaching N 2 molecules at a distance of about 0.54 nm away from the Fe site, indicating a tendency for N 2 molecules to gather around Fe SA sites for N 2 adsorption and a potential suppression of *H adsorption. Moreover, DFT calculations indicated that as an exothermal step of N 2 adsorption, the released energy could reduce the energy barrier of the following hydrogenation steps through the hot atom mechanism . However, it is important to note that the N‐doped carbon (NC) also exhibited catalytic performance for NRR as shown in Figure d.…”

Section: Advanced Catalysts For Nitrogen Conversion To Ammoniamentioning

confidence: 99%

Recent Advanced Materials for Electrochemical and Photoelectrochemical Synthesis of Ammonia from Dinitrogen: One Step Closer to a Sustainable Energy Future

Yan

Xia

et al. 2019

Advanced Energy Materials

127

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Ammonia (NH3), an important raw material for chemical industry and agriculture, is also considered to be an intriguing energy storage and transportation media for chemical conversion schemes. The world's primary NH3 supply is based on the natural nitrogen fixation by diazotrophs through an enzymatic nitrogenase process and the industrial nitrogen fixation through a traditional Haber–Bosch process. The natural synthesis of NH3 can hardly meet the rapidly growing global demand. Meanwhile, the industrial NH3 production is still dominated by the high‐temperature and high‐pressure reaction between nitrogen and hydrogen (N2 + 3H2 → 2NH3), requiring intensive energy input and generating massive CO2. Therefore, seeking a breakthrough in the development of catalysts toward efficient ammonia synthesis has become the frontier of energy and chemical conversion schemes. This review summarizes and discusses the recent progress on developing new strategies to optimize the efficiency of NH3 production coupled with renewable energy sources, with a specific focus on electrocatalytic and photoelectrocatalytic conversion of N2 to NH3. The most recent advances in the development of catalytic materials, the design of the reaction systems, and the computational insights for electrochemical and photoelectrochemical ammonia synthesis are covered.

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Section: Advanced Catalysts For Nitrogen Conversion To Ammoniamentioning

confidence: 99%

Recent Advanced Materials for Electrochemical and Photoelectrochemical Synthesis of Ammonia from Dinitrogen: One Step Closer to a Sustainable Energy Future

Yan

Xia

et al. 2019

Advanced Energy Materials

127

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“…In contrast, Ca and La were electropositive. In addition, the work functions (WFs) of La/Ca and Ru‐terminated (00 l ) surfaces, which were suggested as the dominantly exposed surfaces, were calculated for LaRuSi and CaRuSi (Supplementary Figure 15), and the results for the two compounds were found to be quite similar. The surface information investigated here indicated that the charge states of elements and WFs, which were regarded as important factors to determine the catalytic performance of a catalyst, were not the primary reasons for the different catalytic activities of these intermetallics.…”

Section: Figurementioning

confidence: 99%

Intermetallic Electride Catalyst as a Platform for Ammonia Synthesis

et al. 2018

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Electrides loaded with transition‐metal (TM) nanoparticles have recently attracted attention as emerging materials for catalytic NH3 synthesis. However, they suffer from disadvantages associated with the growth and aggregation of nanoparticles. TM‐containing intermetallic electrides appear to be promising catalysts with the advantages of both electrides and transition metals in a single phase. LaRuSi is reported here to be an intermetallic electride with superior activity for NH3 synthesis, and direct evidence is provided supporting its electride‐character‐induced catalytic performance. The discussion is made mainly based on the contrasting synthesis rates over the isostructural compounds LaRuSi, CaRuSi, and LaRu2Si2, and the N2 isotope‐exchange reactions over these compounds. Lattice hydride ions, which can reversibly exchange with anionic electrons, are shown to be indispensable in the promotion of NHx formation. The mechanism derived from the present findings provides new guidelines for NH3 synthesis.

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“…Ammonia, the nitrogen source of manmade fertilizer,isone of the most fundamental synthetic chemicals for sustaining human life. [1][2][3][4] Notwithstanding N 2 from atmosphere is inexhaustible,t he chemical inertness of dinitrogen renders it difficult in the conversion of N 2 into NH 3 . [5] Industrially,t he synthesis of NH 3 is often accomplished relying on an ironbased catalyst and harsh conditions (300-400 8 8Ca nd ca.…”

mentioning

confidence: 99%

Defect Engineering Metal‐Free Polymeric Carbon Nitride Electrocatalyst for Effective Nitrogen Fixation under Ambient Conditions

et al. 2018

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Electrocatalytic nitrogen reduction reaction (NRR) under ambient conditions provides an intriguing picture for the conversion of N into NH . However, electrocatalytic NRR mainly relies on metal-based catalysts, and it remains a grand challenge in enabling effective N activation on metal-free catalysts. Here we report a defect engineering strategy to realize effective NRR performance (NH yield: 8.09 μg h mg , Faradaic efficiency: 11.59 %) on metal-free polymeric carbon nitride (PCN) catalyst. Illustrated by density functional theory calculations, dinitrogen molecule can be chemisorbed on as-engineered nitrogen vacancies of PCN through constructing a dinuclear end-on bound structure for spatial electron transfer. Furthermore, the N-N bond length of adsorbed N increases dramatically, which corresponds to "strong activation" system to reduce N into NH . This work also highlights the significance of defect engineering for improving electrocatalysts with weak N adsorption and activation ability.

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Ternary intermetallic LaCoSi as a catalyst for N2 activation

Cited by 245 publications

References 51 publications

Recent Advanced Materials for Electrochemical and Photoelectrochemical Synthesis of Ammonia from Dinitrogen: One Step Closer to a Sustainable Energy Future

Recent Advanced Materials for Electrochemical and Photoelectrochemical Synthesis of Ammonia from Dinitrogen: One Step Closer to a Sustainable Energy Future

Intermetallic Electride Catalyst as a Platform for Ammonia Synthesis

Defect Engineering Metal‐Free Polymeric Carbon Nitride Electrocatalyst for Effective Nitrogen Fixation under Ambient Conditions

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