The Use of Controls for Consistent and Accurate Measurements of Electrocatalytic Ammonia Synthesis from Dinitrogen

Greenlee, Lauren F.; Renner, Julie N.; Foster, Shelby L.

doi:10.1021/acscatal.8b02120

Cited by 279 publications

(307 citation statements)

References 24 publications

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“…Notably,i fa ll this extra increased reduction current is used for the NRR under the N 2 -saturated environment (Figure 3a), the NH 3 yield rate at À0.3 Vversus RHE is calculated to be 119.6 mg NH 3 h À1 mg cat. [40][41][42] Moreover, 1 HNMR spectroscopy with isotope-labeled 15 N 2 [43] confirms that the ammonia detected in the NRR experiments was produced from the NRR ( Figure S17). À1 ).…”

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confidence: 56%

Atomically Dispersed Molybdenum Catalysts for Efficient Ambient Nitrogen Fixation

et al. 2019

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NH 3 synthesis by the electrocatalytic N 2 reduction reaction (NRR) under ambient conditions is an appealing alternative to the currently employed industrial method-the Haber-Boschp rocess-that requires high temperature and pressure.W er eport single Mo atoms anchored to nitrogendoped porous carbon as ac ost-effective catalyst for the NRR. Benefiting from the optimally high density of active sites and hierarchically porous carbon frameworks,t his catalyst achieves ah igh NH 3 yield rate (34.0 AE 3.6 mg NH 3 h À1 mg cat. À1 )a nd ahigh Faradaic efficiency (14.6 AE 1.6 %) in 0.1m KOHatroom temperature.T hese values are considerably higher compared to previously reported non-precious-metal electrocatalysts. Moreover,t his catalyst displays no obvious current drop during a5 0000 sN RR, and high activity and durability are achieved in 0.1m HCl. The findings provideapromising lead for the design of efficient and robust single-atom non-preciousmetal catalysts for the electrocatalytic NRR.

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confidence: 56%

Atomically Dispersed Molybdenum Catalysts for Efficient Ambient Nitrogen Fixation

et al. 2019

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“…Nevertheless, the commonly used spectroscopic assays could be impacted by changes in the solution conditions, thus requiring a secondary verification using N 15 ‐labeled N 2 . We should note that commercial N 15 ‐labeled N 2 may contain trace amount of 15 NH 4 + , 15 NO 2 − , and other impurities that need to be removed before being applied into the catalytic system . Treating the 15 N 2 gas with sulfuric acid overnight before the experiment has been reported in literature to remove impurities .…”

Section: Discussionmentioning

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

134

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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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“…Accurate comparation of reported catalyst performance can only be achieved should there be reliable data available. Standard guidelines for control experiments should be followed to exclude any ammonia contamination . By conducting these rigorous control experiments, the possibility of false‐positive results should be minimized, enabling researchers to normalize the catalyst performance for the comparation of the intrinsic catalytic properties.…”

Section: Discussionmentioning

confidence: 99%

“…Qiao and co‐workers have suggested that at least two detection methods should be used for the detection of NH 3 and a third should there be obvious difference in the results . Recently, Greenlee et al have proposed a general protocol for consistent and accurate measurements of the ammonia production during electrocatalysis, as shown in Figure . It is suggested that 15 N isotope study should be carried out to verify the NH 3 production from the NRR, even though control experiments in Ar and repeated measurements for the catalysts are conducted, because of the ubiquity of ammonia due to its polarity and high aqueous solubility.…”

Section: Nitrogen Fixation At Atomic‐scale Active Sitesmentioning

confidence: 99%

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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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The Use of Controls for Consistent and Accurate Measurements of Electrocatalytic Ammonia Synthesis from Dinitrogen

Cited by 279 publications

References 24 publications

Atomically Dispersed Molybdenum Catalysts for Efficient Ambient Nitrogen Fixation

Atomically Dispersed Molybdenum Catalysts for Efficient Ambient Nitrogen Fixation

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

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

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