Recent progress in the electrochemical ammonia synthesis under ambient conditions

Zhao, Runbo; Xie, Heping; Chang, Le; Zhang, Xiaoxue; Zhu, Xiaojuan; Tong, Xin; Wang, Ting; Luo, Yonglan; Wei, Peipei; Wang, Zhiming; Sun, Xuping

doi:10.1016/j.enchem.2019.100011

Cited by 176 publications

(124 citation statements)

References 218 publications

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“…At the (111) facet this will occur through one endothermic step of 0.92 eV and for the (210) facet two endothermic steps of 0.93 eV and 0.70 eV are needed. The overall reaction with the release of a second NH 3 molecule is exothermic at both facets and the calculations show that both reaction pathways are viable . Lanthanum Chromite (LaCrO 3 ) nanoparticles were synthesized and evaluated as the NRR electrocatalyst in an aqueous based cell under ambient conditions.…”

Section: Figurementioning

confidence: 99%

Electrochemical Synthesis of Ammonia Based on a Perovskite LaCrO₃ Catalyst

et al. 2019

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Electrochemical synthesis of ammonia through the nitrogen reduction reaction (NRR) has the possibility to revolutionize our production of ammonia and to save our planet from both emissions and large energy consumption. In this study, a perovskite structured lanthanum chromite catalyst (LaCrO 3 ) is synthesized, characterized as well as electrochemically evaluated for NRR. The highest ammonia yield is obtained at À 0.8 V vs. reversible hydrogen electrode with an ammonia formation rate of 24.8 μg h À 1 mg À 1 cat , and a Faradaic efficiency of 15 %. Material calculation further confirms the possible mechanism of ammonia formation with the aid of LaCrO 3 catalyst. The resulting conclusion offers a great alternative with the easily produced and low-cost perovskite structured electrocatalysts for ammonia production.

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Section: Figurementioning

confidence: 99%

Electrochemical Synthesis of Ammonia Based on a Perovskite LaCrO₃ Catalyst

et al. 2019

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“…One of the cheapest and most abundant metals on earth, iron, is an effective dopant for greatly improving the nitrogen reduction reaction (NRR) performance of TiO 2 nanoparticles in ambient N 2 -to-NH 3 conversion. [5][6][7][8] Noble metals perform the NRR efficiently;however, their scarcity and high cost limits their application in large-scale N 2 reduction. The catalytic mechanism is further probed with theoretical calculations.…”

mentioning

confidence: 99%

“…[1][2][3] To date,the dominant industrial route for NH 3 synthesis is the Haber-Bosch process using N 2 and H 2 as the feeding gases,b ut this process operates at high temperature and high pressure,a nd consumes al arge amount of energy while emitting CO 2 . [5][6][7][8] Noble metals perform the NRR efficiently;however, their scarcity and high cost limits their application in large-scale N 2 reduction. [5][6][7][8] Noble metals perform the NRR efficiently;however, their scarcity and high cost limits their application in large-scale N 2 reduction.…”

mentioning

confidence: 99%

Greatly Improving Electrochemical N₂ Reduction over TiO₂ Nanoparticles by Iron Doping

Zhu

Xing

et al. 2019

Angewandte Chemie

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Titanium-based catalysts are needed to achieve electrocatalytic N 2 reduction to NH 3 with alarge NH 3 yield and ahigh Faradaic efficiency (FE). One of the cheapest and most abundant metals on earth, iron, is an effective dopant for greatly improving the nitrogen reduction reaction (NRR) performance of TiO 2 nanoparticles in ambient N 2 -to-NH 3 conversion. In 0.5 m LiClO 4 ,F e-doped TiO 2 catalyst attains ah igh FE of 25.6 %a nd al arge NH 3 yield of 25.47 mgh À1 mg cat À1 at À0.40 Vv ersus ar eversible hydrogen electrode.This performance compares favorably to those of all previously reported titanium-and iron-based NRR electrocatalysts in aqueous media. The catalytic mechanism is further probed with theoretical calculations.Asanessential activated nitrogen source,NH 3 is extensively used to manufacture dyes,p olymers,f ertilizers,a nd explosives,and it also serves as carbon-neutral energy carrier with high energy density. [1][2][3] To date,the dominant industrial route for NH 3 synthesis is the Haber-Bosch process using N 2 and H 2 as the feeding gases,b ut this process operates at high temperature and high pressure,a nd consumes al arge amount of energy while emitting CO 2 . [4] Electrochemical N 2 reduction offers an attractive alternative in an environmentally benign and sustainable manner,b ut the strong N N bond is fairly inert and thus difficult to break in ac hemical reaction, underlying the need for electrocatalysts with high activity in the nitrogen reduction reaction (NRR). [5][6][7][8] Noble metals perform the NRR efficiently;however, their scarcity and high cost limits their application in large-scale N 2 reduction. [8][9][10][11] NRR research has thus shifted to development of noble-metal-free alternatives. [12][13][14][15][16][17][18][19][20][21][22][23][24] TiO 2 is highly adaptable as asemiconductor catalyst because of its long-term thermodynamic stability,n atural abundance,a nd nontoxicity. [25] Recent studies have demonstrated that TiO 2 with oxygen defects has good electrocatalytic activity for the NRR, [26,27] and heteroatoms (B, [28] C, [29] V, [30] and Zr, [31] )a re effective dopants to enhance the NRR performances of TiO 2 catalysts. However,T i-based catalysts that simultaneously achieve al arge NH 3 yield with ah igh Faradaic efficiency (FE) are not available thus far.As one of the cheapest and most abundant metals on the earth, [32] Fe also exists in biological nitrogenases for natural N 2 fixation. [33] Fe compounds have been widely utilized as catalysts for artificial N 2 fixation in the Haber-Bosch [4] and electrochemical [34][35][36][37][38][39] processes.I ti st hus natural for us to explore use of Fe as ad opant for TiO 2 ,w hich has not been reported before.Herein, we report on our recent experimental results that Fe-doped TiO 2 is superior in performances for electrocatalytic N 2 reduction under ambient conditions.I n 0.5 m LiClO 4 ,t his catalyst achieves ah igh FE of 25.6 %a nd al arge NH 3 yield of 25.47 mgh À1 mg cat À1 at À0.40 Vv ersus ar eversible hydrogen electrode (...

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“…When water is used as a reactant, the reaction potential of synthetic ammonia will decrease with increasing temperature. When water boils, the reaction potential of synthetic ammonia increases as the temperature continues to rise . Hao and co‐workers also confirmed this in the article, as the reaction of the same system at different temperatures has different selectivity for the NRR.…”

Section: Strategy To Improve the Nrrmentioning

confidence: 56%

“…Nitrogen reduction is not a new concept; in nature, plants can convert nitrogen via multiple proton and electron transfer steps that achieves by the catalysis of iron‐molybdenum nitrogenase under ambient conditions . However, due to the complexity of the organism, its nitrogen fixation mechanism is still troublesome to study and understand.…”

Section: Fundamental Understanding Of the Nrrmentioning

confidence: 99%

Recent Advances in Electrochemical Synthesis of Ammonia through Nitrogen Reduction under Ambient Conditions

Wang

Chen

et al. 2020

ChemElectroChem

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Ammonia is an important chemical raw material, widely used in industry and agriculture, as well as an important energy storage intermediate and carbon‐free energy carrier. But, its production is limited to the traditional Haber‐Bosch process. Recently, electrochemical reduction of N2 has been attracting more and more attention, owing to the lower energy consumption and because it is environmentally friendly. However, there are a lot of problems that remain to be solved, and the main challenges are the low selectivity and catalytic activity when using this process. In this Review, we first summarize the recent development of electrocatalysts for electrochemical N2 reduction and elaborate on the reaction mechanisms of the nitrogen reduction reaction (NRR). In addition, the effects of different types of electrolyte on the NRR activity and electrolyte choice are discussed. Finally, the perspectives of electrochemical nitrogen reduction for conversion to ammonia are discussed.

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Recent progress in the electrochemical ammonia synthesis under ambient conditions

Cited by 176 publications

References 218 publications

Electrochemical Synthesis of Ammonia Based on a Perovskite LaCrO₃ Catalyst

Electrochemical Synthesis of Ammonia Based on a Perovskite LaCrO₃ Catalyst

Greatly Improving Electrochemical N₂ Reduction over TiO₂ Nanoparticles by Iron Doping

Recent Advances in Electrochemical Synthesis of Ammonia through Nitrogen Reduction under Ambient Conditions

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Recent progress in the electrochemical ammonia synthesis under ambient conditions

Cited by 176 publications

References 218 publications

Electrochemical Synthesis of Ammonia Based on a Perovskite LaCrO3 Catalyst

Electrochemical Synthesis of Ammonia Based on a Perovskite LaCrO3 Catalyst

Greatly Improving Electrochemical N2 Reduction over TiO2 Nanoparticles by Iron Doping

Recent Advances in Electrochemical Synthesis of Ammonia through Nitrogen Reduction under Ambient Conditions

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Electrochemical Synthesis of Ammonia Based on a Perovskite LaCrO₃ Catalyst

Electrochemical Synthesis of Ammonia Based on a Perovskite LaCrO₃ Catalyst

Greatly Improving Electrochemical N₂ Reduction over TiO₂ Nanoparticles by Iron Doping