High-Performance Electrohydrogenation of N2 to NH3 Catalyzed by Multishelled Hollow Cr2O3 Microspheres under Ambient Conditions

Zhang, Ya; Qiu, Weibin; Ma, Yongjun; Luo, Yonglan; Tian, Ziqi; Cui, Guanwei; Xie, Fengyu; Chen, Liang; Sun, Xuping; Sun, Xuping

doi:10.1021/acscatal.8b02311

Cited by 274 publications

(148 citation statements)

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“…Both NH 3 yields and FEs initially increase with potential being more negative. , 6.78%), [51] and TiO 2 -rGO (15.13 µg h −1 mg −1 cat. These results might result from the competitive hydrogen-evolving process, which can be suppressed in nonaqueous media to achieve higher current efficiency.…”

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confidence: 99%

Electrocatalytic Hydrogenation of N₂to NH₃by MnO: Experimental and Theoretical Investigations

et al. 2018

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NH3 is a valuable chemical with a wide range of applications, but the conventional Haber–Bosch process for industrial‐scale NH3 production is highly energy‐intensive with serious greenhouse gas emission. Electrochemical reduction offers an environmentally benign and sustainable route to convert N2 to NH3 at ambient conditions, but its efficiency depends greatly on identifying earth‐abundant catalysts with high activity for the N2 reduction reaction. Here, it is reported that MnO particles act as a highly active catalyst for electrocatalytic hydrogenation of N2 to NH3 with excellent selectivity. In 0.1 m Na2SO4, this catalyst achieves a high Faradaic efficiency up to 8.02% and a NH3 yield of 1.11 × 10−10 mol s−1 cm−2 at −0.39 V versus reversible hydrogen electrode, with great electrochemical and structural stability. On the basis of density functional theory calculations, MnO (200) surface has a smaller adsorption energy toward N than that of H with the *N2 → *N2H transformation being the potential‐determining step in the nitrogen reduction reaction.

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Electrocatalytic Hydrogenation of N₂to NH₃by MnO: Experimental and Theoretical Investigations

et al. 2018

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“…Finally, the difference in the physicochemical properties of different surfaces should also be taken into consideration. For example, it has been reported that the internal surfaces may be less capped relative to external surfaces in multi‐shelled hollow Cr 2 O 3 microspheres, implying that the internal surfaces are catalytically more active (Figure d) . Overall, pore structure control was demonstrated to be effective for enhancing NRR, although further research in this field is warranted.…”

Section: Design Principles For Electrocatalystsmentioning

confidence: 94%

Section: Design Principles For Electrocatalystsmentioning

confidence: 99%

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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“…Previous studies have proved that noble‐metal based catalysts are efficient N 2 reduction reaction (NRR) electrocatalysts, but their large‐scale uses are severely limited by the high cost and rareness. Considerable recent attention has thus focused on earth‐abundant transition metal‐based alternatives to effectively catalyze the NRR . Nevertheless, metal ions may be released from such catalysts, leading to environmental pollution.…”

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Oxygen‐Doped Porous Carbon Nanosheet for Efficient N₂ Fixation to NH₃ at Ambient Conditions

Chen

Huang

et al. 2019

ChemistrySelect

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NH3 is one of the largest‐volume industrial chemicals synthesized in the world. It not only is a kind of important chemical base materials to produce fertilizers, plastics and explosives, but also can serve as a clean energy carrier with high hydrogen content for a sustainable energy supply. N2 is the most abundant gas in atmosphere, but its inert character caused by the strong triple bond, impedes itself from being converted to NH3. In nature, this shortcoming is overcome by biological N2 fixation utilizing nitrogenase enzymes. Industrially, fixation of N2‐to‐NH3 prevailingly depends on Haber‐Bosch process using Ru‐ or Fe‐based catalysts, but this process consumes large energy and emits heavy carbon which increases crisis of global warming.

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High-Performance Electrohydrogenation of N₂ to NH₃ Catalyzed by Multishelled Hollow Cr₂O₃ Microspheres under Ambient Conditions

Cited by 274 publications

References 53 publications

Electrocatalytic Hydrogenation of N₂to NH₃by MnO: Experimental and Theoretical Investigations

Electrocatalytic Hydrogenation of N₂to NH₃by MnO: Experimental and Theoretical Investigations

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

Oxygen‐Doped Porous Carbon Nanosheet for Efficient N₂ Fixation to NH₃ at Ambient Conditions

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High-Performance Electrohydrogenation of N2 to NH3 Catalyzed by Multishelled Hollow Cr2O3 Microspheres under Ambient Conditions

Cited by 274 publications

References 53 publications

Electrocatalytic Hydrogenation of N2to NH3by MnO: Experimental and Theoretical Investigations

Electrocatalytic Hydrogenation of N2to NH3by MnO: Experimental and Theoretical Investigations

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

Oxygen‐Doped Porous Carbon Nanosheet for Efficient N2 Fixation to NH3 at Ambient Conditions

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High-Performance Electrohydrogenation of N₂ to NH₃ Catalyzed by Multishelled Hollow Cr₂O₃ Microspheres under Ambient Conditions

Electrocatalytic Hydrogenation of N₂to NH₃by MnO: Experimental and Theoretical Investigations

Electrocatalytic Hydrogenation of N₂to NH₃by MnO: Experimental and Theoretical Investigations

Oxygen‐Doped Porous Carbon Nanosheet for Efficient N₂ Fixation to NH₃ at Ambient Conditions