A review on the non-thermal plasma-assisted ammonia synthesis technologies

Peng, Peng; Chen, Paul; Schiappacasse, Charles; Zhou, Nan; Anderson, Erik; Chen, Dongjie; Liu, Juer; Cheng, Yanling; Hatzenbeller, Raymond; Addy, Min; Zhang, Yaning; Liu, Yuhuan; Ruan, Roger

doi:10.1016/j.jclepro.2017.12.229

Cited by 181 publications

(187 citation statements)

References 104 publications

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“…Hence, it is essential to gain a clear insight into the possible reaction pathways under plasma environment. There has been some work carried out on ammonia synthesis using plasma catalysis . Over the years, energy yields have been as high as 35 g‐NH 3 /kWh while using a pulsed AC atmospheric pressure dielectric barrier discharge (DBD) reactor, showing the potential of small‐scale production of ammonia using plasma‐catalysis.…”

Section: Introductionmentioning

confidence: 99%

“…There has been some work carried out on ammonia synthesis using plasma catalysis. [16][17][18] Over the years, energy yields have been as high as 35 g-NH 3 /kWh while using a pulsed AC atmospheric pressure dielectric barrier discharge (DBD) reactor, [19] showing the potential of small-scale production of ammonia using plasma-catalysis. Recently, Peng et al [20] employed a pulsed DBD reactor with MgCl 2 acting as catalyst and absorbent, leading to enhanced conversions.…”

Section: Introductionmentioning

confidence: 99%

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Enhancement of the Yield of Ammonia by Hydrogen‐Sink Effect during Plasma Catalysis

et al. 2019

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Plasma‐catalytic ammonia synthesis has been known since the early 1900s, but only until now efforts to optimize catalysts for this purpose are emerging. Here, we investigate various transition metals, low‐melting‐point metals, and gallium‐rich alloy catalysts for their activity towards ammonia production under a plasma environment. The best three pure metal catalysts were Ni, Sn and Au, which are not traditional catalysts for the current industrial ammonia synthesis. The ammonia yields for these catalysts were 34 %, 29 %, and 19 %, respectively. Synergistic effects were detected when employing alloys, as some alloys presented ∼25–50 % higher yields than their constituent metals. The employed metals were classified into two categories. Category I metals (Cu, Ag, Au and Fe), which are nitrophobic (excluding Fe, the Haber‐Bosch catalyst) and poor hydrogen sinks. For these metals, the measured concentration of Hα in the gas phase tended to correlate inversely with ammonia yield and directly with the H binding strength on the catalyst surface. Category II metals (Ga, In, Sn and Ni), which are good hydrogen sinks, tend to have a lower concentration of Hα in the gas phase than that of category I metals, which is consistent with their expected sink behavior. For these metals, the concentration of Hα correlates with ammonia yield. Plasma characterization experiments and DFT calculations suggest that the higher performance of Ni and Sn is related to the benefit of dissolving hydrogen to slow down H recombination, which is a feature that could be potentially optimized in future studies by rationally altering the catalyst composition.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Enhancement of the Yield of Ammonia by Hydrogen‐Sink Effect during Plasma Catalysis

et al. 2019

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“…[22,23] Since then, Shah et al explored the use of various metal meshes (Fe, Cu, Pd, Ag), low-melting alloys, and metal-organic frameworks as catalysts for ammonia synthesis under non-thermalp lasma conditions. [22,23] Since then, Shah et al explored the use of various metal meshes (Fe, Cu, Pd, Ag), low-melting alloys, and metal-organic frameworks as catalysts for ammonia synthesis under non-thermalp lasma conditions.…”

Section: Plasma-catalyst Interactionsmentioning

confidence: 99%

“…First, the breakdown of nitrogen gas, at hermodynamically stable and kinetically inert molecule, is extremelyc hallenging under atmosphericc onditions. Although the reactor designs and catalysts elections for the general plasma-assisted nitrogen fixation processes [14,21] and NH 3 synthesis [22,23] have already been summarized, the underlying synergistic mechanismso fN TPNF have not been reviewed. Additionally,t he vibrational excitation of dinitrogen molecules can decrease the activation barrier under high temperature-high pressure conditions.…”

Section: Introductionmentioning

confidence: 99%

“…[20] By implementing certain non-thermal plasma-assisted nitrogen fixation (NTPNF) methods,t he use of hydrogen gas can be circumvented by using water and nitrogen (or air) as reactants, thereby significantly reducing the environmental impact of fixing nitrogen. Although the reactor designs and catalysts elections for the general plasma-assisted nitrogen fixation processes [14,21] and NH 3 synthesis [22,23] have already been summarized, the underlying synergistic mechanismso fN TPNF have not been reviewed. The chemical principles involved in NTPNFi nclude reactions occurring in all of the gas/liquid/solid environments.…”

Section: Introductionmentioning

confidence: 99%

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Sustainable Non‐Thermal Plasma‐Assisted Nitrogen Fixation—Synergistic Catalysis

et al. 2019

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In this Minireview, the multiple chemical synergies present in catalytic non‐thermal plasma‐assisted nitrogen fixation (NTPNF) are uncovered through a critical exploration of the underlying mechanisms, during which the catalyst, plasma, and reactants play different roles. For the gas‐phase NTPNF, the synergies consist of different aspects of the catalytic pathways such as electron‐impact dissociation; Zeldovich mechanism in the PNO interactions; and Eley–Rideal, Langmuir–Hinshelwood, surface adsorption, and diffusion mechanisms for the plasma–catalyst interactions. The synergies within the gas–liquid NTPNF involve contributions of plasma and UV excitation to the gas‐phase reactions and the UV excitation of molecules at the liquid–surface interface, which improves synthesis of aqueous nitrate, nitrite, and ammonium products. Based on the various synergistic mechanisms during NTPNF, future potential applications are proposed for how NTPNF could benefit the sustainable nitrogen fixation industry.

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The Role of Defects in Metal–Organic Frameworks for Nitrogen Reduction Reaction: When Defects Switch to Features

Khalil

Xue

Liu

et al. 2021

Adv Funct Materials

109

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The electrochemical nitrogen reduction reaction (NRR), a contributor for producing ammonia under mild conditions sustainably, has recently attracted global research attention. Thus far, the design of highly efficient electrocatalysts to enhance NRR efficiency is a specific focus of the research. Among them, defect engineering of electrocatalysts is considered a significant way to improve electrocatalytic efficiency by regulating the electronic state and providing more active sites that can give electrocatalysts better physicochemical properties. Recently, metal–organic frameworks (MOFs), along with their derivatives, have captured immense interest in electrocatalytic reactions owing to not only their large surface area and high porosity but also the ability to create rich defects in their structures. Hence, they can provide plenty of exposed active sites for electron transfer, NN cleavage, and N2 adsorption to enhance NRR performance. Herein, the concept, the in situ characterizations techniques for defects, and the most common ways to create defects into MOFs have been summarized. Furthermore, the recent advances of MOF‐based electrocatalysts towards NRR have been recapitulated. Ultimately, the major challenges and outlook of defects in MOFs for NRR are proposed. This paper is anticipated to provide critical guidelines for optimizing NRR electrocatalysts.

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A review on the non-thermal plasma-assisted ammonia synthesis technologies

Cited by 181 publications

References 104 publications

Enhancement of the Yield of Ammonia by Hydrogen‐Sink Effect during Plasma Catalysis

Enhancement of the Yield of Ammonia by Hydrogen‐Sink Effect during Plasma Catalysis

Sustainable Non‐Thermal Plasma‐Assisted Nitrogen Fixation—Synergistic Catalysis

The Role of Defects in Metal–Organic Frameworks for Nitrogen Reduction Reaction: When Defects Switch to Features

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