Comprehensive understanding of the thriving electrocatalytic nitrate/nitrite reduction to ammonia under ambient conditions

Zhao, Xinying; Jiang, Yuzhuo; Wang, Mengfan; Huan, Yunfei; Cheng, Qiyang; He, Yanzheng; Qian, Tao; Yan, Chenglin

doi:10.1016/j.jechem.2023.12.024

Cited by 15 publications

(1 citation statement)

References 197 publications

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“…Ammonia (NH 3 ) is a crucial nitrogen-containing chemical widely used in various industries, primarily in the production of nitrogen-based fertilizers, plastics, refrigerants, and dyes. − It is also regarded as a green, clean energy source due to its mild combustion products and high energy density. Presently, the dominant industrial ammonia production method is the Haber-Bosch (H–B) process, which requires high temperatures (400–500 °C) and high pressures (150–300 atm) − and leads to massive fossil energy consumption and carbon dioxide emissions. , Given the dwindling reserves of fossil fuels and the escalating environmental concerns, it is urgent to develop an innovative alternative technology to displace the conventional H–B process for ammonia synthesis . As is known, NO 3 – has a higher solubility in water compared to N 2 .…”

Section: Introductionmentioning

confidence: 99%

CuCo₂O₄/CuO Heterostructure with Oxygen Vacancies Induced by Plasma for Electrocatalytic Nitrate Reduction to Ammonia

Liu,

Cheng,

Zhao

et al. 2024

Inorg. Chem.

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Electrochemical nitrate reduction (NO 3 RR) to ammonia production is regarded as one of the potential alternatives for replacing the Haber-Bosch technology for realizing artificial ammonia synthesis. In this study, a CuCo 2 O 4 /CuO−Ar heterostructure in the shape of dandelion nanospheres formed by nanoarrays has been successfully constructed, demonstrating excellent NO 3 RR performance. Experimental results indicate that Ar plasma etching of CuCo 2 O 4 /CuO-Ar significantly increases the content of oxygen vacancies compared to the sample of CuCo 2 O 4 /CuO-Air etched by air plasma, resulting in improved NO 3 RR performance. Density functional theory calculations further confirm that the existence of more oxygen vacancies effectively decreases the energy barrier of nitrate adsorption, which is due to the generation of more oxygen vacancies facilitating nitrate adsorption and weakening the N−O bonds of nitrate after plasma treatment. As a result, CuCo 2 O 4 /CuO-Ar exhibits a high NH 3 yield of 0.55 mmol h −1 cm −2 and a Faraday efficiency of 95.07% at the optimal potential of −0.9 V (vs RHE) in a neutral medium. Importantly, CuCo 2 O 4 /CuO-Ar also showcases excellent electrocatalytic stability. This study presents new views on the design and structure regulation of NO 3 RR electrocatalysts and their potential applications in the future.

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Section: Introductionmentioning

confidence: 99%

CuCo₂O₄/CuO Heterostructure with Oxygen Vacancies Induced by Plasma for Electrocatalytic Nitrate Reduction to Ammonia

Liu,

Cheng,

Zhao

et al. 2024

Inorg. Chem.

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Hydration‐effect Boosted Active Hydrogen Facilitates Neutral Ammonia Electrosynthesis from Nitrate Reduction

Zhang,

Cheng,

Duan

et al. 2024

Adv Funct Materials

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Electrocatalytic nitrate reduction to ammonia (NO3RR) in a neutral medium is a green and effective strategy for treating nitrate pollution meanwhile producing ammonia. However, the insufficient active hydrogen (H*) on the catalyst surface resulting from the sluggish Volmer step (H2O → H+ + OH−), and the competitive hydrogen evolution reaction (HER) caused by H* coupling severely restrict the enhancement of NO3RR activity. Herein, a hydration‐effect boosted H*‐rich strategy facilitating neutral ammonia electrosynthesis from nitrate reduction is proposed. The introduction of the hydration‐effect‐promoting element aluminum into the copper‐based catalyst forming CuAlO2, which adjusts the electron density distribution in the catalyst system, and the resulting hydration‐effect significantly promotes the H* generation in a neutral medium. Moreover, the rapid charge transfer at the CuO/CuAlO2 interface facilitates the reaction kinetics and the H* diffusion. More importantly, the introduction of Al weakens the overly strong adsorption of intermediates by CuO, thereby accelerating the hydrogenation process and suppressing HER. Thus, under neutral conditions, CuO/CuAlO2 reached a Faradaic efficiency and an ammonia yield as high as 97.81 ± 1.94% and 10.21 ± 0.64 mg h−1 cm−2 at −1.0 V versus RHE toward NO3RR.

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Molecular Dynamics Simulations for Electrocatalytic CO₂ Reduction: Bridging Macroscopic Experimental Observations and Microscopic Explanatory Mechanisms

He,

Wang,

et al. 2024

Adv Funct Materials

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Electrocatalytic carbon dioxide reduction reaction (CO2RR) has been recognized as a promising route to convert carbon emissions to high‐value chemicals and fuels. Significant breakthroughs are usually inseparable from deeper understanding of reaction mechanisms. To this end, molecular dynamics (MD) simulations have been invaluable in providing detailed insights into elucidation of complex reaction pathways and prediction of overall electrochemical performance, thus bridging macroscopic experimental observations and microscopic explanatory mechanisms. Directed by MD simulations, tremendous efforts have been devoted toward enhancing the CO2RR with rational design of electrocatalyst and efficient construction of electrode/electrolyte interface. Herein, a comprehensive review of applications of MD simulations in CO2RR is emerged. To begin with, specific fundamentals along with familiar methods such as algorithm and force fields of various MD simulations have been summed up. Followed, employment of MD simulations in optimization of CO2RR is introduced, encompassing interpretation of electrocatalyst activity, explanation of electrolyte effect, and investigation of electrode microenvironment. Definitively, imminent challenges and avenues for optimization in future MD simulations are contemplated, envisioning this review as a guiding beacon for future endeavors aimed at harnessing MD simulations to propel CO2RR toward a realm of heightened efficiency, economic viability, and practical utility.

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Comprehensive understanding of the thriving electrocatalytic nitrate/nitrite reduction to ammonia under ambient conditions

Cited by 15 publications

References 197 publications

CuCo₂O₄/CuO Heterostructure with Oxygen Vacancies Induced by Plasma for Electrocatalytic Nitrate Reduction to Ammonia

CuCo₂O₄/CuO Heterostructure with Oxygen Vacancies Induced by Plasma for Electrocatalytic Nitrate Reduction to Ammonia

Hydration‐effect Boosted Active Hydrogen Facilitates Neutral Ammonia Electrosynthesis from Nitrate Reduction

Molecular Dynamics Simulations for Electrocatalytic CO₂ Reduction: Bridging Macroscopic Experimental Observations and Microscopic Explanatory Mechanisms

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Comprehensive understanding of the thriving electrocatalytic nitrate/nitrite reduction to ammonia under ambient conditions

Cited by 15 publications

References 197 publications

CuCo2O4/CuO Heterostructure with Oxygen Vacancies Induced by Plasma for Electrocatalytic Nitrate Reduction to Ammonia

CuCo2O4/CuO Heterostructure with Oxygen Vacancies Induced by Plasma for Electrocatalytic Nitrate Reduction to Ammonia

Hydration‐effect Boosted Active Hydrogen Facilitates Neutral Ammonia Electrosynthesis from Nitrate Reduction

Molecular Dynamics Simulations for Electrocatalytic CO2 Reduction: Bridging Macroscopic Experimental Observations and Microscopic Explanatory Mechanisms

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Product

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CuCo₂O₄/CuO Heterostructure with Oxygen Vacancies Induced by Plasma for Electrocatalytic Nitrate Reduction to Ammonia

CuCo₂O₄/CuO Heterostructure with Oxygen Vacancies Induced by Plasma for Electrocatalytic Nitrate Reduction to Ammonia

Molecular Dynamics Simulations for Electrocatalytic CO₂ Reduction: Bridging Macroscopic Experimental Observations and Microscopic Explanatory Mechanisms