Distorted spinel ferrite heterostructure triggered by alkaline earth metal substitution facilitates nitrogen localization and electrocatalytic reduction to ammonia

Jiang, Yuzhuo; Wang, Mengfan; Zhang, Lifang; Liu, Sisi; Cao, Yufeng; Qian, Siyi; Cheng, Yu; Xu, Xinnan; Yan, Chenglin; Qian, Tao

doi:10.1016/j.cej.2022.138226

Cited by 42 publications

(29 citation statements)

References 38 publications

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“…The ability of theoretical calculations to explore atomic-level details of reaction systems holds great potential for the deeper understanding of C−N bond formation. Various computational methods such as DFT calculations, 124 molecular dynamics simulations, 125 and finite element simulations 126 covering orders of magnitude in time and length scales are able to give detailed insights into the reaction mechanisms, reagents distribution, and interface structures, which are strongly correlated with the reaction thermodynamics and kinetics. Moreover, the combination of these computational methods could further bridge the gap between macroscale experimental data and nanoscale computational insights with increasing fidelity.…”

Section: Discussionmentioning

confidence: 99%

Turning Waste into Wealth: Sustainable Production of High-Value-Added Chemicals from Catalytic Coupling of Carbon Dioxide and Nitrogenous Small Molecules

et al. 2022

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Carbon neutrality is one of the central topics of not only the scientific community but also the majority of human society. The development of highly efficient carbon dioxide (CO2) capture and utilization (CCU) techniques is expected to stimulate routes and concepts to go beyond fossil fuels and provide more economic benefits for a carbon-neutral economy. While various single-carbon (C1) and multi-carbon (C2+) products have been selectively produced to date, the scope of CCU can be further expanded to more valuable chemicals beyond simple carbon species by integration of nitrogenous reactants into CO2 reduction. In this Review, research progress toward sustainable production of high-value-added chemicals (urea, methylamine, ethylamine, formamide, acetamide, and glycine) from catalytic coupling of CO2 and nitrogenous small molecules (NH3, N2, NO3 –, and NO2 –) is highlighted. C–N bond formation is a key mechanistic step in N-integrated CO2 reduction, so we focus on the possible pathways of C–N coupling starting from the CO2 reduction and nitrogenous small molecules reduction processes as well as the catalytic attributes that enable the C–N coupling. We also propose research directions and prospects in the field, aiming to inspire future investigations and achieve comprehensive improvement of the performance and product scope of C–N coupling systems.

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Section: Discussionmentioning

confidence: 99%

Turning Waste into Wealth: Sustainable Production of High-Value-Added Chemicals from Catalytic Coupling of Carbon Dioxide and Nitrogenous Small Molecules

et al. 2022

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“…[71] Several uplifting experimental results of NRR have also been obtained in acidic medium through appropriate selection of electrolytes. [23,72] Figure 4a-c exhibited the profiles of the potential, proton and N 2 concentration profiles around the catalyst surface with a fixed saturated N 2 concentration and different HCl concentrations in the electrolytes (10 −3 , 10 −2 , 10 −1 10 0 m). Higher H + concentrations in the electrolyte reduce N 2 concentration near the catalyst surface (Figure 4b,c).…”

Section: Acidic Electrolytementioning

confidence: 99%

Deciphering Electrolyte Selection for Electrochemical Reduction of Carbon Dioxide and Nitrogen to High‐Value‐Added Chemicals

Cheng

Liu

et al. 2023

Adv Funct Materials

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Electrochemical reduction of CO 2 (CO 2 RR) and nitrogen (NRR) constitute alternatives to fossil fuel-based technologies for the production of high-valueadded chemicals. Yet their practical application is still hampered by the low energy and Faradaic efficiencies although numerous efforts have been paid to overcome the fatal shortcomings. To date, most studies have focused on designing and developing advanced electrocatalysts, while the understanding of electrolyte, which would significantly influence the reaction microenvironment, are still not enough to provide insight to construct highly active and selective electrochemical systems. Here, a comprehensive review of the different electrolytes participating in the CO 2 RR and NRR is provided, including acidic, neutral, alkaline, and water-in-salt electrolyte as aqueous electrolytes, as well as organic electrolyte, ionic-liquids electrolyte, and the mixture of the two as non-aqueous electrolytes. Through the discussion of the roles of these various electrolytes, it is aimed to grasp their essential function during the electrochemical process and how these functions can be used as design parameters for improving electrocatalytic performance. Finally, priorities for future studies are suggested to support the in-depth understanding of the electrolyte effects and thus guide efficient selection for next-generation gasinvolving electrochemical reactions.

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“…Theoretical investigations based on DFT calculations mainly focus on the intrinsic properties of catalysts, such as reaction energy barrier or electron orbital information, and are of prime significance in understanding the mechanism in the NRR process. [100] Moreover, through DFT calculations, the Gibbs reaction energies of catalysts can be determined, and several factors, including defect, facet, and functionalization, are thoroughly probed. A volcano map regarding different metal surfaces was illustrated by Nørskov et al according to the linear relation between the reaction intermediates and the chemisorption energy of N adatoms (Figure 5a).…”

Section: Dft Calculations For Nrr Investigationmentioning

confidence: 99%

Advancing the Electrochemistry of Gas‐Involved Reactions through Theoretical Calculations and Simulations from Microscopic to Macroscopic

Liu

Wang

et al. 2022

Adv Funct Materials

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Nowadays, gas‐involved electrochemical reactions, such as carbon dioxide reduction reaction (CO2RR), nitrogen reduction reaction (NRR), and hydrogen evolution reaction (HER), have gradually become viable solutions to the global environmental pollution and energy crisis. However, their further development is inseparable from the in‐depth understanding of reaction mechanisms, which are incredibly complicated and cannot be satisfied by experiments alone. In this context, theoretical calculations and simulations are of great significance in establishing composition–structure–activity relationships, providing priceless mechanistic discernment and predicting prospective electrocatalysts and systems. Among them, density functional theory (DFT), molecular dynamics (MD) simulations, and finite element simulation (FES) are emerging as three mature theoretical tools. This paper presents a review of the basic principles and research progress of DFT, MD, and FES to deepen the understanding of CO2RR, NRR, and HER. Some remarkable work around theoretical calculations and simulations are highlighted, including the utilization of DFT to investigate the intrinsic properties of catalysts and MD or FES to restore the whole reaction systems from different temporal and spatial scales. Eventually, to sum up, forward‐looking insights and perspectives on the future optimizations and application modes of the three computational techniques to compensate for their shortcomings and limitations are presented.

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Distorted spinel ferrite heterostructure triggered by alkaline earth metal substitution facilitates nitrogen localization and electrocatalytic reduction to ammonia

Cited by 42 publications

References 38 publications

Turning Waste into Wealth: Sustainable Production of High-Value-Added Chemicals from Catalytic Coupling of Carbon Dioxide and Nitrogenous Small Molecules

Turning Waste into Wealth: Sustainable Production of High-Value-Added Chemicals from Catalytic Coupling of Carbon Dioxide and Nitrogenous Small Molecules

Deciphering Electrolyte Selection for Electrochemical Reduction of Carbon Dioxide and Nitrogen to High‐Value‐Added Chemicals

Advancing the Electrochemistry of Gas‐Involved Reactions through Theoretical Calculations and Simulations from Microscopic to Macroscopic

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