DFT study of the defective carbon materials with vacancy and heteroatom as catalyst for NRR

Liu, Anmin; Yang, Yanan; Kong, Dezhen; Ren, Xuefeng; Gao, Mengfan; Liang, Xin; Yang, Qiyue; Zhang, Jiale; Gao, Liguo; Ma, Tingli

doi:10.1016/j.apsusc.2020.147851

Cited by 27 publications

(15 citation statements)

References 47 publications

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“…Specifically, a higher HOMO value represents stronger electron-donating ability, whereas a higher LUMO value suggests weaker electron-withdrawing ability. 65 The energy gap between HOMO and LUMO indicates the electron transfer capacity of a substance. 65 As shown in Figure 3c, rGO possessed the highest HOMO and lowest LUMO values among rGO, PAA, and SMX, suggesting both high electrondonating and high electron-withdrawing abilities of rGO.…”

Section: ■ Materials and Methodsmentioning

confidence: 99%

Reduced Graphene Oxide Triggers Peracetic Acid Activation for Robust Removal of Micropollutants: The Role of Electron Transfer

Kong

Zhao

Fan

et al. 2022

Environ. Sci. Technol.

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Peracetic acid (PAA) serves as a potent and lowtoxic oxidant for contaminant removal. Radical-mediated catalytic PAA oxidation processes are typically non-selective, rendering weakened oxidation efficacy under complex water matrices. Herein, we explored the usage of reduced graphene oxide (rGO) for PAA activation via a non-radical pathway. Outperforming the most catalytic PAA oxidation systems, the rGO−PAA system exhibits near-complete removal of typical micropollutants (MPs) within a short time (<2 min). Non-radical direct electron transfer (DET) from MPs to PAA plays a decisive role in the MP degradation, where accelerated DET is achieved by a higher potential of the rGO−PAA reactive surface complexes. Benefitting from DET, the rGO−PAA system shows robust removal of multiple MPs under complex water matrices and with low toxicity. Notably, in the DET regime, the electrostatic attraction of rGO to both PAA and target MP is a critical prerequisite for achieving efficient oxidation, depending on the conditions of solution pH and MP pK a . A heatmap model building on such an electrostatic interaction is further established as guidance for regulating the performance of the DET-mediated PAA oxidation systems. Overall, our work unveils the imperative role of DET for rGO-activated PAA oxidation, expanding the knowledge of PAA-based water treatment strategies.

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Section: ■ Materials and Methodsmentioning

confidence: 99%

Reduced Graphene Oxide Triggers Peracetic Acid Activation for Robust Removal of Micropollutants: The Role of Electron Transfer

Kong

Zhao

Fan

et al. 2022

Environ. Sci. Technol.

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“…This is consistent with the research of Oschatz et al [45] In addition to interface regulation and atom adulteration, construction of a defect engineering is also viewed as a strategy that favors N 2 activation. For example, Ma et al [64] concluded that vacancy defects in N or S atom-doped graphene could increase the reaction activity of graphene according to DFT, and the highly active sites of graphene defects are mainly distributed around carbon atoms. He et al [57] prepared defectenriched ultrathin porous graphene (DG) by the fuse salt method.…”

Section: Carbon-based Non-metallic Materialsmentioning

confidence: 99%

Development of Carbon‐Based Electrocatalysts for Ambient Nitrogen Reduction Reaction: Challenges and Perspectives

2021

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Ammonia is an important chemical and a potential carbon-free hydrogen-storage material. Currently, the industrial synthesis of ammonia is mainly achieved via the Haber-Bosch method, which requires high energy, temperatures, and pressures. An alternative method involves the electrocatalytic nitrogen reduction reaction (NRR), which uses an aqueous solution as a medium and requires mild reaction conditions. The key to the NRR is to select an appropriate catalyst to increase the ammonia yield and Faradic efficiency. With their diverse structures and easy regulation, carbon-based materials can provide abundant active sites for nitrogen absorption and excitation. Moreover, they are abundant, low cost, and readily available, making them promising for use in NRR applications. Accordingly, we review the latest progress in using carbonbased materials in the NRR, and the future development prospects of NRR catalysts are discussed. Finally, challenges and perspectives of the future research of NRR catalysts are provided.

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“…18,19 In recent years, electrochemical production of NH 3 via nitrogen reduction reaction (NRR) has been identied as a highly appealing strategy to substitute the traditional Haber-Bosch process. [20][21][22] In general, however, electrochemical NRR is still impeded by two major issues: [23][24][25] low NRR activity and low NH 3 selectivity.…”

Section: Introductionmentioning

confidence: 99%

Nitric oxide reduction reaction for efficient ammonia synthesis on topological nodal-line semimetal Cu₂Si monolayer

et al. 2022

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DFT study of the defective carbon materials with vacancy and heteroatom as catalyst for NRR

Cited by 27 publications

References 47 publications

Reduced Graphene Oxide Triggers Peracetic Acid Activation for Robust Removal of Micropollutants: The Role of Electron Transfer

Reduced Graphene Oxide Triggers Peracetic Acid Activation for Robust Removal of Micropollutants: The Role of Electron Transfer

Development of Carbon‐Based Electrocatalysts for Ambient Nitrogen Reduction Reaction: Challenges and Perspectives

Nitric oxide reduction reaction for efficient ammonia synthesis on topological nodal-line semimetal Cu₂Si monolayer

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DFT study of the defective carbon materials with vacancy and heteroatom as catalyst for NRR

Cited by 27 publications

References 47 publications

Reduced Graphene Oxide Triggers Peracetic Acid Activation for Robust Removal of Micropollutants: The Role of Electron Transfer

Reduced Graphene Oxide Triggers Peracetic Acid Activation for Robust Removal of Micropollutants: The Role of Electron Transfer

Development of Carbon‐Based Electrocatalysts for Ambient Nitrogen Reduction Reaction: Challenges and Perspectives

Nitric oxide reduction reaction for efficient ammonia synthesis on topological nodal-line semimetal Cu2Si monolayer

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Nitric oxide reduction reaction for efficient ammonia synthesis on topological nodal-line semimetal Cu₂Si monolayer