Cooperatively interface role of surface atoms and aqueous media on single atom catalytic property for H2O2 synthesis

Fang, Qiaojun; Pan, Jin-kong; Zhang, Wei; Sun, Fu-li; Chen, Wenxian; Yu, Yingda; Hu, Anfu; Zhuang, Gui‐Lin

doi:10.1016/j.jcis.2022.03.052

Cited by 12 publications

(10 citation statements)

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“…The initial adsorption energy of an intact H 2 O 2 molecule on the catalyst is only −0.12 eV, which is a weak physical adsorption behavior, and the activation of H 2 O 2 on the catalyst may result in two configurations, *O + H 2 O and 2*OH, as shown in Figure S2. The *O + H 2 O configuration has an adsorption energy of −2.58 eV and is the most energetically stable product after H 2 O 2 activation, which is consistent with previous studies. , It is notable that H 2 O 2 is a green oxidant and its activation products have great oxidation properties. Based on previous studies, *OH is a principal product of H 2 O 2 activation .…”

Section: Resultssupporting

confidence: 91%

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NO Oxidation Using H₂O₂ at a Single-Atom Iron Catalyst

et al. 2023

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Nitrogen oxide (NO) is a major worldwide environmental pollutant, which can be eliminated effectively by catalytic oxidation. However, conventional catalysts generally suffer from poor activity and low oxidation rates, limiting the development of gas pollutant removal. To overcome this issue, the high activity of a single-atom catalyst and the strong oxidizability of H2O2 are proposed for the catalytic oxidation of NO in this work. Herein, the 14 reaction pathways of NO oxidation using H2O2 were obtained through spin-polarized density functional theory calculation with van der Waals corrections and microkinetic modeling. Considering the possible H2O2 activation products of *OH, *OOH, and *O, we obtained the dominant reaction pathways for different oxidizing species: (i) Langmuir–Hinshelwood mechanism of *OH (mainly forming *HNO2), (ii) Eley–Rideal mechanism of *O (forming *NO2), and (iii) *OOH (forming *HNO3), with the energy barriers of 0.94, 1.42, and 0.14 eV, respectively. Among the three reaction patterns, NO oxidation using *OOH is the most favorable, with the highest reaction rate. *HNO3 is the most likely oxidation product of NO oxidation using H2O2. Meanwhile, it is notable that the *OH catalytic oxidation of NO has multiple reaction pathways and products, including HNO2, NO2, and HNO3. Compared to the use of conventional oxidants and catalysts, using H2O2 to oxidize NO at Fe–N4–C catalyst has lower reaction energy barriers and allows for the deep oxidation of NO. This study illustrates the reaction pathway of NO oxidation using H2O2 and demonstrates that it is theoretically feasible, which provides guidance for the subsequent preparation of the material.

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Section: Resultssupporting

confidence: 91%

“…58 eV and is the most energetically stable product after H 2 O 2 activation, which is consistent with previous studies. 23,37 It is notable that H 2 O 2 is a green oxidant and its activation products have great oxidation properties. Based on previous studies, *OH is a principal product of H 2 O 2 activation.…”

Section: Computation and Modeling Methodsmentioning

confidence: 99%

NO Oxidation Using H₂O₂ at a Single-Atom Iron Catalyst

et al. 2023

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“…This temperature has been widely accepted for evaluating thermal stability. 71–74 It was found that after 5000 fs, they could still maintain structural integrity, and their average potential energy remained almost unchanged, indicating their high thermal stabilities. Moreover, we also investigated the electronic behavior of these eight structures by calculating their density of states (DOSs).…”

Section: Resultsmentioning

confidence: 99%

Realizing a high OER activity in new single-atom catalysts formed by introducing TMN_x (x = 3 and 4) units into carbon nanotubes using high-throughput calculations

Yang,

Yu,

Chen

2024

Nanoscale

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“…Also, the large number of approximations and the limited number of calculated atoms make the DFT results somewhat inaccurate and lacking in generality. For AIMD [152,153], the large computational workload makes it unsuitable for complex systems. In addition, the established descriptors are scanty and with strong specificity, which further limits the use of these calculations.…”

Section: Inferring Reaction Mechanism By Associating In-situ Studies ...mentioning

confidence: 99%

A Review of In-Situ Techniques for Probing Active Sites and Mechanisms of Electrocatalytic Oxygen Reduction Reactions

et al. 2022

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Electrocatalytic oxygen reduction reaction (ORR) is one of the most important reactions in electrochemical energy technologies such as fuel cells and metal–O2/air batteries, etc. However, the essential catalysts to overcome its slow reaction kinetic always undergo a complex dynamic evolution in the actual catalytic process, and the concomitant intermediates and catalytic products also occur continuous conversion and reconstruction. This makes them difficult to be accurately captured, making the identification of ORR active sites and the elucidation of ORR mechanisms difficult. Thus, it is necessary to use extensive in-situ characterization techniques to proceed the real-time monitoring of the catalyst structure and the evolution state of intermediates and products during ORR. This work reviews the major advances in the use of various in-situ techniques to characterize the catalytic processes of various catalysts. Specifically, the catalyst structure evolutions revealed directly by in-situ techniques are systematically summarized, such as phase, valence, electronic transfer, coordination, and spin states varies. In-situ revelation of intermediate adsorption/desorption behavior, and the real-time monitoring of the product nucleation, growth, and reconstruction evolution are equally emphasized in the discussion. Other interference factors, as well as in-situ signal assignment with the aid of theoretical calculations, are also covered. Finally, some major challenges and prospects of in-situ techniques for future catalysts research in the ORR process are proposed.

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Cooperatively interface role of surface atoms and aqueous media on single atom catalytic property for H2O2 synthesis

Cited by 12 publications

References 54 publications

NO Oxidation Using H₂O₂ at a Single-Atom Iron Catalyst

NO Oxidation Using H₂O₂ at a Single-Atom Iron Catalyst

Realizing a high OER activity in new single-atom catalysts formed by introducing TMN_x (x = 3 and 4) units into carbon nanotubes using high-throughput calculations

A Review of In-Situ Techniques for Probing Active Sites and Mechanisms of Electrocatalytic Oxygen Reduction Reactions

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Cooperatively interface role of surface atoms and aqueous media on single atom catalytic property for H2O2 synthesis

Cited by 12 publications

References 54 publications

NO Oxidation Using H2O2 at a Single-Atom Iron Catalyst

NO Oxidation Using H2O2 at a Single-Atom Iron Catalyst

Realizing a high OER activity in new single-atom catalysts formed by introducing TMNx (x = 3 and 4) units into carbon nanotubes using high-throughput calculations

A Review of In-Situ Techniques for Probing Active Sites and Mechanisms of Electrocatalytic Oxygen Reduction Reactions

Contact Info

Product

Resources

About

NO Oxidation Using H₂O₂ at a Single-Atom Iron Catalyst

NO Oxidation Using H₂O₂ at a Single-Atom Iron Catalyst

Realizing a high OER activity in new single-atom catalysts formed by introducing TMN_x (x = 3 and 4) units into carbon nanotubes using high-throughput calculations