Diffusion behavior of hydrogen in oxygen saturated and unsaturated plutonium dioxide: An ab initio molecular dynamics study

Tang, Jun; Qiu, Ruizhi; Chen, Jinfan; Ao, Bingyun

doi:10.1016/j.jallcom.2020.155113

Cited by 13 publications

(5 citation statements)

References 58 publications

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“…At this stage, however, it is not clear whether the second Cu–N bond breakage in the Cu-N 3 structure facilitates the adsorption and activation of oxygen molecules or the adsorption of oxygen on the Cu-N 3 structure triggers the cleavage of the second Cu–N bond. To address this question may rely on time-resolved spectroscopy as well as advanced MD methods. , …”

Section: Resultsmentioning

confidence: 99%

Dynamic Behavior of Single-Atom Catalysts in Electrocatalysis: Identification of Cu-N₃ as an Active Site for the Oxygen Reduction Reaction

et al. 2021

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Atomically dispersed M-N-C (M refers to transition metals) materials represent the most promising catalyst alternatives to the precious metal Pt for the electrochemical reduction of oxygen (ORR), yet the genuine active sites in M-N-C remain elusive. Here, we develop a two-step approach to fabricate Cu-N-C single-atom catalysts with a uniform and well-defined Cu 2+ -N 4 structure that exhibits comparable activity and superior durability in comparison to Pt/C. By combining operando X-ray absorption spectroscopy with theoretical calculations, we unambiguously identify the dynamic evolution of Cu-N 4 to Cu-N 3 and further to HO-Cu-N 2 under ORR working conditions, which concurrently occurs with reduction of Cu 2+ to Cu + and is driven by the applied potential. The increase in the Cu + /Cu 2+ ratio with the reduced potential indicates that the low-coordinated Cu + -N 3 is the real active site, which is further supported by DFT calculations showing the lower free energy in each elemental step of the ORR on Cu + -N 3 than on Cu 2+ -N 4 . These findings provide a new understanding of the dynamic electrochemistry on M-N-C catalysts and may guide the design of more efficient low-cost catalysts.

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Section: Resultsmentioning

confidence: 99%

Dynamic Behavior of Single-Atom Catalysts in Electrocatalysis: Identification of Cu-N₃ as an Active Site for the Oxygen Reduction Reaction

et al. 2021

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“…25 The AIMD simulations were performed using canonical ensemble (NVT) and Nosé-Hoover thermostat method at 300-500 K (from room temperature to FCs operating temperature and even higher) and lasted for 10-15 ps, in which the timestep is set as 1 fs by increasing the hydrogen mass to 2 atomic mass unit (H/D-exchange) to reduce the computational cost. [26][27][28][29][30]…”

Section: Methodsmentioning

confidence: 99%

Theoretically probing the possible degradation mechanisms of an FeNC catalyst during the oxygen reduction reaction

Chen

Peng

et al. 2021

Chem. Sci.

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“…The theoretical study can be very close to wet laboratory experiment data, or it can also be incompatible. As a consequence of using quantum mechanical methods in theoretical calculations, it is necessary to validate the theoretical approach by comparing experimental data [51]. For this purpose, we have tested the compatibility of the 6-311++G (d,p) method and basis set options with the studied system (Figure 1).…”

Section: Resultsmentioning

confidence: 99%

Quantum Chemical and Monte Carlo Simulation Studies on Inhibition Performance of Caffeine and Its Derivatives against Corrosion of Copper

et al. 2020

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Performance tests on caffeine’s corrosion inhibition properties and their derivatives against copper corrosion have been previously reported experimentally using gravimetric and electrochemical analyses. The test was able to measure the efficiency of their corrosion inhibition accurately. However, the caffeine and its derivatives’ structure patterns and coating mechanisms when interacting with metals during copper corrosion inhibition have not been explained in detail by experimental studies. In the present study, the theoretical density functional study (DFT), ab initio MP2, and Monte Carlo simulation approaches explain the problem. The geometrical and quantum chemical parameters of inhibitors were compared under normal and protonated conditions in the gas and aqueous environments. Theoretical studies can accurately determine the molecule’s geometrical parameters and successfully explain the quantum parameters of inhibitors. Molecular dynamics are applied to study the mechanism of interaction between inhibitors and metal surfaces in an explicit water molecule environment. The energy absorption of caffeine and its derivatives on metal surfaces was linear, with quantum parameters calculated from the density functional theory and an ab initio approach. Furthermore, these theoretical study results align with the previously reported experimental studies published by de Souza et al. The inhibition efficiency ranking of studied molecules preventing copper corrosion was caffeine > theobromine > theophylline. This theoretical approach is expected to bridge the gap in designing effective corrosion inhibitors.

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Diffusion behavior of hydrogen in oxygen saturated and unsaturated plutonium dioxide: An ab initio molecular dynamics study

Cited by 13 publications

References 58 publications

Dynamic Behavior of Single-Atom Catalysts in Electrocatalysis: Identification of Cu-N₃ as an Active Site for the Oxygen Reduction Reaction

Dynamic Behavior of Single-Atom Catalysts in Electrocatalysis: Identification of Cu-N₃ as an Active Site for the Oxygen Reduction Reaction

Theoretically probing the possible degradation mechanisms of an FeNC catalyst during the oxygen reduction reaction

Quantum Chemical and Monte Carlo Simulation Studies on Inhibition Performance of Caffeine and Its Derivatives against Corrosion of Copper

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Diffusion behavior of hydrogen in oxygen saturated and unsaturated plutonium dioxide: An ab initio molecular dynamics study

Cited by 13 publications

References 58 publications

Dynamic Behavior of Single-Atom Catalysts in Electrocatalysis: Identification of Cu-N3 as an Active Site for the Oxygen Reduction Reaction

Dynamic Behavior of Single-Atom Catalysts in Electrocatalysis: Identification of Cu-N3 as an Active Site for the Oxygen Reduction Reaction

Theoretically probing the possible degradation mechanisms of an FeNC catalyst during the oxygen reduction reaction

Quantum Chemical and Monte Carlo Simulation Studies on Inhibition Performance of Caffeine and Its Derivatives against Corrosion of Copper

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Product

Resources

About

Dynamic Behavior of Single-Atom Catalysts in Electrocatalysis: Identification of Cu-N₃ as an Active Site for the Oxygen Reduction Reaction

Dynamic Behavior of Single-Atom Catalysts in Electrocatalysis: Identification of Cu-N₃ as an Active Site for the Oxygen Reduction Reaction