Probing the origin of group VB transition metal monocarbides for high-efficiency hydrogen evolution reaction: A DFT study

Wang, Yanwei; Tian, Wenjing; Wan, Jin; Fu, Weiwei; Zhang, Han; Li, Yuke; Wang, Yu

doi:10.1016/j.apsusc.2020.148312

Cited by 32 publications

(24 citation statements)

References 47 publications

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“…More importantly, when value is close to 0, the overall reaction rate for HER achieves a maximum and the Tafel mechanism plays a dominant role in the HER. 37,38 Thus, in order to understand the underlying mechanism of the HER on TM@NP, we further calculate the energy barrier of the above excellent HER SACs following the Tafel mechanism (two H atoms adsorbed on TM and the nearest N atom react to form H 2 ). We use five images, including initial and final positions, for CI-NEB calculations.…”

Section: Resultsmentioning

confidence: 99%

NP monolayer supported transition-metal single atoms for electrochemical water splitting: a theoretical study

Wang

Tian

Wan

et al. 2022

Phys. Chem. Chem. Phys.

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Section: Resultsmentioning

confidence: 99%

NP monolayer supported transition-metal single atoms for electrochemical water splitting: a theoretical study

Wang

Tian

Wan

et al. 2022

Phys. Chem. Chem. Phys.

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“…To investigate the electronic transfer in the OHadsorption step on pristine BCF (denoted as BCF-OH) and strained BCF-325 (denoted as BCF-325-OH), we calculated the electronic work function for our samples. Electronic work function represents the minimum thermodynamic work needed for an electron to escape from material lattice to a point outside material surface, 54 where the value of work function (Φ) can be calculated as the electrostatic potential difference between vacuum level and Fermi level. 54 It was reported that a lower work function is instrumental to enhance the electronic transport between catalyst and reactants in liquid.…”

Section: Figurementioning

confidence: 99%

A universal chemical-induced tensile strain tuning strategy to boost oxygen-evolving electrocatalysis on perovskite oxides

Guan

Zhong

et al. 2022

Applied Physics Reviews

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Exploring effective, facile, and universal tuning strategies to optimize material physicochemical properties and catalysis processes is critical for many sustainable energy systems, but still challenging. Herein, we succeed to introduce tensile strain into various perovskites via a facile thermochemical reduction method, which can greatly improve material performance for the bottleneck oxygen-evolving reaction in water electrolysis. As an ideal proof-of-concept, such a chemical-induced tensile strain turns hydrophobic Ba5Co4.17Fe0.83O14- δ perovskite into the hydrophilic one by modulating its solid–liquid tension, contributing to its beneficial adsorption of important hydroxyl reactants as evidenced by fast operando spectroscopy. Both surface-sensitive and bulk-sensitive absorption spectra show that this strategy introduces oxygen vacancies into the saturated face-sharing Co-O motifs of Ba5Co4.17Fe0.83O14- δ and transforms such local structures into the unsaturated edge-sharing units with positive charges and enlarged electrochemical active areas, creating a molecular-level hydroxyl pool. Theoretical computations reveal that this strategy well reduces the thermodynamic energy barrier for hydroxyl adsorption, lowers the electronic work function, and optimizes the charge/electrostatic potential distribution to facilitate the electron transport between active sites and hydroxyl reactants. Also, this strategy is reliable for other single, double, and Ruddlesden–Popper perovskites. We believe that this finding will enlighten rational material design and in-depth understanding for many potential applications.

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“…However, it is interesting that for the Co-10 nanorods about 2.5nm, the dband are all shifted to higher energy levels. In the pure Ni system (Figure S9b According to previous reports, many catalytic processes (such as HER) require an appropriate 𝜀 𝑑 value to maintain the interaction strength between the reaction substrate and the catalytic site at an appropriate level 44 . Based on our calculation results, we found that the d-band center of Co-Ni nanorods changes regularly during the growth process, so we also provide researchers with a method for rationally designing catalysts.…”

Section: D-band Center and Partial Densities Of States (Pdos)mentioning

confidence: 98%

“…In order to further explore the relationship between terminal σ-hole and chemical activity, the change in reactivity and catalytic activity caused by the growth process of geometric structure and charge transfer, we further studied the electronic structure of the system, plotted the density of states of different orbitals of Co-Ni nanoclusters/rods, and calculated the d-band center. The calculation formula for the d-band center is as follows 44 :…”

Section: D-band Center and Partial Densities Of States (Pdos)mentioning

confidence: 99%

Exceptional electrostatic phenomenon in ultrathin nanorods: the terminal σ‑hole

Guan

2021

Preprint

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An in-depth understanding of the physicochemical properties of nanorods during the initial growth process has a profound impact on the rational design of high-performance nanorods catalysts. Herein, we conducted a systematic DFT study on the transition metal Co, Ni and alloyed nanoclusters/rods systems to simulate an atomic process from the initial nanoclusters growth to nanorods/wires. We found that the highly active sites of nanorods depend on an interesting electrostatic phenomenon. The surface electrostatic potential analysis shows that all nanoclusters and nanorods structures have formed σ-hole. Unlike nanoclusters, the σ-hole only appears at terminal sites in nanorods, called terminal σ-hole. The elemental composition in nanorods has a certain influence on the maximal surface electrostatic potential (VS,max) i.e., terminal σ-hole. Interestingly, we found that the terminal σ-hole formed in nanorods is generally higher in magnitude than smaller nanoclusters. First-principle calculations show that terminal σ-hole is closely related to the physicochemical activities of nanorods. For example, the work function of the directions forming terminal σ-hole is smaller than other directions. More interestingly, we found that in almost all nanorods, compared with other atoms, the d-orbital of the atoms forming terminal σ‑hole shifts close to the Fermi level and exhibits a shallower d-band center, showing higher chemical activity. In short, it is the first time that we discovered terminal σ-hole in nanorods, explained the theoretical basis of terminal σ-hole in nanorod systems, and provided theoretical guidance for the rational design of high-performance nanorods catalysts.

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Probing the origin of group VB transition metal monocarbides for high-efficiency hydrogen evolution reaction: A DFT study

Cited by 32 publications

References 47 publications

NP monolayer supported transition-metal single atoms for electrochemical water splitting: a theoretical study

NP monolayer supported transition-metal single atoms for electrochemical water splitting: a theoretical study

A universal chemical-induced tensile strain tuning strategy to boost oxygen-evolving electrocatalysis on perovskite oxides

Exceptional electrostatic phenomenon in ultrathin nanorods: the terminal σ‑hole

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