Hydrogen evolution from water molecule reactions with Ge7 and Ge6Al clusters

Lei, Jia-Le; Shi, Shunping; Guo, Wei; Wan, Mingjie; Yan, Min; Liu, Yiliang; Li, Xia

doi:10.1016/j.ijhydene.2021.01.092

Cited by 12 publications

(11 citation statements)

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“…Germanium (Ge) has been widely used in electrocatalysis as a semiconductor metal. [72][73][74] The broadening of the antibonding (1 π*) orbitals confirmed the strong hybridization of N 2 with GeSe, as shown by DOS calculations. This means that GeSe Small 2023, 19, 2206776 Li, l) DOS plot of dinitrogen adsorbed Al 12 Li @graphene complex, m) CDD plot of dinitrogen adsorbed Al 12 Li @graphene complex.…”

Section: P-block Carbon Group Metal-based Catalystssupporting

confidence: 65%

“…Germanium (Ge) has been widely used in electrocatalysis as a semiconductor metal. [ 72–74 ] The broadening of the antibonding (1 π*) orbitals confirmed the strong hybridization of N 2 with GeSe, as shown by DOS calculations. This means that GeSe provides a strong capability to absorb and activate N 2 by coupling antibonding orbitals.…”

Section: The P‐block Metal‐based Electrocatalysts For Electrochemical...supporting

confidence: 55%

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P‐Block Metal‐Based Electrocatalysts for Nitrogen Reduction to Ammonia: A Minireview

Wang

et al. 2023

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limited total amount and the advancement of mining technology have triggered a booming decline of fossil fuel reserves, resulting in a severe energy depletion crisis. [2][3][4] NH 3 is an essential primary raw material for synthesizing chemicals and fertilizers in the chemical industry. [5,6] Currently, NH 3 production relies on the traditional Haber-Bosch process. [7,8] However, the reaction conditions are very harsh, which entail thermocatalytic conversion of N 2 and H 2 (N 2 + 3H 2 → 2NH 3 , ΔG = −16.48 kJ mol −1 ) under high temperature (≈300-600 °C) and intense pressure (≈15-40 MPa). [9,10] Moreover, the Haber-Bosch process requires complex and extensive production equipment. Recently, the electrochemical nitrogen reduction reaction (NRR) to NH 3 has received tremendous attention due to its merits of energy saving and environmental friendliness, aiming to achieve clean and sustainable production of NH 3 using renewable energy. [11][12][13] Unfortunately, electrochemical NRR is seriously limited by the lack of effective catalysts that can both greatly activate N 2 and suppress the hydrogen evolution reaction (HER). Currently, strategies to solve these problems mainly focus on the design of catalysts to achieve effective activation of N 2 and inhibit the occurrence of HER side reaction. [14,15] Maingroup elements play an essential role in NRR due to various electronic structures. That N 2 molecule can be effectively activated through Lewis acid-based interaction, p electron reverse contribution, heteroatomic doping, and defect engineering. [16] In addition, intrinsically poor proton binding, hydrophobic electrode surface engineering, and alkali metal cation effect can effectively inhibit HER. [17] However, the main-group elements have poor NRR activity. Because of the empty d-orbitals for electron donation and back-donation for N 2 capture and activation, transition metal-based catalysts have been extensively studied for NRR. But the d-orbitals of transition metal-based catalysts and H-s orbital coupling resulted in fierce HER-competition on the catalytic surface, which would not only hindered the active sites of N 2 adsorption but also significantly reduced the Faradaic efficiency (FEs) of the catalyst. [18] Noble metal catalysts have high NH 3 yield and FEs, [19][20][21] but their high price limit applications. In contrast, metal-free electrocatalysts have been explored by more researchers. [22][23][24] Porous metal-free Electrochemical nitrogen reduction reaction (NRR) to ammonia (NH 3 ) using renewable electricity provides a promising approach towards carbon neutral. What's more, it has been regarded as the most promising alternative to the traditional Haber-Bosch route in current context of developing sustainable technologies. The development of a class of highly efficient electrocatalysts with high selectivity and stability is the key to electrochemical NRR. Among them, P-block metal-based electrocatalysts have significant application potential in NRR for which possessing a strong interaction with the N ...

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Section: P-block Carbon Group Metal-based Catalystssupporting

confidence: 65%

Section: The P‐block Metal‐based Electrocatalysts For Electrochemical...supporting

confidence: 55%

P‐Block Metal‐Based Electrocatalysts for Nitrogen Reduction to Ammonia: A Minireview

Wang

et al. 2023

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“…[84] Lei et al studied the energy barrier of Ge 6 M (M = Ge, Al) clusters towards HER and found the dopant Al atom can improve the reactivity of Ge 7 cluster with H 2 O. [85]…”

Section: Heteroatomic Dopingmentioning

confidence: 99%

Advances in the Electrocatalytic Hydrogen Evolution Reaction by Metal Nanoclusters‐based Materials

Ding

Yang

Zhang

et al. 2022

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With the development of renewable energy systems, clean hydrogen is burgeoning as an optimal alternative to fossil fuels, in which its application is promising to retarding the global energy and environmental crisis. The hydrogen evolution reaction (HER), capable of producing high‐purity hydrogen rapidly in electrocatalytic water splitting, has received much attention. Abundant research about HER has been done, focusing on advanced electrocatalyst design with high efficiency and robust stability. As potential HER catalysts, metal nanoclusters (MNCs) have been studied extensively. They are composed of several to a hundred metal atoms, with sizes being comparable to the Fermi wavelength of electrons, that is, < 2.0 nm. Different from metal atoms/nanoparticles, they exhibit unique catalytic properties due to their quantum size effect and low‐coordination environment. In this review, the activity‐enhancing approaches of MNCs applied in HER electrocatalysis are mainly summarized. Furthermore, recent progress in MNCs classified with different stabilization strategies, that is, the freestanding MNCs, MNCs with organic, metal and carbon supports, are introduced. Finally, the current challenges and deficiencies of these MNCs for HER are prospected.

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“…The reaction path of In The reaction mechanism of In 7 + H 2 O reveals that the rate-determining step is the A 1 →B 1 elementary reaction, with an electronic energy barrier of 1.597 eV. The hydrogen evolution reaction of Ge 7 cluster involves a slowest step with an electronic energy barrier of 3.174 eV [14], while in the case of Pt 4 gasphase clusters, the corresponding free-energy barrier is around 2.7 eV [40]. This observation indicates that the surface active sites of In 7 clusters are more potent than those of Ge 7 and Pt 4 clusters.…”

Section: Resultsmentioning

confidence: 99%

DFT Study of Hydrogen Evolution Reactions of Water Molecule with In7 and In6Al Clusters

Liu

Liú

Shi

et al. 2023

Preprint

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The specific process of hydrogen generation by the reaction of In7 and In6Al clusters with H2O molecules is explored through density functional theory in this study. Based on the prediction of the lowest energy structure of In7 and In6Al clusters, the geometric and electronic structures of In7@H2O and In6Al@H2O are obtained by using the dispersion-corrected density functional theory B3LYP-D3. The corresponding reaction paths are constructed according to the transition states in the searched reactions. Then we discuss the reaction path, energy barrier and reaction energy release. The results show that both In7 and In6Al clusters can react with H2O molecules and release hydrogen. Both reactions are exothermic reactions, and the structure of the reaction product are very similar. The comparison of adsorption energy, energy barrier and reaction release energy show that the Al-doped In7 cluster can significantly improve its ability to react with H2O and reduce the energy barrier that has to be overcome for the reaction process. The generated H2 exists on the cluster surface in the form of physical adsorption, which is judged by the adsorption energy, the distance between the H2 molecule and the cluster surface, and the interaction region indicator.

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Hydrogen evolution from water molecule reactions with Ge7 and Ge6Al clusters

Cited by 12 publications

References 50 publications

P‐Block Metal‐Based Electrocatalysts for Nitrogen Reduction to Ammonia: A Minireview

P‐Block Metal‐Based Electrocatalysts for Nitrogen Reduction to Ammonia: A Minireview

Advances in the Electrocatalytic Hydrogen Evolution Reaction by Metal Nanoclusters‐based Materials

DFT Study of Hydrogen Evolution Reactions of Water Molecule with In7 and In6Al Clusters

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