Boosting the alkaline hydrogen evolution of Ru nanoclusters anchored on B/N–doped graphene by accelerating water dissociation

Ye, Shenghua; Luo, Feiyan; Xu, Tingting; Zhang, Pingyu; Shi, Hongdong; Qin, Shiqi; Wu, Jiaping; He, Chuanxin; Ouyang, Xiaoping; Zhang, Qianling; Liu, Jianhong; Sun, Xueliang

doi:10.1016/j.nanoen.2019.104301

Cited by 148 publications

(74 citation statements)

References 47 publications

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“…[1] Although the alkaline water splitting technique has been industrialized for decades,i tr emains highly energy-intensive,a nd thus more efficient electrocatalysts are needed to decrease energy losses and costs.T he hydrogen evolution reaction (HER) is one of the two halfreactions of electrochemical water splitting and occurs at the cathode. [2] According to activity volcano plots, [3] the HER rate is largely determined by the free energy of hydrogen adsorption. [4] To achieve optimal catalytic activity,the hydrogen binding energy on the catalyst surface must be neither too weak nor too strong, as Sabatiersp rinciple.…”

Section: Introductionmentioning

confidence: 99%

The Heterostructure of Ru₂P/WO₃/NPC Synergistically Promotes H₂O Dissociation for Improved Hydrogen Evolution

et al. 2020

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Facilitating the dissociation of water and desorption of hydrogen are both crucial challenges for improving the hydrogen evolution reaction (HER) in alkaline media. Herein, we report the synthesis of heterostructure of Ru2P/WO3@NPC (N, P co‐doped carbon) by a simple hydrothermal reaction using ruthenium and tungsten salts as precursors, followed by pyrolyzing under an Ar atmosphere. The Ru2P/WO3@NPC electrocatalyst exhibits an outstanding HER activity with an overpotential of 15 mV at a current density of 10 mA cm−2 and excellent durability in a 1.0 M KOH solution, outperforming state‐of‐the‐art Pt/C and most reported electrocatalysts. Experimental results combined with density functional calculations reveal that the electron density redistribution in Ru2P/WO3@NPC is achieved by electron transfer from NPC to Ru2P/WO3 and from Ru2P to WO3, which directly promotes the dissociation of water on W sites in WO3 and desorption of hydrogen on Ru sites in Ru2P.

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Section: Introductionmentioning

confidence: 99%

The Heterostructure of Ru₂P/WO₃/NPC Synergistically Promotes H₂O Dissociation for Improved Hydrogen Evolution

et al. 2020

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“…[7] For example, in the hybrids of carbon and metal, introducing heteroatoms (i.e., N, P, and B) or defects to carbon is convenient for improving the electrocatalytic performance including both activity and stability by enhancing the metalsupport interaction. [8] As such, confining the SNMC on the defective carbon may be a good strategy to enhance the metal-support interaction, thereby simultaneously boosting the activity and stability of sub-nanometric metal clusters (SNMC). However, the chemical confinement of carbon defects alone is often not enough for preventing aggregation of metals during high-temperature calcination, leading to the formation of nanoparticles other than SNMC.…”

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confidence: 99%

Facile Synthesis of Sub‐Nanometric Copper Clusters by Double Confinement Enables Selective Reduction of Carbon Dioxide to Methane

Han

et al. 2020

Angewandte Chemie

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Previous density-functional theory (DFT) calculations show that sub-nanometric Cu clusters (i.e., 13 atoms) favorably generate CH 4 from the CO 2 reduction reaction (CO 2 RR), but experimental evidence is lacking. Herein, a facile impregnation-calcination route towards Cu clusters, having a diameter of about 1.0 nm with about 10 atoms, was developed by double confinement of carbon defects and micropores. These Cu clusters enable high selectivity for the CO 2 RR with a maximum Faraday efficiency of 81.7 % for CH 4. Calculations and experimental results show that the Cu clusters enhance the adsorption of *H and *CO intermediates, thus promoting generation of CH 4 rather than H 2 and CO. The strong interactions between the Cu clusters and defective carbon optimize the electronic structure of the Cu clusters for selectivity and stability towards generation of CH 4. Provided here is the first experimental evidence that sub-nanometric Cu clusters facilitate the production of CH 4 from the CO 2 RR.

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“…The electron deficiency of Ru facilitates the nucleophilic attack from H 2 O, which induces HÀ OH bond cleavage to accelerate the water dissociation step during the HER. [25] Furthermore, the change of surface state of all catalysts was probed by FTIR in Figure 3d. In comparison to CNT, OCNT shows new peaks at 1700, 1405, and 1215 cm À 1 corresponding to the stretch vibrations of C=O, OÀ H, and CÀ O, respectively.…”

Section: Resultsmentioning

confidence: 99%

Hierarchical Architectures Based on Ru Nanoparticles/Oxygen‐Rich‐Carbon Nanotubes for Efficient Hydrogen Evolution

Ding

Lin

Pei

et al. 2021

Chemistry A European J

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Highly active and durable electrocatalysts are essential for producing hydrogen fuel through the hydrogen evolution reaction (HER). Here, a uniform deposition of Ru nanoparticles strongly interacting with oxygen-rich carbon nanotube architectures (Ru-OCNT) through ozonation and hydrothermal approaches has been designed. The hierarchical structure of Ru-OCNT is made by self-assembly of oxygen functionalities of OCNT. Ru nanoparticles interact strongly with OCNT at the Ru/OCNT interface to give excellent catalytic activity and stability of the Ru-OCNT, as further confirmed by density functional theory. Owing to the hierarchical structure and adjusted surface chemistry, Ru-OCNT has an overpotential of 34 mV at 10 mA cm À 2 with a Tafel slope of 27.8 mV dec À 1 in 1 M KOH, and an overpotential of 55 mV with Tafel slope of 33 mV dec À 1 in 0.5 M H 2 SO 4 . The smaller Tafel slope of Ru-OCNT than Ru-CNT and commercial Pt/C in both alkaline and acidic electrolytes indicates high catalytic activity and fast charge transfer kinetics. The asproposed chemistry provides the rational design of hierarchically structured CNT/nanoparticle electrocatalysts for HER to produce hydrogen fuel.

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Boosting the alkaline hydrogen evolution of Ru nanoclusters anchored on B/N–doped graphene by accelerating water dissociation

Cited by 148 publications

References 47 publications

The Heterostructure of Ru₂P/WO₃/NPC Synergistically Promotes H₂O Dissociation for Improved Hydrogen Evolution

The Heterostructure of Ru₂P/WO₃/NPC Synergistically Promotes H₂O Dissociation for Improved Hydrogen Evolution

Facile Synthesis of Sub‐Nanometric Copper Clusters by Double Confinement Enables Selective Reduction of Carbon Dioxide to Methane

Hierarchical Architectures Based on Ru Nanoparticles/Oxygen‐Rich‐Carbon Nanotubes for Efficient Hydrogen Evolution

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Boosting the alkaline hydrogen evolution of Ru nanoclusters anchored on B/N–doped graphene by accelerating water dissociation

Cited by 148 publications

References 47 publications

The Heterostructure of Ru2P/WO3/NPC Synergistically Promotes H2O Dissociation for Improved Hydrogen Evolution

The Heterostructure of Ru2P/WO3/NPC Synergistically Promotes H2O Dissociation for Improved Hydrogen Evolution

Facile Synthesis of Sub‐Nanometric Copper Clusters by Double Confinement Enables Selective Reduction of Carbon Dioxide to Methane

Hierarchical Architectures Based on Ru Nanoparticles/Oxygen‐Rich‐Carbon Nanotubes for Efficient Hydrogen Evolution

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The Heterostructure of Ru₂P/WO₃/NPC Synergistically Promotes H₂O Dissociation for Improved Hydrogen Evolution

The Heterostructure of Ru₂P/WO₃/NPC Synergistically Promotes H₂O Dissociation for Improved Hydrogen Evolution