Phase Engineering of a Ruthenium Nanostructure toward High-Performance Bifunctional Hydrogen Catalysis

Li, Leigang; Liu, Cheng; Liu, Shangheng; Wang, Juan; Han, Jiajia; Chan, Ting‐Shan; Li, Youyong; Hu, Z.; Shao, Qi; Zhang, Qiaobao; Huang, Xiaoqing

doi:10.1021/acsnano.2c05776

Cited by 58 publications

(54 citation statements)

References 49 publications

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“…More recently, they have directly proved that phase engineering plays a crucial role in determining the electro-catalytic performance of Ru-based catalyst by synthesizing the MoO x À Ru both the face-centered-cubic (fcc) structure and hexagonal-close-packed (hcp) structure (Figure 6a-e). [86] According to the electrochemical measurements, it is disclosed that the MoO x À Ru fcc is highly superior to MoO x À Ru hcp in catalyzing HER with remarkably higher activity and durabil- ity. DFT calculations revealed that the modification effect of MoO x gave rise to optimal adsorption H and OH especially on fcc Ru (Figure 6f-i), which thus accounted for the superior electrocatalytic performance.…”

Section: Phase Engineeringmentioning

confidence: 99%

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Strategies for Promoting Catalytic Performance of Ru‐Based Electrocatalysts towards Oxygen/Hydrogen Evolution Reaction

Chu

Wang

et al. 2023

The Chemical Record

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Ru‐based materials hold great promise for substituting Pt as potential electrocatalysts toward water electrolysis. Significant progress is made in the fabrication of advanced Ru‐based electrocatalysts, but an in‐depth understanding of the engineering methods and induced effects is still in their early stage. Herein, we organize a review that focusing on the engineering strategies toward the substantial improvement in electrocatalytic OER and HER performance of Ru‐based catalysts, including geometric structure, interface, phase, electronic structure, size, and multicomponent engineering. Subsequently, the induced enhancement in catalytic performance by these engineering strategies are also elucidated. Furthermore, some representative Ru‐based electrocatalysts for the electrocatalytic HER and OER applications are also well presented. Finally, the challenges and prospects are also elaborated for the future synthesis of more effective Ru‐based catalysts and boost their future application.

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Section: Phase Engineeringmentioning

confidence: 99%

“…Reproduced from ref. [86], Copyright (2022), with the permission from American Chemical Society. f).…”

Section: Coupling Ru With Other Active Species For Synergistically Pr...mentioning

confidence: 99%

Strategies for Promoting Catalytic Performance of Ru‐Based Electrocatalysts towards Oxygen/Hydrogen Evolution Reaction

Chu

Wang

et al. 2023

The Chemical Record

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“…Meanwhile, Ga-Ru/C (Figure 1b,d) also processes a typical hcp structure with lattice spacings of 0.140 and 0.209 nm, corresponding to the (110) and (101) planes, which is also basically along low-index zone axis [−111]. Compared with Ru/C (Figure S4), 22 the crystal plane spacings of Sn-Ru/C and Ga-Ru/C display certain increases, further verifying the successful doping of Sn atoms and Ga atoms into the Ru lattices. Furthermore, the HAADF-STEM image and corresponding energy-dispersive X-ray spectrometry (EDX) mappings of Sn-Ru/C show that Ru is uniformly distributed and Sn also exists in the nanoparticles Moreover, as shown in Figure S6, Ga in Ga-Ru/C is also in the form of metallic Ga (1117.20 eV) and partial oxidation states.…”

Section: ■ Results and Discussionmentioning

confidence: 99%

Boosting Hydrogen Oxidation Kinetics by Promoting Interfacial Water Adsorption on d-p Hybridized Ru Catalysts

Liang

et al. 2023

ACS Catal.

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The search for highly efficient and cost-effective electrocatalysts for hydrogen oxidation reaction (HOR) under alkaline electrolytes is essential for the commercial application of anion exchange membrane fuel cells. However, the kinetics of HOR in an alkaline media is much slower than that in an acidic electrolyte, which usually results in orders of magnitude decrease in the catalytic performance. Herein, we report the synthesis of d-p orbital hybridized Ru catalysts through Sn/Ga doping. Density functional theory (DFT) calculations and experimental results including H 2 -temperature programmed desorption (H 2 -TPD) and in situ Raman spectra unveil that the electronic structure modification of Ru derived from the unconventional d-p hybridization could lead to the promoted interfacial water adsorption ability and optimized hydrogen adsorption free energy during the alkaline HOR process. As expected, the d-p hybridized Ru catalyst shows much decreased formation energy of water, which contributes to the changed potential-determining step (PDS) and remarkable HOR activity with the mass activity up to 1790 mA mg Ru −1 . This work not only illustrates the key role of interfacial water adsorption ability but also provides a strategy for rationally designing advanced electrocatalysts for alkaline HOR.

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“…6) revealed that the ratio of Rh/Mo was 84:16, in accordance with the inductively coupled plasma atomic emission spectroscopy (ICP-AES) result (85:15). The oxidation state of Rh in RhMo NSs was studied by X-ray absorption near-edge spectra (XANES) at the Rh-K edge, which was highly sensitive to the valence state of the 4d element since the absorption edge shifted by more than one eV when the valence state increased by one 28,29 . The energy position of RhMo NSs spectrum shifts by more than 4 eV to lower energy relative to Rh 3+ reference (Rh 2 O 3 ), but was located very close to that of Rh foil, indicating a basic metallic nature of Rh in RhMo NSs (Supplementary Fig.…”

Section: Morphological and Structural Characterizationsmentioning

confidence: 99%

Atomic-thick metastable phase RhMo nanosheets for hydrogen oxidation catalysis

Zhang

Liu

et al. 2023

Nat Commun

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Metastable phase two-dimensional catalysts provide great flexibility for modifying their chemical, physical, and electronic properties. However, the synthesis of ultrathin metastable phase two-dimensional metallic nanomaterials is highly challenging, mainly due to the anisotropic nature of metallic materials and their thermodynamically unstable ground-state. Here, we report free-standing RhMo nanosheets with atomic thickness and a unique core/shell (metastable phase/stable phase) structure. The polymorphic interface between the core region and shell region stabilizes and activates metastable phase catalysts; the RhMo Nanosheets/C shows excellent hydrogen oxidation activity and stability. Specifically, the mass activities of RhMo Nanosheets/C is 6.96 A mgRh−1; this is 21.09 times higher than that of commercial Pt/C (0.33 A mgPt−1). Density functional theory calculations suggest that the interface aids in the dissociation of H2 and the H species can then spillover to weak H binding sites for desorption, providing excellent hydrogen oxidation activity for RhMo nanosheets. This work advances the highly controlled synthesis of two-dimensional metastable phase noble metals and provides great directions for the design of high-performance catalysts for fuel cells and beyond.

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Phase Engineering of a Ruthenium Nanostructure toward High-Performance Bifunctional Hydrogen Catalysis

Cited by 58 publications

References 49 publications

Strategies for Promoting Catalytic Performance of Ru‐Based Electrocatalysts towards Oxygen/Hydrogen Evolution Reaction

Strategies for Promoting Catalytic Performance of Ru‐Based Electrocatalysts towards Oxygen/Hydrogen Evolution Reaction

Boosting Hydrogen Oxidation Kinetics by Promoting Interfacial Water Adsorption on d-p Hybridized Ru Catalysts

Atomic-thick metastable phase RhMo nanosheets for hydrogen oxidation catalysis

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