Neighboring Cationic Vacancy Assisted Adsorption Optimization on Single-Atom Sites for Improved Oxygen Evolution

Wang, Dongdi; Xue, Jiawei; Ding, Xilan; Wei, Jie; Chen, Feng; Wang, Ruyang; Ma, Peiyu; Wang, Sicong; Cao, Heng; Wang, Jingyan; Zuo, Ming J.; Zhou, Shiming; Zhang, Zhirong; Zeng, Jie; Bao, Jun

doi:10.1021/acscatal.2c03476

Cited by 20 publications

(5 citation statements)

References 58 publications

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“…Furthermore, the selected rectangular regions show the change in the line intensity profile, where atomic positions with significantly reduced intensity indicates the presence of Ni v (Figure 1h). [ 17,18 ] The nanosheets are successfully exfoliated from ≈25 nm to ≈5 nm (Figure 1i,j), as further confirmed by atomic force microscopy (AFM). [ 19 ] The generation of Ni NPs is also verified by the Ni 2p X‐ray photoelectron spectroscopy (XPS) spectra with the appearance of Ni(0) (Figure 1k).…”

Section: Resultsmentioning

confidence: 73%

“One Stone Five Birds” Plasma Activation Strategy Synergistic with Ru Single Atoms Doping Boosting the Hydrogen Evolution Performance of Metal Hydroxide

Yan

Yang

Lin

et al. 2023

Adv Funct Materials

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Layered metal hydroxides (LMHs) are promising catalysts for oxygen evolution reaction. However, the hydrogen evolution reaction (HER) activity of LMHs is unsatisfactory due to their poor conductivity and limited active sites. Herein, taking Ni(OH)2 as demonstration, a novel “one stone five birds” plasma activation strategy synergistic with Ru single atoms (Ru SAs) doping is developed to boost the HER activity of Ni(OH)2 by constructing heterostructured β‐Ni(OH)2/Ni‐Ru SAs nanosheet arrays (NSAs). Benefiting from the structural/compositional features and optimized electronic state, the as‐obtained β‐Ni(OH)2/Ni‐Ru SAs NSAs exhibit splendid HER activity with a low overpotential of 16 mV at 10 mA cm−2 and a small Tafel slope of 21 mV dec−1 in alkaline solution. Excellent HER performance in alkaline seawater and neutral solutions are also demonstrated by the β‐Ni(OH)2/Ni‐Ru SAs NSAs. The plasma activation and Ru SAs doping play important roles in enhancing water adsorption and accelerating the kinetics of water dissociation. Density functional theory (DFT) calculations reveal that the introduction of Ru SAs in the system facilitates the generation of surface OH vacancies for providing more active sites as well as decreases the antibonding state density of the generated mid‐gap state for enhancing H adsorption strength toward the optimal range.

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Section: Resultsmentioning

confidence: 73%

“One Stone Five Birds” Plasma Activation Strategy Synergistic with Ru Single Atoms Doping Boosting the Hydrogen Evolution Performance of Metal Hydroxide

Yan

Yang

Lin

et al. 2023

Adv Funct Materials

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“…introduced a strategy of utilizing cationic vacancies in the support of SAC to enhance the OER performance. [ 177 ] The OER performance of the catalyst Ru 1 ‐V Co ‐Co(OH) 2 , which has neighboring Co 2+ vacancies on the Co(OH) 2 , was found to be superior compared to a catalyst without Co 2+ vacancies (Ru 1 ‐Co(OH) 2 ). The mass activity of Ru 1 ‐V Co ‐Co(OH) 2 is 4.7 times higher than that of Ru 1 ‐Co(OH) 2 .…”

Section: Energy Conversion Applicationsmentioning

confidence: 99%

Surface Engineered Single‐atom Systems for Energy Conversion

Yu,

Zhu,

Huang

2024

Advanced Materials

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Single‐atom catalysts (SACs) have been demonstrated to show exceptional reactivity and selectivity in catalytic reactions by effectively utilizing metal species, making them a favorable choice among the different active materials for energy conversion. However, SACs are still in the early stage of energy conversion, and problems like agglomeration and low energy conversion efficiency are hampering their practical applications. Substantial researches focus on support modifications, which are vital for SAC reactivity and stability due to the intimate relationship between metal atoms and support. In this review, a category of supports and a variety of surface engineering strategies employed in SA systems are summarized, including surface site engineering (heteroatom doping, vacancy introducing, surface groups grafting, and coordination tunning) and surface structure engineering (size/morphology control, cocatalyst deposition, facet engineering, and crystallinity control). Also, the merits of support surface engineering in single‐atom systems are systematically introduced. Highlights are the comprehensive summary and discussions on the utilization of surface engineered SACs in diversified energy conversion applications including photocatalysis, electrocatalysis, thermocatalysis, and energy conversion devices. At the end of this review, we have discussed the potential and obstacles of using surface engineered SACs in the field of energy conversion. This review aims to guide the rational design and manipulation of SACs for target‐specific applications by capitalizing on the characteristic benefits of support surface engineering.This article is protected by copyright. All rights reserved

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“…The adjustment of the coordination environment can not only change the kind of coordination atoms but also change the vacancies around the metal center. Bao and coauthors reported that a Ru single-atom catalyst with neighboring Co 2+ vacancies based on Co(OH) 2 shows 4.73 times activity in OER performance compared to that of a catalyst without Co 2+ vacancies . The result of DFT calculations manifested that with Co 2+ vacancies *OOH intermediates can form a hydrogen bond with the neighboring O atom, which tunes the absorption configuration of *OOH and lowers the energy barrier of OER.…”

Section: Intrinsic Activity Of Single Sitementioning

confidence: 99%

Challenges and Perspectives of Single-Atom-Based Catalysts for Electrochemical Reactions

Chen

et al. 2023

JACS Au

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Single-atom catalysts (SACs) are emerging as the most promising catalysts for various electrochemical reactions. The isolated dispersion of metal atoms enables high density of active sites, and the simplified structure makes them ideal model systems to study the structure–performance relationships. However, the activity of SACs is still insufficient, and the stability of SACs is usually inferior but has received little attention, hindering their practical applications in real devices. Moreover, the catalytic mechanism on a single metal site is unclear, leading the development of SACs to rely on trial-and-error experiments. How can one break the current bottleneck of active sites density? How can one further increase the activity/stability of metal sites? In this Perspective, we discuss the underlying reasons for the current challenges and identify precisely controlled synthesis involving designed precursors and innovative heat-treatment techniques as the key for the development of high-performance SACs. In addition, advanced operando characterizations and theoretical simulations are essential for uncovering the true structure and electrocatalytic mechanism of an active site. Finally, future directions that may arise breakthroughs are discussed.

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Neighboring Cationic Vacancy Assisted Adsorption Optimization on Single-Atom Sites for Improved Oxygen Evolution

Cited by 20 publications

References 58 publications

“One Stone Five Birds” Plasma Activation Strategy Synergistic with Ru Single Atoms Doping Boosting the Hydrogen Evolution Performance of Metal Hydroxide

“One Stone Five Birds” Plasma Activation Strategy Synergistic with Ru Single Atoms Doping Boosting the Hydrogen Evolution Performance of Metal Hydroxide

Surface Engineered Single‐atom Systems for Energy Conversion

Challenges and Perspectives of Single-Atom-Based Catalysts for Electrochemical Reactions

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