Modulating Built‐In Electric Field via Variable Oxygen Affinity for Robust Hydrogen Evolution Reaction in Neutral Media

Zhai, Lingling; She, Xiaojie; Zhuang, Lyuchao; Li, Yanyong; Ding, Ran; Guo, Xuyun; Zhang, Yongqi; Zhu, Ye; Xu, Ke; Fan, Hong Jin; Lau, Shu Ping

doi:10.1002/anie.202116057

Cited by 211 publications

(130 citation statements)

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“…The difference of semiconductor work function (W) or Fermi energy level (E f ) is the internal driving force of charge transfer of heterojunction catalysts. 61 The Fermi levels of Mo-MOFs were also determined by UPS results (Figure S12). The dashed red lines mark the baseline and tangents of the curve in Figure S12.…”

Section: ■ Results and Discussionmentioning

confidence: 99%

Energy Level Engineering: Ru Single Atom Anchored on Mo-MOF with a [Mo₈O₂₆(im)₂]^4– Structure Acts as a Biomimetic Photocatalyst

et al. 2022

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Section: ■ Results and Discussionmentioning

confidence: 99%

Energy Level Engineering: Ru Single Atom Anchored on Mo-MOF with a [Mo₈O₂₆(im)₂]^4– Structure Acts as a Biomimetic Photocatalyst

et al. 2022

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“…The addition of Mo may affect the charge redistribution of FeCoNiMo HEA/C and regulate the adsorption process of the OER intermediate . The zeta potentials of FeCoNiMo HEA/C in neutral and alkaline medias are a little bit higher than those of FeCoNi/C (Figure S17), suggesting the most negative charge on the FeCoNiMo HEA/C catalytic surface, which is of benefit to OH* to react with the catalyst.…”

Section: Resultsmentioning

confidence: 99%

High-Entropy Alloy with Mo-Coordination as Efficient Electrocatalyst for Oxygen Evolution Reaction

et al. 2022

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Electrochemical hydrolytic hydrogen production is the most promising method for renewable energy storage and conversion. However, the kinetic slow oxygen evolution reaction (OER) limits the development of water electrolysis at the anode. The state-of-the-art OER catalysts face a dilemma of high content of noble metals and low OER activities. Herein, a strategy for achieving efficient and stable high-entropy alloy (HEA) catalysts by Mo-coordination is reported. The earth-abundant FeCoNiMo HEA catalyst provides an overpotential as low as 250 mV at the current density of 10 mA cm −2 in alkaline medium, which is 89 mV lower than that of state-of-the-art IrO 2 . The turnover frequency of 0.051 s −1 at the overpotential of 300 mV of FeCoNiMo HEA is 3 times higher than that of commercial IrO 2 catalyst and even 11 times higher than that of the FeCoNi alloy without Mo-coordination. Importantly, the FeCoNiMo HEA exhibits high OER stability at a high current density of 100 mA cm −2 . Methanol molecular probe experiment and X-ray photoelectron spectroscopy analyses suggest that the electrons of Mo transfer to Fe, Co, and Ni in the FeCoNiMo HEA catalyst, which leads to a weakened OH* bonding and, as a result, enhanced OER performance of the FeCoNiMo HEA catalyst. Consistent with the methanol molecular probe analysis, the real-time OER kinetic simulation reveals that the coordination of Mo within FeCoNi can speed up the rate-determining OH* deprotonation step of OER. Our finding opens up a routine for designing efficient cost-effective electrocatalysts for OER, which could facilitate discoveries in OER catalysts.

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“…[54][55][56][57] In addition, Pt/Pd hetero-metallene has a large number of Pt/Pd heterointerfaces, and the built-in electric field constructed spontaneously at the interface can adjust the electronic structure of Pt and Pd atoms, thereby enhancing the adsorption and activation of reactant molecules. 58,59…”

Section: Resultsmentioning

confidence: 99%

Interface Engineering-Inspired Electron Regulation in Pt/Pd Hetero-Metallene for Methanol-Assisted Hydrogen Evolution

Wang¹

2022

Enlab

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The small molecule oxidation reaction instead of oxygen evolution reaction coupled with hydrogen evolution reaction can greatly reduce the reaction overpotential of electrochemical water splitting, which is a very efficient and energy-saving hydrogen evolution strategy. Herein, we report an interface engineering constructed two-dimensional ultrathin curled Pt/Pd hetero-metallene for efficient electrocatalytic hydrogen evolution assisted by methanol. The thin-sheet structure of Pt/Pd hetero-metallene provides a large specific surface area and exposes numerous surface atoms that could act as reactive sites, thus accelerating the reaction mass transfer process. More importantly, the constructed Pt/Pd hetero-metallene possesses abundant Pt/Pd heterointerface, which can maximize the strong metal-metal interaction and increase the utilization of metal atoms, thereby optimizing the adsorption and activation of reactants during the reaction. Pt/Pd hetero-metallene can produce hydrogen stably and efficiently in 1 M KOH + 1 M CH3OH, and the voltage only needs 0.83 V at @100 mA cm-2 when used in electrocatalytic hydrogen evolution, which is much lower than the voltage required for the traditional electrochemical water splitting process (1.94 V). This work not only provides a powerful approach to rational design and construction of hetero-metallene through interface engineering, but also builds a bridge between hetero-metallene and methanol-assisted hydrogen evolution.

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Modulating Built‐In Electric Field via Variable Oxygen Affinity for Robust Hydrogen Evolution Reaction in Neutral Media

Cited by 211 publications

References 56 publications

Energy Level Engineering: Ru Single Atom Anchored on Mo-MOF with a [Mo₈O₂₆(im)₂]^4– Structure Acts as a Biomimetic Photocatalyst

Energy Level Engineering: Ru Single Atom Anchored on Mo-MOF with a [Mo₈O₂₆(im)₂]^4– Structure Acts as a Biomimetic Photocatalyst

High-Entropy Alloy with Mo-Coordination as Efficient Electrocatalyst for Oxygen Evolution Reaction

Interface Engineering-Inspired Electron Regulation in Pt/Pd Hetero-Metallene for Methanol-Assisted Hydrogen Evolution

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Modulating Built‐In Electric Field via Variable Oxygen Affinity for Robust Hydrogen Evolution Reaction in Neutral Media

Cited by 211 publications

References 56 publications

Energy Level Engineering: Ru Single Atom Anchored on Mo-MOF with a [Mo8O26(im)2]4– Structure Acts as a Biomimetic Photocatalyst

Energy Level Engineering: Ru Single Atom Anchored on Mo-MOF with a [Mo8O26(im)2]4– Structure Acts as a Biomimetic Photocatalyst

High-Entropy Alloy with Mo-Coordination as Efficient Electrocatalyst for Oxygen Evolution Reaction

Interface Engineering-Inspired Electron Regulation in Pt/Pd Hetero-Metallene for Methanol-Assisted Hydrogen Evolution

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Energy Level Engineering: Ru Single Atom Anchored on Mo-MOF with a [Mo₈O₂₆(im)₂]^4– Structure Acts as a Biomimetic Photocatalyst

Energy Level Engineering: Ru Single Atom Anchored on Mo-MOF with a [Mo₈O₂₆(im)₂]^4– Structure Acts as a Biomimetic Photocatalyst