Engineering active sites on hierarchical transition bimetal oxides/sulfides heterostructure array enabling robust overall water splitting

Zhai, Panlong; Zhang, Yanxue; Wu, Yunzhen; Gao, Junfeng; Zhang, Bo; Cao, Shuyan; Zhang, Yanting; Li, Zhuwei; Sun, Licheng; Hou, Jungang

doi:10.1038/s41467-020-19214-w

Cited by 512 publications

(280 citation statements)

References 83 publications

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“…38), indicating its high intrinsic catalytic activity towards the HER. 44,45 The volcano map drawn based on the exchange current density (j 0 ) and ΔG H* is shown in Fig. 5f and the trend basically in line with DFT prediction (Fig.…”

Section: Electrochemical Properties and Catalytic Activitysupporting

confidence: 65%

Comprehensive Evaluation of Transition Metal Doped Ni3N to Construct High-Efficiency Hydrogen Evolution Catalyst

Wang

et al. 2021

Preprint

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Density functional theory (DFT) calculation indicators (ΔG, densities of state, D-band and bader charge) are commonly used to predict and analyze the hydrogen evolution reaction (HER) activity of catalysts, and most studies discuss only one or few of these indicators’ impact on catalysis, but still no report has comprehensively evaluated the influence of all these indicators on catalytic performance. Herein, foreseen by comprehensive consideration first, we report transition metal doped Ni3N nanosheets combined on Ni foam for utra-efficient alkaline hydrogen evolution. For dual transition metals doped Ni3N, Co,V-Ni3N exhibits remarkable HER performance with a significantly low overpotential of only 10 mV in alkaline electrolyte and 41 mV in alkaline seawater electrolyte at 10 mA cm− 2; while for single transition metal doped Ni3N, V-Ni3N exhibits the best performance with an overpotential of 15 mV and a Tafel slope of 37 mV dec− 1. Our work highlights the importance of comprehensive evaluation of DFT calculation indexes, and opens up a new method for the rational design of efficient and low-cost catalysts.

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Section: Electrochemical Properties and Catalytic Activitysupporting

confidence: 65%

Comprehensive Evaluation of Transition Metal Doped Ni3N to Construct High-Efficiency Hydrogen Evolution Catalyst

Wang

et al. 2021

Preprint

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“…Hydrous NiMoO 4 possesses an overpotential of 220 mV at a current density of 10 mA cm −2 . The OER activity of NiMoO 4 @Co 3 O 4 is promising and exceeds the activity of the most efficient catalysts recently published (Ni-Fe oxy hydroxide@NiFe, [23] Ni-Fe oxyhydroxide, [24] NiMoOx/ NiMoS [25] in terms of onset potential, and overpotential needed to produce a current density of 10 mA cm −2 .…”

Section: Electrochemical Characterizationsmentioning

confidence: 83%

NiMoO₄@Co₃O₄ Core–Shell Nanorods: In Situ Catalyst Reconstruction toward High Efficiency Oxygen Evolution Reaction

Solomon

Landström

Mazzaro

et al. 2021

Advanced Energy Materials

142

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The sluggish kinetics of the oxygen evolution reaction (OER) is the bottleneck for the practical exploitation of water splitting. Here, the potential of a core–shell structure of hydrous NiMoO4 microrods conformally covered by Co3O4 nanoparticles via atomic layer depositions is demonstrated. In situ Raman and synchrotron‐based photoemission spectroscopy analysis confirms the leaching out of Mo facilitates the catalyst reconstruction, and it is one of the centers of active sites responsible for higher catalytic activity. Post OER characterization indicates that the leaching of Mo from the crystal structure, induces the surface of the catalyst to become porous and rougher, hence facilitating the penetration of the electrolyte. The presence of Co3O4 improves the onset potential of the hydrated catalyst due to its higher conductivity, confirmed by the shift in the Fermi level of the heterostructure. In particular NiMoO4@Co3O4 shows a record low overpotential of 120 mV at a current density of 10 mA cm−2, sustaining a remarkable performance operating at a constant current density of 10, 50, and 100 mA cm−2 with negligible decay. Presented outcomes can significantly contribute to the practical use of the water‐splitting process, by offering a clear and in‐depth understanding of the preparation of a robust and efficient catalyst for water‐splitting.

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“…5d and Table 2). It demonstrated the formation of W-NiS0.5Se0.5 nanosheets/NiS0.5Se0.5 nanorods heterostructures, which will improve its electrocatalytic HER/OER performance [36][37][38] . Particularly, our strategy can also be popularized to synthesize other W single-atom modified TMCs, such as NiS and NiSe (Supplementary Fig.…”

Section: And 17mentioning

confidence: 99%

“…The ∆G* of W-NiS0.5Se0.5 and NiS0.5Se0.5 for OER is illustrated in Supplementary Fig. 36 Volcano plots of j0 measured in alkaline solution as a function of the ΔGH* for pure metals 55,56 (black circles) and the state-of-the-art Pt/C (green diamond), as well as the W-NiS0.5Se0.5 (red star). The dashed lines are used to guide the eye.…”

Section: First-principles Calculationsmentioning

confidence: 99%

Single-Atom Tungsten Doped Nis0.5Se0.5 Nanosheets@Nanorods Heterostructures Catalyze Water Splitting Highly Active and Durable

Wang

Zhang

et al. 2021

Preprint

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Developing robust nonprecious electrocatalysts towards hydrogen/oxygen evolution reaction (HER/OER) is crucial for the spread of hydrogen energy industrialization. Here, we prepared a highly active and durable electrocatalyst of W single-atoms doped NiS0.5Se0.5 nanosheets@NiS0.5Se0.5 nanorods heterostructure (W-NiS0.5Se0.5). The W-NiS0.5Se0.5 exhibits superior catalytic activity for HER and OER with an ultralow overpotential (39, 106 mV for HER and 171, 239 mV for OER) and excellent long-term durability (500 h) at 10 and 100 mA cm− 2, outperforming commercial precious-metal catalysts and many other reported transition-metal-based compounds. The spin state of Ni was delocalized by introducing low spin-state of W single-atom, thus increasing the electron density of Ni 2p orbital, optimizing the adsorption/desorption process of H, significantly reducing the energy barrier of the rate-determining step (O* → OOH*), finally accelerating thermodynamics and kinetics of HER/OER. This work provides a rational feasible strategy to design single-atom catalysts for water splitting and develop advanced transition metal-based electrocatalysts via regulating delocalized spin states.

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Engineering active sites on hierarchical transition bimetal oxides/sulfides heterostructure array enabling robust overall water splitting

Cited by 512 publications

References 83 publications

Comprehensive Evaluation of Transition Metal Doped Ni3N to Construct High-Efficiency Hydrogen Evolution Catalyst

Comprehensive Evaluation of Transition Metal Doped Ni3N to Construct High-Efficiency Hydrogen Evolution Catalyst

NiMoO₄@Co₃O₄ Core–Shell Nanorods: In Situ Catalyst Reconstruction toward High Efficiency Oxygen Evolution Reaction

Single-Atom Tungsten Doped Nis0.5Se0.5 Nanosheets@Nanorods Heterostructures Catalyze Water Splitting Highly Active and Durable

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Engineering active sites on hierarchical transition bimetal oxides/sulfides heterostructure array enabling robust overall water splitting

Cited by 512 publications

References 83 publications

Comprehensive Evaluation of Transition Metal Doped Ni3N to Construct High-Efficiency Hydrogen Evolution Catalyst

Comprehensive Evaluation of Transition Metal Doped Ni3N to Construct High-Efficiency Hydrogen Evolution Catalyst

NiMoO4@Co3O4 Core–Shell Nanorods: In Situ Catalyst Reconstruction toward High Efficiency Oxygen Evolution Reaction

Single-Atom Tungsten Doped Nis0.5Se0.5 Nanosheets@Nanorods Heterostructures Catalyze Water Splitting Highly Active and Durable

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NiMoO₄@Co₃O₄ Core–Shell Nanorods: In Situ Catalyst Reconstruction toward High Efficiency Oxygen Evolution Reaction