Chemically activating MoS2 via spontaneous atomic palladium interfacial doping towards efficient hydrogen evolution

Luo, Zhaohui; Ouyang, Yixin; Zhang, Hao; Xiao, Meiling; Ge, Junjie; Jiang, Zheng; Wang, Jinlan; Tang, Dai‐Ming; Cao, Xingzhong; Liu, Changpeng; Wang, Xing

doi:10.1038/s41467-018-04501-4

Cited by 551 publications

(433 citation statements)

References 46 publications

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“…Another effective method for evaluating the intrinsic activities of a catalyst on a per‐site basis is the turnover frequency (TOF). Impressively, SA‐Ru‐MoS 2 exhibit a much higher TOF value than most previously reported catalysts in the literature at various overpotentials (see Table S4 for details, Supporting Information) …”

Section: Resultsmentioning

confidence: 74%

“…Figure a shows two apparent peaks at the positions of 228.47 and 231.63 eV, corresponding to 3d 5/2 and 3d 3/2 of Mo, respectively. Note that after partial peak fitting, Mo exhibits a mixed valence state consistent with pure MoS 2 , i.e., Mo 3+ (3d 3/2 at 231.5 eV and 3d 5/2 at 228.3 eV respectively) and Mo 4+ (3d 3/2 at 231.9 eV and 3d 5/2 at 228.7 eV respectively) . Combined with Energy dispersive spectrometer (EDS) quantitative analysis, the atomic ratio of Mo: S is about 1:1.64 (see Table S2, Supporting Information).…”

Section: Resultsmentioning

confidence: 99%

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Single‐Atom Ru Doping Induced Phase Transition of MoS₂ and S Vacancy for Hydrogen Evolution Reaction

et al. 2019

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Using electrochemical water splitting to produce hydrogen is still a grand challenge due to the lack of economical and efficient Pt‐free catalysts. Herein, a single‐atom Ru supported on MoS2 (SA‐Ru‐MoS2) electrocatalyst for the hydrogen evolution reaction (HER) is reported. Results indicate that single‐atom Ru doping induces phase transition of MoS2 and generation of S vacancies, which significantly improve the performance of inert 2D MoS2 for HER. In particular, the SA‐Ru‐MoS2 electrocatalyst exhibits a low overpotential of 76 mV at 10 mA cm−2 in alkaline media, which is superior to most electrocatalysts previously reported in the literature. Combining experimental results with density functional theory (DFT) calculations, it is further revealed that the origin of high HER activity is mainly attributed to the synergy effects of single‐atom Ru doping and S vacancies and phase transition of local structure of MoS2, which efficiently tailors the electronic structure of SA‐Ru‐MoS2 and extremely reduces the energy barrier of the Volmer step and the adsorption/desorption of H* intermediate step. In short, this work provides a single‐atom doping strategy to transfer the inert MoS2 into the highly efficient electrocatalysts.

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Section: Resultsmentioning

confidence: 74%

Section: Resultsmentioning

confidence: 99%

Single‐Atom Ru Doping Induced Phase Transition of MoS₂ and S Vacancy for Hydrogen Evolution Reaction

et al. 2019

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“…It suggests a reduction in the unoccupied Mo 4d state due to the charge transfer. In addition, according to the Mo K ‐edge XAFS spectrum, the P‐MoSe 2 /N‐MSC presents smaller energy of absorption edge ( Figure a and Figure S7a, Supporting Information), implying higher average electron density than that of MoSe 2 /N‐MSC sample, where Mo foil is used as the reference . The oscillation curves of Mo K ‐edge in the k range of 0–14.0 Å −1 are shown in Figure b.…”

Section: Resultsmentioning

confidence: 98%

Coupled Biphase (1T‐2H)‐MoSe₂ on Mold Spore Carbon for Advanced Hydrogen Evolution Reaction

Deng

Luo

et al. 2019

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Performance breakthrough of MoSe2‐based hydrogen evolution reaction (HER) electrocatalysts largely relies on sophisticated phase modulation and judicious innovation on conductive matrix/support. In this work the controllable synthesis of phosphate ion (PO43−) intercalation induced‐MoSe2 (P‐MoSe2) nanosheets on N‐doped mold spore carbon (N‐MSC) forming P‐MoSe2/N‐MSC composite electrocatalysts is realized. Impressively, a novel conductive N‐MSC matrix is constructed by a facile mold fermentation method. Furthermore, the phase of MoSe2 can be modulated by a simple phosphorization strategy to realize the conversion from 2H‐MoSe2 to 1T‐MoSe2 to produce biphase‐coexisted (1T‐2H)‐MoSe2 by PO43‐ intercalation (namely, P‐MoSe2), confirmed by synchrotron radiation technology and spherical aberration‐corrected TEM (SACTEM). Notably, higher conductivity, lower bandgap and adsorption energy of H+ are verified for the P‐MoSe2/N‐MSC with the help of density functional theory (DFT) calculation. Benefiting from these unique advantages, the P‐MoSe2/N‐MSC composites show superior HER performance with a low Tafel slope (≈51 mV dec‐1) and overpotential (≈126 mV at 10 mA cm‐1) and excellent electrochemical stability, better than 2H‐MoSe2/N‐MSC and MoSe2/carbon nanosphere (MoSe2/CNS) counterparts. This work demonstrates a new kind of carbon material via biological cultivation, and simultaneously unravels the phase transformation mechanism of MoSe2 by PO43‐ intercalation.

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Section: Application Of Noble‐metal‐based Nanostructures In Electrochmentioning

confidence: 99%

Recent Advances on Water‐Splitting Electrocatalysis Mediated by Noble‐Metal‐Based Nanostructured Materials

Sun

Qin

et al. 2020

Advanced Energy Materials

688

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Electrochemical water splitting plays a crucial role in the development of clean and renewable energy production and conversion, which is a promising pathway to reduce social dependence on fossil fuels. Thus, highly active, cost‐efficient, and robust catalysts must be developed to reduce the reaction overpotential and increase electrocatalytic efficiency. In this review, recent research efforts toward developing advanced electrocatalysts based on noble metals with outstanding performance for water splitting catalysis, which is mainly dependent on their structure engineering, are summarized. First, a simple description of the water‐splitting mechanism and some promising structure engineering strategies are given, including heteroatom incorporation, strain engineering, interface/hybrid engineering, and single atomic construction. Then, the underlying relationship between noble metal electronic/geometric structure and performance for water splitting is discussed with the assistance of theoretical simulation. Finally, a personal perspective is provided in order to highlight the challenges and opportunities for developing novel electrocatalysts suitable for a wide range of commercial uses in water splitting for structural engineering applications.

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Chemically activating MoS2 via spontaneous atomic palladium interfacial doping towards efficient hydrogen evolution

Cited by 551 publications

References 46 publications

Single‐Atom Ru Doping Induced Phase Transition of MoS₂ and S Vacancy for Hydrogen Evolution Reaction

Single‐Atom Ru Doping Induced Phase Transition of MoS₂ and S Vacancy for Hydrogen Evolution Reaction

Coupled Biphase (1T‐2H)‐MoSe₂ on Mold Spore Carbon for Advanced Hydrogen Evolution Reaction

Recent Advances on Water‐Splitting Electrocatalysis Mediated by Noble‐Metal‐Based Nanostructured Materials

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Chemically activating MoS2 via spontaneous atomic palladium interfacial doping towards efficient hydrogen evolution

Cited by 551 publications

References 46 publications

Single‐Atom Ru Doping Induced Phase Transition of MoS2 and S Vacancy for Hydrogen Evolution Reaction

Single‐Atom Ru Doping Induced Phase Transition of MoS2 and S Vacancy for Hydrogen Evolution Reaction

Coupled Biphase (1T‐2H)‐MoSe2 on Mold Spore Carbon for Advanced Hydrogen Evolution Reaction

Recent Advances on Water‐Splitting Electrocatalysis Mediated by Noble‐Metal‐Based Nanostructured Materials

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Resources

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Single‐Atom Ru Doping Induced Phase Transition of MoS₂ and S Vacancy for Hydrogen Evolution Reaction

Single‐Atom Ru Doping Induced Phase Transition of MoS₂ and S Vacancy for Hydrogen Evolution Reaction

Coupled Biphase (1T‐2H)‐MoSe₂ on Mold Spore Carbon for Advanced Hydrogen Evolution Reaction