One-pot synthesis of porous 1T-phase MoS2 integrated with single-atom Cu doping for enhancing electrocatalytic hydrogen evolution reaction

Ji, Liang; Yan, Pengfei; Zhu, Chuanhui; Ma, Chunyan; Wu, Wenzhuo; Wei, Cong; Shen, Yonglong; Chu, Shengqi; Wang, Jiaou; Du, Yi; Chen, Jun; Yang, Xinan; Xu, Qun

doi:10.1016/j.apcatb.2019.03.053

Cited by 183 publications

(152 citation statements)

References 45 publications

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“…In the work conducted by Yang et al (89), the difference between Gibbs free energies for four-electron and two-electron transfer ORR (G H2O -G H2O2 ) of Fe@pyridinic N, Fe@pyrrolic N, and Pt (111) was found to be consistent with the production of H 2 O 2 (Fig. 3D), indicating the Fe-pyrrolic-N species as the main active sites for ORR.…”

Section: Oxygen Reduction Reactionmentioning

confidence: 67%

Microenvironment modulation of single-atom catalysts and their roles in electrochemical energy conversion

et al. 2020

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Single-atom catalysts (SACs) have become the most attractive frontier research field in heterogeneous catalysis. Since the atomically dispersed metal atoms are commonly stabilized by ionic/covalent interactions with neighboring atoms, the geometric and electronic structures of SACs depend greatly on their microenvironment, which, in turn, determine the performances in catalytic processes. In this review, we will focus on the recently developed strategies of SAC synthesis, with attention on the microenvironment modulation of single-atom active sites of SACs. Furthermore, experimental and computational advances in understanding such microenvironment in association to the catalytic activity and mechanisms are summarized and exemplified in the electrochemical applications, including the water electrolysis and O2/CO2/N2 reduction reactions. Last, by highlighting the prospects and challenges for microenvironment engineering of SACs, we wish to shed some light on the further development of SACs for electrochemical energy conversion.

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Section: Oxygen Reduction Reactionmentioning

confidence: 67%

Microenvironment modulation of single-atom catalysts and their roles in electrochemical energy conversion

et al. 2020

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“…As can be seen, it confirms that the flower-like particles are composed of an agglomeration of few MoS2 layers, whereas Figure 4b shows the detail of a few MoS2 stacked layers in the same sample, which are composed of about 10 atomic layers. Further, a layer spacing of 0.66 nm can be observed, corresponding to the (002) crystalline plane of 2H-MoS2 [21]. The most noticeable difference between the pristine MoS2 and Re-doped MoS2 samples is the curvature associated in the latter ( Figure S1).…”

Section: Scanning Transmission Electron Microscopy Analysismentioning

confidence: 92%

Electrochemical Hydrogen Evolution over Hydrothermally Synthesized Re-Doped MoS2 Flower-Like Microspheres

et al. 2019

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In this research, we report a simple hydrothermal synthesis to prepare rhenium (Re)- doped MoS2 flower-like microspheres and the tuning of their structural, electronic, and electrocatalytic properties by modulating the insertion of Re. The obtained compounds were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), high-resolution transmission electron microscopy (HRTEM), Raman spectroscopy, and X-ray photoelectron spectroscopy (XPS). Structural, morphological, and chemical analyses confirmed the synthesis of poorly crystalline Re-doped MoS2 flower-like microspheres composed of few stacked layers. They exhibit enhanced hydrogen evolution reaction (HER) performance with low overpotential of 210 mV at current density of 10 mA/cm2, with a small Tafel slope of 78 mV/dec. The enhanced catalytic HER performance can be ascribed to activation of MoS2 basal planes and by reduction in charge transfer resistance during HER upon doping.

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“…To improve both HER and photoresponsive performances, a common strategy is to dope with heterogeneous atoms. [ 15 ] Recently, Co, [ 16 ] Cu, [ 17 ] Zn, [ 18 ] etc.‐doped TMD nanostructures showed improved HER catalytic activity, but both inevitable change of layered crystal structures and limit doping amount result in a poor use of such strategy. In addition, it was found that replacing the main group atoms (Ge, [ 19 ] Si, [ 20 ] Sn, [ 21 ] etc.)…”

Section: Figurementioning

confidence: 99%

Dual‐Enhanced Doping in ReSe₂ for Efficiently Photoenhanced Hydrogen Evolution Reaction

Wang

Han

et al. 2020

Advanced Science

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metal dichalcogenides (TMDs) are a typical 2D nanomaterial and have shown substantial progress in terms of catalysis and energy storage applications. [2] In the last few years, TMD-based catalysts have been optimized by introducing additional basalplane vacancies and metastable metallic crystal structures to overcome their low concentration of electrocatalytic activity sites and poor intrinsic electroconductibility; thus, the catalysts exhibited much enhanced HER catalytic activity. [3] In addition to achieving significant advances in structural designs, other driving forces, such as thermal energy, [4] field effect, [5] and strain engineering, [6] have also been utilized to boost the HER performance of electrocatalysts. [7] Because solar energy is an available clean and sustainable energy, solar-driven photocatalytic and photoelectrochemical water splitting has become one of the hottest topics in materials science. [8] Rhenium dichalcogenides (ReX 2 , X = S or Se) are a unique category of compounds that have both distorted triclinic symmetry (1T) crystal structure and excellent photoelectric properties with weak interlayer coupling; these characteristics ensure their excellent Rhenium dichalcogenides (ReX 2 , X = S or Se) are catalysts that have great promise for the photoenhanced hydrogen evolution reaction (PE-HER) because of their unique physiochemical properties. However, the catalytic performance is still restricted by their low concentration of electrocatalytic activity sites and poor injection of hot electrons. Herein, dual-enhancement in ReSe 2 nanosheets (NSs) with high concentration of active sites and efficient use of hot electrons is simultaneously achieved with moderate Mo doping. Contributions from exposed catalytically active sites, improved electrical conductivity, and enhanced solar spectral response are systematically investigated. Superior PE-HER catalytical performance is obtained in Re 0.94 Mo 0.06 Se 2 , which has more catalytically active sites and optimized band structure than other Re 1−x Mo x Se 2 samples. Here, it is demonstrated that only doping can reduce the overpotential (η 10 ) from 239 to 174 mV at −10 mA cm −2 (Δ1η 10 = 65 mV). Then, η 10 is further improved to 137 mV under simulated AM 1.5 sun illumination (Δ2η 10 = 37 mV). The total improvement (Δη 10 ) toward PE-HER is 102 mV (Δ1η 10 + Δ2η 10 = 102 mV) in optimal Re 0.94 Mo 0.06 Se 2 . This work presents a new perspective for researching highefficiency photoenhanced HER ReSe 2 -based electrocatalysts and other layered transition metal dichalcogenides. Figure 4. XANES spectra (inset in panel (a)) and a) EXAFS spectra of the as-exfoliated ReSe 2 and Re 0.94 Mo 0.06 Se 2 NSs. b) Density functional theory schematic diagram. c) HER free-energy diagram. d) Density of states plots for monolayers of ReSe 2 , Re 0.94 Mo 0.06 Se 2 , and MoSe 2 . e-g) Schematic diagrams of the separation and recombination process for an electron-hole in Re 1−x Mo x Se 2 . www.advancedsciencenews.com 2000216 (7 of 7)

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One-pot synthesis of porous 1T-phase MoS2 integrated with single-atom Cu doping for enhancing electrocatalytic hydrogen evolution reaction

Cited by 183 publications

References 45 publications

Microenvironment modulation of single-atom catalysts and their roles in electrochemical energy conversion

Microenvironment modulation of single-atom catalysts and their roles in electrochemical energy conversion

Electrochemical Hydrogen Evolution over Hydrothermally Synthesized Re-Doped MoS2 Flower-Like Microspheres

Dual‐Enhanced Doping in ReSe₂ for Efficiently Photoenhanced Hydrogen Evolution Reaction

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One-pot synthesis of porous 1T-phase MoS2 integrated with single-atom Cu doping for enhancing electrocatalytic hydrogen evolution reaction

Cited by 183 publications

References 45 publications

Microenvironment modulation of single-atom catalysts and their roles in electrochemical energy conversion

Microenvironment modulation of single-atom catalysts and their roles in electrochemical energy conversion

Electrochemical Hydrogen Evolution over Hydrothermally Synthesized Re-Doped MoS2 Flower-Like Microspheres

Dual‐Enhanced Doping in ReSe2 for Efficiently Photoenhanced Hydrogen Evolution Reaction

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Dual‐Enhanced Doping in ReSe₂ for Efficiently Photoenhanced Hydrogen Evolution Reaction