Abstract:Interfacial electronic characteristics is crucial for hydrogen evolution reaction (HER), especially in nanoscale heterogeneous catalysts. In this work, we found that the synergistic promotions between CoS2 and MoS2 (2H-MoS2 and...
“…The HER mechanism in an alkaline medium involves three steps: 31,32 Volmer step: H 2 O + e − + H* → OH − Heyrovsky step: H* + H 2 O + e − → OH − + H 2 Tafel step : H* + H* → H 2 It is well known that the Volmer step is the adsorption reaction ( b = 120 mV dec −1 ), while the Heyrovsky ( b = 40 mV dec −1 ) and Tafel step ( b = 30 mV dec −1 ) are the electrochemical sorption and desorption of H 2 . 33 The Tafel slope of 80.6 mV dec −1 for FMS 0.5 illustrates that the HER reaction is in accordance with the Heyrovsky–Volmer mechanism. The interfacial coupling between the 1T-MoS 2 nanoflowers and FeS nanosheets in FMS 0.5 would promote the adsorption of H* and dissociation of H 2 O.…”
The exploration of highly efficient noble metal-free catalysts for overall water splitting is crucial for industrial application. In this work, FeS nanosheets/1T-MoS2 nanoflowers on conductive iron foam (IF) was prepared...
“…The HER mechanism in an alkaline medium involves three steps: 31,32 Volmer step: H 2 O + e − + H* → OH − Heyrovsky step: H* + H 2 O + e − → OH − + H 2 Tafel step : H* + H* → H 2 It is well known that the Volmer step is the adsorption reaction ( b = 120 mV dec −1 ), while the Heyrovsky ( b = 40 mV dec −1 ) and Tafel step ( b = 30 mV dec −1 ) are the electrochemical sorption and desorption of H 2 . 33 The Tafel slope of 80.6 mV dec −1 for FMS 0.5 illustrates that the HER reaction is in accordance with the Heyrovsky–Volmer mechanism. The interfacial coupling between the 1T-MoS 2 nanoflowers and FeS nanosheets in FMS 0.5 would promote the adsorption of H* and dissociation of H 2 O.…”
The exploration of highly efficient noble metal-free catalysts for overall water splitting is crucial for industrial application. In this work, FeS nanosheets/1T-MoS2 nanoflowers on conductive iron foam (IF) was prepared...
“…ΔG H is widely used as a measure of HER activity, with values close to zero indicating high catalytic activity. 68 Figure 7a shows the calculated adsorption energies of N,P-2H-MoS reduces ΔG H to 0.66 and 0.37 eV for N and P doping, respectively, which increases the number of active sites on the basal plane. For N,P-2H-MoS 2 , the ΔG H is comparable to that of N-MoS 2 (0.66 eV), while N,P-1T-MoS 2 exhibits a significantly lower ΔG H of 0.13 eV, indicating that the presence of the 1T phase activates more active sites and has a significant impact on the HER catalytic performance.…”
Section: ■ Results and Discussionmentioning
confidence: 99%
“…First, to validate the role of N and P doping, we calculated the adsorption energies (Δ G H ) of H* at different adsorption sites. Δ G H is widely used as a measure of HER activity, with values close to zero indicating high catalytic activity Figure a shows the calculated adsorption energies of N,P-2H-MoS 2 , N,P-1T-MoS 2 , N-MoS 2 , P-MoS 2 , 2H-MoS 2 and 1T-MoS 2 at S sites.…”
The
multiple strategy design is crucial for enhancing the efficiency
of nonprecious electrocatalysts in hydrogen evolution reaction (HER).
In this work, we successfully synthesized N, P-codoped MoS2 nanosheets as highly efficient catalysts by integrating doping effects
and phase engineering using a porous metal–organic framework
(MOF) template. The electrocatalysts exhibit excellent bifunctional
activity and stability in alkaline media. The N, P codoping induces
electron redistribution to enhance conductivity and promote the intrinsic
activity of the electrocatalysts. It optimizes the H* adsorption free
energy and the dissociative adsorption energy, resulting in significant
enhancement of HER activity. Moreover, the porous MOF structure exposes
a large number of electrochemically active sites and facilitates the
diffusion of ions and gases, which improve charge transfer efficiency
and structural stability. Specifically, at a current density of 10
mA cm–2, the overpotential of the HER is only 32
mV, with a Tafel slope of 47 mV dec–1 and Faradaic
efficiency as high as 98.51% (at 100 mA cm–2). Only
a 338 mV overpotential is required to achieve a current density of
50 mA cm–2 for oxygen evolution reaction (OER),
and a potential of 1.49 V (at 10 mA cm–2) is sufficient
to drive overall water splitting. Further experimental measurements
and first-principles calculations evidence that the exceptional performance
is primarily attributed to the dual functionality of N and P dopants,
which not only activate additional S sites but also initialize the
phase transition of 2H to 1T-MoS2 to facilitate the rapid
charge transfer. Through in-depth exploration of the combined design
of multiple strategies for efficient catalysts, our work paves a new
way for the development of future efficient nonprecious metal catalysts.
“…Furthermore, the implementation of heterogeneous structures offers a viable approach to improve the efficiency of electrocatalytic hydrogen evolution. − By comprehensively considering factors such as material composition, vacancy, structure, and electron transfer, catalysts can be engineered to exhibit more efficient, stable, and controllable performance in reactions like water electrolysis. This is particularly significant for advancing the field of renewable energy, especially in the hydrogen industry. , Considering the properties of MoS 2 and CoS 2 , combining CoS 2 with MoS 2 , especially in the construction of effective heterojunctions, emerges as a highly potential approach for generating hydrogen across a wide range of pH levels. ,, Recent studies have provided valuable insights. Tao and co-workers demonstrated that both the two hexagonal (2H) and one trigonal (1T) phases of MoS 2 and CoS 2 heterojunctions exhibit synergistic catalytic activity surpassing that of individual components across the entire pH range .…”
Section: Introductionmentioning
confidence: 99%
“…This is particularly significant for advancing the field of renewable energy, especially in the hydrogen industry. , Considering the properties of MoS 2 and CoS 2 , combining CoS 2 with MoS 2 , especially in the construction of effective heterojunctions, emerges as a highly potential approach for generating hydrogen across a wide range of pH levels. ,, Recent studies have provided valuable insights. Tao and co-workers demonstrated that both the two hexagonal (2H) and one trigonal (1T) phases of MoS 2 and CoS 2 heterojunctions exhibit synergistic catalytic activity surpassing that of individual components across the entire pH range . Wang and co-workers reported that 2D–2D CoS 2 –MoS 2 heterostructures, leveraging the synergistic effects of electron transfer and geometric structure, attain a current density of 10 mA cm –2 with overpotentials of 251 mV in alkaline and 218 mV in acidic conditions, respectively .…”
The practical utilization of the hydrogen evolution reaction
(HER)
necessitates the creation of electrocatalysts that are both efficient
and abundant in earth elements, capable of operating effectively within
a wide pH range. However, this objective continues to present itself
as an arduous obstacle. In this research, we propose the incorporation
of sulfur vacancies in a novel heterojunction formed by MoS2@CoS2, designed to exhibit remarkable catalytic performances.
This efficacy is attributed to the advantageous combination of the
low work function and space charge zone at the interface between MoS2 and CoS2 in the heterojunction. The MoS2@CoS2 heterojunction manifests outstanding hydrogen evolution
activity over an extensive pH range. Remarkably, achieving a current
density of 10 mA cm–2 in aqueous solutions 1.0 M
KOH, 0.5 M H2SO4, and 1.0 M phosphate-buffered
saline (PBS), respectively, requires only an overpotential of 48,
62, and 164 mV. The Tafel slopes for each case are 43, 32, and 62
mV dec–1, respectively. In this study, the synergistic
effect of MoS2 and CoS2 is conducive to electron
transfer, making the MoS2@CoS2 heterojunction
show excellent electrocatalytic performance. The synergistic effects
arising from the heterojunction and sulfur vacancy not only contribute
to the observed catalytic prowess but also provide a valuable model
and reference for the exploration of other efficient electrocatalysts.
This research marks a significant stride toward overcoming the challenges
associated with developing electrocatalysts for practical hydrogen
evolution applications.
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