Doping
nonmetal atoms into layered transition metal dichalcogenide
MX2 structures has emerged as a promising strategy for
enhancing their catalytic activities for the hydrogen evolution reaction.
In this study, we developed a new and efficient one-step approach
that involves simultaneous plasma-induced doping and exfoliating of
MX2 bulk into nanosheets–such as MoSe2, WSe2, MoS2, and WS2 nanosheets–within
a short time and at a low temperature (ca. 80 °C). Specifically,
by utilizing active plasma that is generated with an asymmetric electrical
field during the electrochemical reaction at the surface of the submerged
cathode tip, we are able to achieve doping of nitrogen atoms, from
the electrolytes, into the semiconducting 2H-MX2 structures
during their exfoliation process from the bulk states, forming N-doped
MX2. We selected N-doped MoS2 nanosheets for
demonstrating their catalytic hydrogen evolution potential. We modulated
the electronic and transport properties of the MoS2 structure
with the synergy of nitrogen doping and exfoliating for enhancing
their catalytic activity. We found that the nitrogen concentration
of 5.2 atom % at N-doped MoS2 nanosheets have an excellent
catalytic hydrogen evolution reaction, where a low overpotential of
164 mV at a current density of 10 mA cm–2 and a
small Tafel slope of 71 dec mV–1–much lower
than those of exfoliated MoS2 nanosheets (207 mV, 82 dec
mV–1) and bulk MoS2 (602 mV, 198 dec
mV–1)–as well as an extraordinary long-term
stability of >25 h in 0.5 M H2SO4 can be
achieved.
A novel redox gel polymer electrolyte based on redox additive, phloroglucinol, incorporated PVA–LiClO4 and graphene nanosheet-based electrodes for symmetrical supercapacitors.
With the goal of obtaining sustainable earth-abundant electrocatalyst materials displaying high performance in the hydrogen evolution reaction (HER), here we propose a facile one-pot plasmainduced electrochemical process for the fabrication of new core−shell structures of ultrathin MoS 2 nanosheets engulfed within onion-like graphene nanosheets (OGNs@MoS 2 ). The resultant OGNs@MoS 2 structures not only increased the number of active sites of the semiconducting MoS 2 nanosheets but also enhanced their conductivity. Our OGNs@MoS 2 composites exhibited high HER performance, characterized by a low overpotential of 118 mV at a current density of 10 mA cm −2 , a Tafel slope of 73 mV dec −1 , and long-time stability of 10 5 s without degradation; this performance is much better than that of the sheet-like graphene-wrapped MoS 2 composite GNs@MoS 2 (182 mV, 82 mV dec −1 ) and is among the best ever reported for composites involving MoS 2 and graphene nanosheets prepared through a simple one-batch process and using a low temperature and a short time for the HER. This approach appears to be an effective and simple strategy for tuning the morphologies of composites of graphene and transition metal dichalcogenide materials for a broad range of energy applications.
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