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Nanomaterials 2020, 10, 1407 14 of 26 any kind, since its electrochemical properties do not affect the behavior of the working one. However, when the Pt wire was used as the counter electrode, the electrochemical catalytic activity of CNHs towards HER was greatly improved and was even as good as the commercial Pt/C. This was attributed to the dissolution of the Pt electrode from the oxidation reaction (Pt0 to Pt2+), which is favored in long time tests under acidic medium. The dissolved Pt2+ transfers to the working electrode surface and is deposited on the electrode materials, which leads to increased catalytic performance. However, this was not observed when graphite rod was used as a counter electrode. The above findings demonstrate the importance of evaluating all parameters to avoid reaching misleading conclusions. The turf of water splitting engaging CNHs as electrocatalysts remains quite unexplored, since only few works have been reported so far regarding this concept. In this regard, hybridization of nonprecious metals with CNHs by employing diverse designs and strategies is a highly appealing concept in order to enhance their performance [96,138]. Furthermore, there is no question that use of CNHs has been an effective way to minimize the loading of precious metals. In this route, Pt nanoparticles were immobilized on amine-bearing CNHs onto poly(amido amine) (PAMAM) dendrimers [139], as shown in Figure 4. The dendrimer was used as linkage for the stabilization of the Pt nanoparticles on the modified CNHs, but also as a stabilizer to prevent the agglomeration of the nanoparticles. The so-formed CNH-based hybrid material showed excellent HER activity, durability, and stability even with low loading (~1 wt%) of Pt, which was approximately 40 times lower than commercial 40 wt% Pt/C. The hybrid’s HER efficiency was comparable to 40 wt% Pt/C as well as to Pt/MoS2-based electrocatalysts consisting of 10 and 2.03 wt% Pt. In addition, the Volmer–Heyrovsky mechanism was found to be the rate-limiting step for as-prepared catalyst, whereas for Pt/C, the Volmer–Tafel mechanism characterizes the kinetics of the reaction. The role of CNHs as electrocatalytic supports for MoS2 and polydopamine (PDA)/Pd nanoparticles was also studied and their performance towards HER was evaluated [140]. The presence of PDA ensured the uniform distribution of Pd nanoparticles on the surface of CNHs without aggregation, generating the PDA-Pd/CNHs hybrid material, whereas the thin coating of PDA reduced the inhibition for the reversible oxidation nature of Pd nanoparticles. In the same work, the MoS2 and CNH-based hybrid material, MoS2/CNHs, was acquired via the in situ preparation of MoS2 in the presence of CNHs by using a hydrothermal method [140]. In general, transition metal dichalcogenides (TMDs) are able to minimize overpotential for HER and lower Tafel slope values due to their innate catalytic activities [141]. Hence, they have been massively studied and employed in the development of electrocatalysts for HER with various architectures [142–146]. Moreover, carbon-based nanomaterials, like graphene and heteroatom-doped graphene, have been effectually combined with TMDs (MoS2, WS2, MoSe, etc.), further boosting their catalytic activity [67,147–149]. However, the MoS2/CNHs electrocatalyst showed poor performance for HER, attributed to the ineffective interactions between the two elements, since MoS2 sheets wrapped around CNHs, blocking the exposure of their defective sites. On the other hand, the contribution of CNHs to PDA-Pd triggered a superior hydrogen production than MoS2/CNHs. This was further screened from the lower Tafel slope value of the metal-based electrocatalyst (61 mV/dec) compared to MoS2/CNHs (86 mV/dec).PDF Image | Carbon Nanohorn-Based Electrocatalysts for Energy Conversion
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