Pore Surface Engineering of Covalent Triazine Frameworks@MoS₂ Electrocatalyst for the Hydrogen Evolution Reaction

Abstract

Electrochemical water splitting is an important strategy for the mass production of hydrogen. Development of synthesizable catalysts has always been one of the biggest obstacles to replace platinum‐group catalysts. In this work, a high quality crystal polymer covalent triazine framework [CTF; Brunauer–Emmett–Teller (BET) surface area of 1562.6 m2 g−1] is synthesized and MoS2 nanoparticles are grown in situ into/onto the 1 D channel arrays or the external surface for electrocatalysis [hydrogen evolution reaction (HER)] . The state‐of‐the‐art CTFs@MoS2 structure exhibits superior catalytic kinetics with an overpotential of 93 mV and Tafel slope of 43 mV dec−1, which is improved over most other reported analogous catalysts. The inherent π‐conjugated crystal channels in CTFs provides a multifunctional support for electron transmission and mass diffusion during the hydrogen evolution process. Catalytic kinetics analysis shows that the HER performance is closely correlated to the hierarchical pore parameters and aggregated thickness of MoS2 nanoparticles. This work provides an attractive and durable alternative to synthesize high activity and stable catalysts for HER.

MoS2-Carbon Inter-overlapped Structures as Effective Electrocatalysts for the Hydrogen Evolution Reaction

“…The XRD spectra for as-prepared samples at different reaction temperatures and after the carbonization step are shown in Figure 1. After hot-injection of the S-precursor and the reaction temperature being held at 280 °C, several peaks related to MoOx complex (mixture of MoO3, Mo8O23, Mo4O11 and MoO2 [24]) were observed in the XRD spectra, in Figure 1a, thus indicating that the temperature was not sufficient for the formation of MoS2. When the temperature was further increased to 350 °C, which is closer to the boiling point of OLA, the reaction was under an intense environment that could trigger MoOx recrystallization to monolayer MoS2.…”

“…Consequently, 1T-MoS 2 nanosheets have attracted significant attention in the research community due to their outstanding performance in energy storage devices [ 7 , 10 , 11 , 18 , 20 ], electrocatalysis [ 8 , 21 , 22 , 23 , 24 ], photoelectrochemical cells [ 14 , 22 , 25 , 26 ] and field-effect transistors [ 27 , 28 ], among others. Additionally, integrating 1T-MoS 2 with interlayer carbonaceous materials like grapheme [ 21 , 27 ], carbon nanotubes (CNTs) [ 29 , 30 ], reduced graphene oxide (RGO) [ 31 ], N-doped carbon or spherical carbon via anchoring [ 32 ], growth [ 33 ], loading or dispersion can further increase electrical conductivity, structural integrity and electrocatalytic activity [ 30 , 34 ].…”

Activating CoMoS with CoP3 Phase for High‐efficient Hydrogen Evolution Reaction in Acidic Condition

“…Molybdenum sulfide‐based nanomaterials have been considered as the most promising candidate for HER due to their remarkable HER activities and popular price [14–19] . However, molybdenum sulfide nanomaterials have the catalytic threshold due to their restricted active sites, high sulfur leaching rate and poor electrical conductivity.…”

“…[8][9][10][11][12][13] Molybdenum sulfide-based nanomaterials have been considered as the most promising candidate for HER due to their remarkable HER activities and popular price. [14][15][16][17][18][19] However, molybdenum sulfide nanomaterials have the catalytic threshold due to their restricted active sites, high sulfur leaching rate and poor electrical conductivity. Thus, lots of efforts have been spent on optimizing the electrocatalytic performances and conductivity of MoS x -based nanomaterials, such as the doping of metals from 3d period.…”

[Mo2O2S8]2− small molecule dimer as a basis for hydrogen evolution reaction (HER) catalyst materials

“…In terms of the second approach regarding site density, work has largely centered on replacing typically sheet-like and crystalline MoS 2 with new morphologies. High surface area constructs, such as highly dispersed nanoparticles [24,25] and porous networks [26][27][28][29], maximize the edge to bulk ratio in order to obtain substantial HER currents. Amorphous MoS x morphologies offer a large numbers of defects as compared to crystalline MoS 2 , thereby creating more active sulfur moieties [30].…”