Yijie Yang,Shun Yao,Ying Li,Yuanhang Wu,Chang Li,Congshu Hang,Hui Li
Development of efficient, low-cost, and bifunctional catalysts based on ultrathin heterostructures for both the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is critical for advancing overall water splitting. In this study, we design a simple intercalation-sulfidation strategy by rigid segment-containing Polysulfide as a sulfur source and in-situ intercalation for the construction of the metastable 1 T'-2H'-phase Mo-Ni 3 S 2 heterostructures (1 T'-2H'-Mo-Ni 3 S 2 ). It is found that the Polysulfides with rigid segments can be controlled by various monomers reacted with reverse sulfurization reactions between various monomers and elemental sulfur, such as Poly (sulfur-random-1,3-Benzenedithiol), Poly (sulfur-random-1,4-Benzenedithiol), and Poly (sulfur-random-4,4′-Biphenyldithiol), which can be used to assist in the synthesis process of metastable. Attributing to favorable synergy interaction in composition and structure, the resultant 1 T'-2H' phase Mo-Ni 3 S 2 heterostructures shows the superior performances toward OER and water splitting in alkaline medium. The resultant Mo-Ni 3 S 2 -BDP needs only an overpotential of 103 mV at a current density of 10 mA cm −2 and for OER. For HER, it demonstrates a low overpotential of 136 mV at 10 mA cm −2 , and a relatively low cell voltage of 1.672 V for water splitting. The present provides a new strategy to design and develop the phase engineering of other materials with various Polymorphs.
Electrolytic water splitting using transition metal sulfide catalysts has garnered a lot of attention lately. Herein, a composite material consisting of Mo-doped Ni 3 S 2 nanoparticles supported on N-doped carbon layers with anchored Ni single atoms (Mo–Ni 3 S 2 /Ni–N–C) was synthesized using a two-step hydrothermal process. These features enable Mo–Ni 3 S 2 /Ni–N–C to achieve low overpotentials of 71, 58, and 89 mV for the hydrogen evolution reaction (HER) at 10 mA cm −2 in 1 M KOH, 0.5 M H 2 SO 4 , and 1 M PBS, respectively. After 20 h of durability testing, its current density retains over 95 % of the initial value across diverse pH electrolytes. Mo doping enhances structural stability, enabling wide pH applicability. Electron transfer from Ni 3 S 2 nanoparticles to Ni single atoms accelerates kinetics and boosts intrinsic activity, which improves HER performance. Theoretical calculations confirm that Ni single atoms possess ideal H∗ adsorption energy, which optimizes H∗ adsorption capability of Ni 3 S 2 . This work offers suggestions for creating excellent low-cost electrolytic water catalysts.
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