Li Ziya, Zhang Chao, Wang Haipeng, Zhang Delu, Zhuang Tao, Lv Zhiguo
School of Chemical Engineering, Qingdao University of Science and Technology, Qingdao 266042, China.
School of Chemical Engineering, Qingdao University of Science and Technology, Qingdao 266042, China.
J Colloid Interface Sci. 2025 Jul;689:137282. doi: 10.1016/j.jcis.2025.137282. Epub 2025 Mar 10.
Combining single atoms via phase transition engineering (from 2H to 1T) remains a challenge in MoS-based catalysts. Herein, we report that Pt single atoms (Pt) were doped into a 3D flower-like 1T-MoS catalyst (Pt@MoS) using a Pt-S bonding strategy. Doping with Pt induced a phase transition in MoS from the 2H phase to the 1T phase. Pt@MoS exhibited outstanding hydrogen evolution reaction (HER) performance, featuring an overpotential of 25 mV at 10 mA cm, a Tafel slope of 43.6 mV dec, and excellent long-term stability. The Pt-S first-shell scattering of Pt@MoS in extended X-ray absorption fine structure (EXAFS) directly indicated that the Pt was anchored near S atoms, forming Pt-S bonds. Furthermore, S atoms proximal to Pt functioned as catalytically active sites for HER, with Pt acting as an electron transfer mediator, facilitating the electron transfer from Mo to Pt and then to S. The p-band center of S showed a positive shift, indicating that Pt@MoS interacted weakly with hydrogen, thereby accelerating the desorption of H atoms to generate H. Additionally, Pt@MoS exhibited a ΔG of only -0.13 eV, which also favored H production.
通过相变工程（从2H相转变为1T相）来结合单原子，在基于MoS的催化剂中仍然是一项挑战。在此，我们报道了利用Pt-S键合策略将Pt单原子（Pt）掺杂到三维花状1T-MoS催化剂（Pt@MoS）中。Pt的掺杂诱导了MoS从2H相到1T相的相变。Pt@MoS表现出出色的析氢反应（HER）性能，在10 mA cm时过电位为25 mV，塔菲尔斜率为43.6 mV dec，并且具有出色的长期稳定性。在扩展X射线吸收精细结构（EXAFS）中，Pt@MoS的Pt-S第一壳层散射直接表明Pt锚定在S原子附近，形成了Pt-S键。此外，靠近Pt的S原子充当HER的催化活性位点，Pt作为电子转移介质，促进电子从Mo转移到Pt，然后再转移到S。S的p带中心出现正移，表明Pt@MoS与氢的相互作用较弱，从而加速H原子的脱附以生成H。此外，Pt@MoS的吉布斯自由能变化（ΔG）仅为-0.13 eV，这也有利于H的生成。
