| ZnSe@氮掺杂多孔碳异质结构诱导的高效析氢性能 | |
| Efficient hydrogen evolution reaction activity induced by ZnSe@nitrogen doped porous carbon heterojunction | |
| 摘要: 以锌基沸石咪唑酯骨架(Zn-based zeolitic imidazolate framework，Zn-ZIF)为前驱体，通过简单的一步热解策略制备出锌纳米粒子修饰的氮掺杂多孔碳(N-C)催化剂(Zn@N-C)，进一步将其负载的Zn纳米粒子通过硒化反应转化为ZnSe纳米颗粒，构建出ZnSe@N-C异质结催化剂。采用X射线衍射(XRD)、拉曼(Raman)光谱、X射线光电子能谱(XPS)、场发射扫描电子显微镜(FESEM)和透射电子显微镜(TEM)对催化剂的组分、结构和形貌进行了表征，并通过电化学测试系统评估了2种催化剂在析氢反应(hydrogen evolution reaction，HER)中的催化活性和稳定性。结果表明：通过硒化处理，催化剂的形貌由规整的菱形十二面体(Zn@N-C)转变为结构塌陷、褶皱变形的十二面体(ZnSe@N-C)，这增加了结构缺陷，从而引入了更多的催化活性位点。同时ZnSe和N-C基底间存在异质界面结构，这促进了电子的传输，提高了催化剂的活性。ZnSe@N-C在碱性HER过程中，在10 mA·cm-2的电流密度下获得了165.8 mV的过电位，优于Zn@N-C (190.8 mV)。此外，ZnSe@N-C在碱性溶液中具有良好的电化学稳定性。 | |
| 关键词: 析氢反应 硒化 ZnSe 氮掺杂多孔碳 催化剂 | |
| 基金项目: 青海理工大学(筹)新进教师(博士/硕士)论文延伸科研培育计划项目(No.2023011wys017)和青海理工大学(筹“)昆仑英才”人才引进项目(No.2023-QLGKLYCZX-021)资助。 | |
| Abstract: Zn nanoparticles-modified nitrogen-doped porous carbon (N-C) catalysts (Zn@N-C) were prepared by a simple one-step pyrolysis strategy using Zn-based zeolite imidazolate framework (Zn-ZIF) as the precursor. Subsequently, the Zn nanoparticles were further converted to the ZnSe nanoparticles by using a selenization strategy; meanwhile, the heterostructure between the ZnSe and N-C was constructed to enhance the catalytic activity of the catalysts. The components, structures, and morphologies of as-prepared catalysts were characterized by using X-ray diffraction (XRD), Raman, X - ray photoelectron spectroscopy (XPS), field emission scanning electron microscopy (FESEM), and transmission electron microscopy (TEM). Electrochemical tests in water splitting systematically evaluated the hydrogen evolution reaction (HER) catalytic activity and stability of the catalysts. Results showed that the morphology of the catalyst was transformed from a regular rhombic dodecahedron (Zn@N-C) to a structurally collapsed, folded, and deformed dodecahedron (ZnSe@N-C) by selenization, which increased the structural defects and introduced more catalytic active sites. Meanwhile, the existence of a heterogeneous interfacial structure between the ZnSe and N-C substrates was beneficial to the electron transport and improved the catalytic activity of the catalysts. ZnSe@N-C yielded a low overpotential of 165.8 mV at a current density of 10 mA·cm-2 in the HER process, which was superior to that of Zn@N-C (190.8 mV). ZnSe@N-C also demonstrated good electrochemical stability in an alkaline solution. | |
| Keywords: hydrogen evolution reaction selenization ZnSe nitrogen-doped porous carbon catalyst | |
| 投稿时间：2024-10-25 修订日期：2025-01-13 | |
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| 张永伟,朱闯,吴文斌,马永湧,杨恒.ZnSe@氮掺杂多孔碳异质结构诱导的高效析氢性能[J].无机化学学报,2025,41(4):650-660. | |
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