Li Wei, Choi Jin-Ho
College of Energy, Soochow Institute for Energy and Materials Innovations, Soochow University, Suzhou 215006, People's Republic of China.
Key Laboratory of Advanced Carbon Materials and Wearable Energy Technologies of Jiangsu Province, Soochow University, Suzhou 215006, People's Republic of China.
Nanotechnology. 2021 May 10;32(31). doi: 10.1088/1361-6528/abf777.
The development of low-cost, high-efficiency catalysts for the hydrogen evolution reaction is important for hydrogen production. In this study we investigate hydrogen adsorption at the interfaces of C/BN hetero-nanotubes using first-principles density functional theory calculations. Substantial charge redistributions associated with states near the Fermi level occur at the interfaces. More importantly, such electronic modification can enhance hydrogen adsorption at the interfacial atoms. As a result, the adsorption free energies Δof hydrogen for the interfaces range from -0.26 to 0.30 eV, depending on hydrogen coverage. These values are much closer to zero than those for the basal plane, suggesting that the interfaces could be active sites for the hydrogen evolution reaction. The interfacial adsorption sites show a distinctive hybridization between the H s and C p orbitals, which accounts for the enhanced hydrogen adsorption at the interfaces. These findings have important implications for hydrogen energy applications.
开发用于析氢反应的低成本、高效催化剂对制氢至关重要。在本研究中，我们使用第一性原理密度泛函理论计算研究了C/BN异质纳米管界面处的氢吸附。与费米能级附近的态相关的大量电荷重新分布发生在界面处。更重要的是，这种电子修饰可以增强界面原子处的氢吸附。结果，界面处氢的吸附自由能Δ根据氢覆盖率在-0.26至0.30 eV范围内。这些值比基面的值更接近零，表明界面可能是析氢反应的活性位点。界面吸附位点在H s和C p轨道之间表现出独特的杂化，这解释了界面处氢吸附的增强。这些发现对氢能应用具有重要意义。
