Ahmed Muhammad, Kour Gurpreet, Sun Ziqi, Du Aijun, Mao Xin
School of Chemistry and Physics, Faculty of Science, Queensland University of Technology, Gardens Point Campus, Brisbane, QLD 4001, Australia.
QUT Centre for Materials Science, Queensland University of Technology, Gardens Point Campus, Brisbane, QLD 4001, Australia.
Nanomaterials (Basel). 2023 Jul 21;13(14):2122. doi: 10.3390/nano13142122.
The hydrogen evolution reaction (HER) is a remarkable mechanism which yields the production of hydrogen through a process of water electrolysis. However, the evolution of hydrogen requires highly conductive and stable catalysts, such as the noble metal platinum (Pt). However, the problem lies in the limitations that this catalyst and others of its kind present. Due to limited availability, as well as the costs involved in acquiring such catalysts, researchers are challenged to manufacture catalysts that do not present these limitations. Carbon nanotubes (CNTs), which are nanomaterials, are known to have a wide range of applications. However, specifically, the pristine carbon nanotube is not suitable for the HER due to the binding free energy of its positive H-atoms. Hence, for the first time, we demonstrated the use of the proposed aryl-functionalised catalysts, i.e., Aryl-L@SWCNT (L = Br, CCH, Cl, COCH, F, I, NO, or t-butyl), along with the effect of the sp2-sp3 hybridised interface through the density functional theory (DFT). We performed calculations of single-walled carbon nanotubes with multiple aryl functional groups. By employing the DFT calculations, we proved that the curvature of the nanotubes along with the proposed aryl-functionalised catalysts had a noteworthy effect on the performance of the HER. Our study opens the door to investigating a promising group of catalysts for sustainable hydrogen production.
析氢反应（HER）是一种通过水电解过程产生氢气的重要机制。然而，氢气的析出需要高导电性和稳定性的催化剂，比如贵金属铂（Pt）。然而，问题在于这种催化剂以及同类的其他催化剂存在局限性。由于其可用性有限，以及获取此类催化剂的成本问题，研究人员面临着制造不存在这些局限性的催化剂的挑战。碳纳米管（CNTs）作为纳米材料，具有广泛的应用。然而，具体来说，原始碳纳米管因其正氢原子的结合自由能而不适用于析氢反应。因此，我们首次展示了所提出的芳基功能化催化剂，即芳基-L@单壁碳纳米管（L = Br、CCH、Cl、COCH、F、I、NO或叔丁基）的应用，以及通过密度泛函理论（DFT）研究sp2-sp3杂化界面的影响。我们对具有多个芳基官能团的单壁碳纳米管进行了计算。通过采用DFT计算，我们证明了纳米管的曲率以及所提出的芳基功能化催化剂对析氢反应性能有显著影响。我们的研究为探索一组有前景的可持续制氢催化剂打开了大门。
