Wang Rongzhi, Zheng Jin-Cheng
Department of Physics, Fujian Provincial Key Laboratory of Theoretical and Computational Chemistry, Xiamen University, Xiamen 361005, China.
Department of Physics and Department of New Energy Science and Engineering, Xiamen University Malaysia, Sepang 43900, Malaysia.
Phys Chem Chem Phys. 2024 Feb 14;26(7):5848-5857. doi: 10.1039/d3cp05241a.
Hydrogen is identified as one of the most promising sustainable and clean energy sources. The development of a hydrogen evolution reaction (HER) catalyst with high activity is essential to meet future needs. Considering the novel advantages of two-dimensional materials and the high catalytic activity of atomic transition metals, in this study, using density functional theory calculations, the HER on a single transition metal (10 different TM atoms) adsorbed and doped ZnO monolayer (ZnO-m) has been investigated. The Volmer-Tafel reaction mechanisms and strain engineering of the three best HER catalysts are also discussed. The results show that Pt@ZnO-m, Co-doped ZnO-m and Ir-doped ZnO-m with high stability all have a smaller absolute H adsorption free energy than Pt, and the optimal value of Pt@ZnO-m is -0.017 eV. The calculation of the reaction energy barriers shows that the Volmer-Tafel step is favorable. Co@ZnO-m and Ir@ZnO-m have high HER activity, the widest pH range, and acid-alkali resistance. Pt@ZnO-m and Co-doped ZnO-m maintain excellent HER performances in the strain range of -4% to 4%.
氢被认为是最有前途的可持续清洁能源之一。开发具有高活性的析氢反应（HER）催化剂对于满足未来需求至关重要。考虑到二维材料的新颖优势和原子级过渡金属的高催化活性，在本研究中，使用密度泛函理论计算，研究了吸附和掺杂有单一过渡金属（10种不同的过渡金属原子）的ZnO单层（ZnO-m）上的析氢反应。还讨论了三种最佳析氢催化剂的Volmer-Tafel反应机理和应变工程。结果表明，具有高稳定性的Pt@ZnO-m、Co掺杂的ZnO-m和Ir掺杂的ZnO-m的绝对氢吸附自由能均比Pt小，Pt@ZnO-m的最佳值为-0.017 eV。反应能垒的计算表明Volmer-Tafel步骤是有利的。Co@ZnO-m和Ir@ZnO-m具有高析氢活性、最宽的pH范围以及耐酸碱性能。Pt@ZnO-m和Co掺杂的ZnO-m在-4%至4%的应变范围内保持优异的析氢性能。
