Yan Ai-Ping, Qiu Yu-Jue, Wang Xing-En, Wang Guang-Hua, Wei Xian-Kui, Li Xin-Tian, Chen Xiao-Die, Shang Xing, Deng Shun-Liu, Zheng Jian-Wei, Xie Su-Yuan
State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China.
Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), Xiamen 361005, China.
iScience. 2024 Jun 29;27(8):110420. doi: 10.1016/j.isci.2024.110420. eCollection 2024 Aug 16.
CN is widely applied in the synthesis of single-atom catalysts. However, understanding on the active site and the reaction mechanism is not fully in consensus. Especially, bare studies have considered the coordination environment of the single-atomic dopant and the effect of nitrogen vacancy on CN. In this study, we found that the presence of nitrogen vacancies promotes the activation of water and reduces the activation energy barrier for hydrogen generation. The results show that a synergistic effect between single-atom Pt and nitrogen vacancies enables the catalyst to achieve a superior hydrogen production rate of 3,890 μmol/g/h, which is 16.8 times higher than that of pristine CN. Moreover, the catalyst is also applicable for photocatalytic hydrogen production from seawater without significantly decreased hydrogen production rate. This study paves the way for the rational design and optimization of next-generation photocatalysts for sustainable energy applications, particularly in solar-driven hydrogen production.
氮化碳广泛应用于单原子催化剂的合成。然而，对于活性位点和反应机理的理解尚未完全达成共识。特别是，以往的研究仅考虑了单原子掺杂剂的配位环境以及氮空位对氮化碳的影响。在本研究中，我们发现氮空位的存在促进了水的活化并降低了产氢的活化能垒。结果表明，单原子铂与氮空位之间的协同效应使催化剂能够实现3890 μmol/g/h的优异产氢速率，这比原始氮化碳高出16.8倍。此外，该催化剂也适用于海水的光催化产氢，且产氢速率不会显著降低。本研究为合理设计和优化用于可持续能源应用的下一代光催化剂，特别是太阳能驱动的产氢，铺平了道路。
