Xin Changhui, Sun Hezheng, Yao Jiaxin, Wang Bin, Yu Xin, Tang Yanting
Henan Engineering Research Center of Resource & Energy Recovery from Waste, School of Energy Science and Technology, Henan University, Zhengzhou 450046, China.
Henan Engineering Research Center of Resource & Energy Recovery from Waste, School of Energy Science and Technology, Henan University, Zhengzhou 450046, China.
J Colloid Interface Sci. 2024 Sep;669:477-485. doi: 10.1016/j.jcis.2024.04.224. Epub 2024 May 1.
Solar-light photosynthesis of ammonia form N reduction in ultrapure water over the artificial photocatalysts is attractive but still challenging compared with Haber-Bosch process. In this work, ultrathin Fe-TaO nanobelts were fabricated via the controllable solvothermal process for ammonia photosynthesis. The formed oxygen vacancies and Fe doping narrowed their bandgap energies and promoted the carriers' separation and transfer for Fe-TaO nanobelts. In addition, Fe doping also resulted in the reduced working functions of the samples, indicating a weaker electron binding restriction and stronger separation and transfer of photo-induced carriers. The experimental results showed that Fe-TaO nanobelts showed remarkably enhanced photocatalytic ammonia production performance under simulated sunlight irradiation, and the relevant ammonia production rate reached approximately 3030.86 μM g h, which was 9.63 times of pristine TaO and 491.0 times of commercial TaO, and a relatively stable photocatalytic ammonia production performance under simulated sunlight irradiation for Fe-TaO nanobelts. Meanwhile, it was also found that Fe doping has great influences on the photocatalytic performance under visible light and simulated sunlight irradiation, mainly because of their suitable bandgap energies and enhanced solar-light harvesting capacity. Current work indicates the great potentials of ultrathin tantalum-based functional materials for high-efficiency ammonia photosynthesis.
与哈伯-博施法相比，利用人工光催化剂在超纯水中通过太阳能光合成将氮还原为氨具有吸引力，但仍具有挑战性。在这项工作中，通过可控的溶剂热法制备了超薄Fe-TaO纳米带用于氨的光合成。形成的氧空位和Fe掺杂使Fe-TaO纳米带的带隙能量变窄，促进了载流子的分离和转移。此外，Fe掺杂还导致样品的功函数降低，表明电子束缚限制减弱，光生载流子的分离和转移增强。实验结果表明，Fe-TaO纳米带在模拟太阳光照射下表现出显著增强的光催化产氨性能，相关产氨速率达到约3030.86 μM g h，是原始TaO的9.63倍，商业TaO的491.0倍，并且在模拟太阳光照射下Fe-TaO纳米带具有相对稳定的光催化产氨性能。同时，还发现Fe掺杂对可见光和模拟太阳光照射下的光催化性能有很大影响，主要是因为它们具有合适的带隙能量和增强的太阳光捕获能力。当前的工作表明超薄钽基功能材料在高效氨光合成方面具有巨大潜力。
