Henan Engineering Research Center of Resource & Energy Recovery from Waste, College of Chemistry and Chemical Engineering, Henan University, Kaifeng 475004, China.
Key Laboratory of Microsystems and Microstructures Manufacturing, Ministry of Education, Harbin Institute of Technology, Harbin 150001, China.
J Colloid Interface Sci. 2020 Feb 15;560:359-368. doi: 10.1016/j.jcis.2019.09.123. Epub 2019 Oct 12.
Highly ordered mesocrystalline semiconductors often indicate tremendous prospects in the clean energy production and environmental photocatalysis mainly because of their unique superstructure for efficient charge transport pathways and long-lived charges. Here, superstructure TaN mesocrystals with the high-energy surface {2 0 0} planes exposed were the first time to be successfully fabricated by topological transformation of TaO mesocrystals. The prepared TaN mesocrystals showed enhanced visible-light photocatalytic hydrogen production activity of 98.67 μmol g for 180 min irradiation, which was approximately 5.28 times that of comm-TaN prepared with commercial TaO as the starting material, mainly due to the formation of long-distance electron conduction pathways and long-lived charges. The detailed electronic band structures of the prepared TaN mesocrystals were also investigated by electrochemical method. Finally, possible visible-light photocatalytic mechanisms of TaN mesocrystals for enhanced hydrogen production was also proposed in detail. Current work also indicates that tantalum-based mesocrystals show great potential to enhance the charge separation for efficient photocatalytic water splitting.
高度有序的介孔半导体通常因其独特的超结构而在清洁能源生产和环境光催化方面具有巨大的前景，为有效的电荷传输途径和长寿命电荷提供了保障。在这里，首次通过 TaO 介晶的拓扑转变成功制备了暴露高能表面{200}面的 TaN 介晶超结构。所制备的 TaN 介晶在可见光照射 180 分钟下的光催化产氢活性提高到 98.67 μmol·g-1，是使用商业 TaO 作为起始原料制备的 comm-TaN 的 5.28 倍，主要是由于形成了长距离的电子传导途径和长寿命电荷。还通过电化学方法研究了所制备的 TaN 介晶的详细电子能带结构。最后，还详细提出了 TaN 介晶增强光催化产氢的可能可见光光催化机制。目前的工作还表明，基于钽的介晶在增强电荷分离以实现高效光催化水分解方面具有巨大的潜力。
