Department of Materials Science and Engineering, College of Engineering, Peking University, Beijing, 100871, China.
State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan, 030001, China.
Adv Mater. 2019 Feb;31(5):e1807226. doi: 10.1002/adma.201807226. Epub 2018 Dec 5.
Inspired by natural photosynthesis, the design of new Z-scheme photocatalytic systems is very promising for boosting the photocatalytic performance of H production and CO reduction; however, until now, the direct synthesis of efficient Z-scheme photocatalysts remains a grand challenge. Herein, it is demonstrated that an interesting Z-scheme photocatalyst can be constructed by coupling In O and ZnIn Se semiconductors based on theoretical calculations. Experimentally, a class of ultrathin In O -ZnIn Se (denoted as In O -ZISe) spontaneous Z-scheme nanosheet photocatalysts for greatly enhancing photocatalytic H production is made. Furthermore, Mo atoms are incorporated in the Z-scheme In O -ZISe nanosheet photocatalyst by forming the MoSe bond, confirmed by X-ray photoelectron spectroscopy, in which the formed MoSe works as cocatalyst of the Z-scheme photocatalyst. As a consequence, such a unique structure of In O -ZISe-Mo makes it exhibit 21.7 and 232.6 times higher photocatalytic H evolution activity than those of In O -ZnIn Se and In O nanosheets, respectively. Moreover, In O -ZISe-Mo is also very stable for photocatalytic H production by showing almost no activity decay for 16 h test. Ultraviolet-visible diffuse reflectance spectra, photoluminescence spectroscopy, transient photocurrent spectra, and electrochemical impedance spectroscopy reveal that the enhanced photocatalytic performance of In O -ZISe-Mo is mainly attributed to its widened photoresponse range and effective carrier separation because of its special structure.
受自然光合作用的启发,设计新型 Z 型光催化体系对于提高光催化产氢和 CO 还原性能具有很大的应用前景;然而,到目前为止,高效 Z 型光催化剂的直接合成仍然是一个巨大的挑战。在此,通过理论计算证明,可以通过耦合 In O 和 ZnIn Se 半导体来构建有趣的 Z 型光催化剂。实验上,制备了一类超薄的 In O-ZnIn Se(表示为 In O-ZISe)自支撑 Z 型纳米片光催化剂,用于大大提高光催化产氢性能。此外,通过 X 射线光电子能谱证实,在 Z 型 In O-ZISe 纳米片光催化剂中形成了 MoSe 键,从而掺入 Mo 原子,其中形成的 MoSe 作为 Z 型光催化剂的助催化剂。结果,In O-ZISe-Mo 的这种独特结构使其光催化产氢活性分别比 In O-ZnIn Se 和 In O 纳米片提高了 21.7 倍和 232.6 倍。此外,In O-ZISe-Mo 对于光催化产氢也非常稳定,在 16 小时的测试中几乎没有活性衰减。紫外可见漫反射光谱、光致发光光谱、瞬态光电流谱和电化学阻抗谱表明,In O-ZISe-Mo 增强的光催化性能主要归因于其特殊结构引起的光响应范围拓宽和载流子有效分离。