Wang Yuhong, Jiang Wenjun, Yao Wei, Liu Zailun, Liu Zhe, Wang Yajun, Shi Lijie, Gao Lizhen
College of Environmental Science and Engineering, Taiyuan University of Technology, Taiyuan 030024, PR China; Qian Xuesen Laboratory of Space Technology, China Academy of Space Technology, 104 Youyi Road, Beijing 100094, PR China.
Qian Xuesen Laboratory of Space Technology, China Academy of Space Technology, 104 Youyi Road, Beijing 100094, PR China.
J Colloid Interface Sci. 2021 May 15;590:144-153. doi: 10.1016/j.jcis.2021.01.043. Epub 2021 Jan 21.
Addressing the inherent holes transport limitation of BiVO photoanode is crucial to achieve efficient photoelectrochemical (PEC) water splitting. The construction of the hole-transfer bridge between co-catalysts and BiVO photoanode could be an effective way to overcome sluggish hole-transfer kinetics of BiVO photoanode. Herein, CN/BiVO photoanode was prepared by coupling carbon nitride hydrogel (CNH) containing unsaturated N on the BiVO photoanode during annealing. CN/BiVO photoanode exhibited excellent PEC performance and stability. Photoelectrochemical tests proved that the coupling of CN accelerated holes transfer and enhanced oxygen evolution kinetics. X-ray photoelectron spectroscopy (XPS) and theoretical calculations confirmed the existence of the BiNV bond between BiVO photoanode and CN, which could serve as the hole-transfer bridge to significantly accelerate separation and transfer of carriers driven by the interfacial electric field. Moreover, it was found that the coupling of CN effectively inhibited the dissociation of metal ions through changing their coordination environment, resulting in the excellent stability of CN/BiVO photoanode. This result provides unique insights into vital roles of the interfacial structure, which might have a significant impact on the construction of PEC devices.
解决BiVO光阳极固有的空穴传输限制对于实现高效的光电化学(PEC)水分解至关重要。在共催化剂与BiVO光阳极之间构建空穴传输桥可能是克服BiVO光阳极缓慢的空穴转移动力学的有效方法。在此,通过在退火过程中将含有不饱和N的氮化碳水凝胶(CNH)耦合到BiVO光阳极上来制备CN/BiVO光阳极。CN/BiVO光阳极表现出优异的PEC性能和稳定性。光电化学测试证明,CN的耦合加速了空穴转移并增强了析氧动力学。X射线光电子能谱(XPS)和理论计算证实了BiVO光阳极与CN之间存在Bi-N键,其可作为空穴传输桥,显著加速由界面电场驱动的载流子的分离和转移。此外,发现CN的耦合通过改变金属离子的配位环境有效地抑制了金属离子的解离,从而导致CN/BiVO光阳极具有优异的稳定性。该结果为界面结构的重要作用提供了独特的见解,这可能对PEC器件的构建产生重大影响。