Wang Fang, Liu Tongliang, Liu Zhaoting, Zhang Zhengguo, Min Shixiong
School of Chemistry and Chemical Engineering, North Minzu University, Yinchuan, 750021, P. R. China.
Dalton Trans. 2022 Jul 26;51(29):11029-11039. doi: 10.1039/d2dt01402e.
Nanostructured H evolution cocatalysts are able to promote charge separation and thus enhance the efficiency of the photocatalytic H evolution reaction (HER). However, the nanosized cocatalyst particles are easily detached from the surfaces of semiconductors or severely aggregated in reaction systems, which not only greatly reduces the photocatalytic HER efficiency during long-term use but also greatly increases the difficulty of recovery. Moreover, powdery cocatalysts have poor compatibility with the scale-up photoelectrochemical devices. In this paper, a monolithic cocatalyst is developed by controllably growing NiP nanowire arrays on Ni foam substrate (NiP NWAs/NF) a direct vapor-phase phosphorization method. The grown NiP NWAs with high specific surface areas can not only offer ample active sites for the HER, but also serve as scaffolds for anchoring dye molecules to maximize the light utilization efficiency, which endows the NiP NWAs/NF monolithic cocatalyst with excellent HER activity. When sensitized with Erythrosin B (ErB) in triethanolamine (TEOA) solution, the turnover number (TON) of H evolution based on ErB reaches 9.7 in 5 h under visible light. Notably, the good structural integrity and inherent magnetism enable the NiP NWAs/NF to be easily separated from the reaction solution and excellent catalytic H evolution stability over a 45 h cycling reaction. This work presents a new strategy of fabricating monolithic cocatalysts with controllable microstructure and functionalities as well as high activity, durability, and device-compatibility for large-scale solar energy conversion applications.
纳米结构的析氢助催化剂能够促进电荷分离,从而提高光催化析氢反应(HER)的效率。然而,纳米尺寸的助催化剂颗粒很容易从半导体表面脱落,或者在反应体系中严重聚集,这不仅会在长期使用过程中大大降低光催化HER效率,还会大大增加回收难度。此外,粉末状助催化剂与放大规模的光电化学装置的兼容性较差。在本文中,通过直接气相磷化法在泡沫镍基底上可控生长NiP纳米线阵列(NiP NWAs/NF)来制备整体式助催化剂。生长的具有高比表面积的NiP NWAs不仅可以为HER提供充足的活性位点,还可以作为锚定染料分子的支架,以最大限度地提高光利用效率,这赋予了NiP NWAs/NF整体式助催化剂优异的HER活性。当在三乙醇胺(TEOA)溶液中用赤藓红B(ErB)敏化时,基于ErB的析氢周转数(TON)在可见光下5小时内达到9.7。值得注意的是,良好的结构完整性和固有磁性使NiP NWAs/NF能够很容易地从反应溶液中分离出来,并且在45小时的循环反应中具有出色的催化析氢稳定性。这项工作提出了一种制备具有可控微观结构和功能以及高活性、耐久性和与装置兼容性的整体式助催化剂的新策略,用于大规模太阳能转换应用。