Yan Chenyu, Tang Zheng, Wang Linjie, Piao Zhe, Wang Honggui, Zhang Ya
School of Environmental Science and Engineering, Yangzhou University, Yangzhou, Jiangsu 225127, China.
Langmuir. 2024 Jun 18;40(24):12427-12436. doi: 10.1021/acs.langmuir.4c00679. Epub 2024 May 28.
In recent years, increasing attention has been paid to photoelectrochemical (PEC) hydrogen production owing to the utilization of sustainable solar energy and its promising performance. Silicon-based composites are generally considered ideal materials for PEC hydrogen production. However, slow reaction kinetics and poor stability are still key factors hindering the development of silicon-based photoelectrocatalysts. Herein, we present an n-p Si pyramidal photocathode assembly method to load reduced graphene oxide (rGO) onto the surface of the n-p Si pyramid by covalently linking (Si/rGO). rGO is utilized as a conductive layer to reduce the interfacial charge-transfer resistance. Then, MoS can be successfully electrodeposited on the surface of Si/rGO to form the Si/rGO/MoS composite, which possesses excellent PEC hydrogen evolution performance with a high and stable photocurrent of -41.6 mA cm and a hydrogen evolution rate of about 18.1 μmol min cm under 0 V (vs RHE). The covalently linking rGO layer effectively enhances the transfer of photogenerated carriers between the Si substrate and MoS. MoS provides abundant hydrogen evolution active sites, which accelerate the surface reaction kinetics, as well as a protective layer for the Si pyramidal array structure. This work provides a low-cost, convenient, and efficient way of preparing silicon-based photocathodes.
近年来,由于可持续太阳能的利用及其良好的性能,光电化学(PEC)制氢受到了越来越多的关注。硅基复合材料通常被认为是PEC制氢的理想材料。然而,缓慢的反应动力学和较差的稳定性仍然是阻碍硅基光催化剂发展的关键因素。在此,我们提出一种n-p硅金字塔光阴极组装方法,通过共价连接(Si/rGO)将还原氧化石墨烯(rGO)负载到n-p硅金字塔表面。rGO用作导电层以降低界面电荷转移电阻。然后,可以在Si/rGO表面成功电沉积MoS,形成Si/rGO/MoS复合材料,该复合材料具有优异的PEC析氢性能,在0 V(相对于可逆氢电极)下具有-41.6 mA cm的高且稳定的光电流和约18.1 μmol min cm的析氢速率。共价连接的rGO层有效地增强了光生载流子在硅基底和MoS之间的转移。MoS提供了丰富的析氢活性位点,加速了表面反应动力学,同时也为硅金字塔阵列结构提供了一层保护。这项工作提供了一种低成本、便捷且高效的制备硅基光阴极的方法。