Enhancement of photocatalytic H2 evolution on pyrene-based polymer promoted by MoS2 and visible light
Enhancement of photocatalytic H2 evolution on pyrene-based polymer promoted by MoS2 and visible light
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DOI：
10.1016/j.apcatb.2019.03.061
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发表时间：
2019-08
期刊：
影响因子：
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通讯作者：
Shaohong Zang;Guigang Zhang;Zhi‐An Lan;Dandan Zheng;Xinchen Wang
中科院分区：
文献类型：
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作者：
Shaohong Zang;Guigang Zhang;Zhi‐An Lan;Dandan Zheng;Xinchen Wang
共轭聚合物由于其优异的性能，如优化灵活性，成本效益和强大的稳定性，在聚合物中引起了特别的兴趣。芘基聚合物（PyP）作为共轭聚合物的一种，由于其合适的能带结构、可见光吸收和高比表面积，具有很大的水裂解潜力。然而，由于快速电荷载流子复合受到具有高激子结合能的弗伦克尔激子的限制，原始形式的PyP对于光催化析氢几乎没有活性。简洁的异质结结构是加速电荷分离、提高光生e−/h+对寿命、降低析氢反应活化能垒的可行途径。在这项工作中，一系列的过渡金属硫化物作为助催化剂已被沉积在PyP构建异质结的光催化析氢反应（HER）。考察了助催化剂的负载技术（浸渍法、原位法和光沉积法）和负载量。优化的MoS 2/PyP样品与未经修饰的纯PyP相比表现出10倍的增加。扩展的π-共轭、高表面积和广泛暴露的2D界面突出了PyP作为稳定均匀分散的MoS 2的有效载体的重要性，从而产生有效的光催化活性。该研究为构建低成本、可持续、高效的光催化制氢复合系统提供了新的思路。
Conjugated polymers have gathered particular interests in photocatalysis because of their excellent properties such as optimization flexibility, cost-effective, and robust stability. The pyrene-based polymer (PyP), as one of the conjugated polymers, holds a great potential for water splitting because of their suitable band structure, visible light absorption, and high surface area. However, because of the fast charge carrier recombination confined by Frenkel excitons with high exciton binding energy, PyP in its pristine form remains barely active for photoctalytic hydrogen evolution. The concise construction of heterojunction is a feasible way to accelerate the charge separation, increase the lifetime of the photogenerated e−/h+pair and decrease the activation barriers of hydrogen evolution reaction. In this work, a series of transition metal sulfides as cocatalysts have been deposited on PyP to construct heterojunctions for photocatalytic H2evolution reaction (HER). The loading techniques (immersion, in-situ and photodeposition) and the loading contents of cocatalysts have been investigated. The optimized MoS2/PyP sample exhibited a 10-fold increase in comparison with pure PyP without modification. The extended π-conjugation, high surface area, and widely exposed 2D interface highlight the importance of PyP as effective supports for stabilizing the homogeneously dispersed MoS2, thereby resulting in an efficient photocatalytic activity. This study provides a new idea to construct low-cost, sustainable and efficient hybrid system for photocatalytic hydrogen production.