Wang Jianhai, Zhou Qing, Shen Yanfei, Chen Xinghua, Liu Songqin, Zhang Yuanjian
Jiangsu Engineering Laboratory of Smart Carbon-Rich Materials and Device, Jiangsu Province Hi-Tech Key Laboratory for Bio-Medical Research, School of Chemistry and Chemical Engineering, Medical School , Southeast University , Nanjing 211189 , China.
Langmuir. 2019 Sep 24;35(38):12366-12373. doi: 10.1021/acs.langmuir.9b01796. Epub 2019 Sep 11.
Photocatalytic water splitting holds huge potential to meet the current challenges of energy and environments. Among them, polymeric carbon nitride (CN) has drawn much attention as a promising metal-free photocatalyst. As it is known, a number of promising co-catalysts have been developed to improve catalytic reactions, Pt nanoparticles is still among the best co-catalysts for CN in photocatalytic H evolution, due to the suitable Fermi level to transfer excited electrons and the low overpotential for H reduction. Herein, we report the interface engineering of urea-derived bulk CN and Pt co-catalyst by using a small portion of N-doped carbon (N-C) as a transition layer with a boosted photocatalytic activity up to 7 times. It was revealed that the activation energy of the Pt co-catalyst for water reduction was lowered in the presence of N-C, and the intimate interaction between CN and N-C, ascribing to the similar elemental composition and crystal structure, promoted the efficient separation and migration of charge carriers. This study may open a new avenue to develop CN-based photocatalysts for solar fuel conversion with even higher activity by photocatalyst/co-catalyst interface engineering.
光催化水分解在应对当前能源和环境挑战方面具有巨大潜力。其中，聚合氮化碳（CN）作为一种有前景的无金属光催化剂备受关注。众所周知，人们已开发出多种有前景的助催化剂来改善催化反应，由于其具有适合转移激发电子的费米能级以及较低的析氢过电位，铂纳米颗粒仍是光催化析氢反应中CN的最佳助催化剂之一。在此，我们报道了通过使用一小部分氮掺杂碳（N-C）作为过渡层对尿素衍生的块状CN和Pt助催化剂进行界面工程，光催化活性提高了7倍。结果表明，在N-C存在下，Pt助催化剂用于水还原的活化能降低，并且由于元素组成和晶体结构相似，CN与N-C之间的紧密相互作用促进了电荷载流子的有效分离和迁移。这项研究可能为通过光催化剂/助催化剂界面工程开发具有更高活性的用于太阳能燃料转化的CN基光催化剂开辟一条新途径。
