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使用具有增强光催化析氢性能的氮掺杂碳对氮化碳助催化剂进行活化

Carbon Nitride Co-catalyst Activation Using N-Doped Carbon with Enhanced Photocatalytic H Evolution.

作者信息

Wang Jianhai, Zhou Qing, Shen Yanfei, Chen Xinghua, Liu Songqin, Zhang Yuanjian

机构信息

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.

出版信息

Langmuir. 2019 Sep 24;35(38):12366-12373. doi: 10.1021/acs.langmuir.9b01796. Epub 2019 Sep 11.

Abstract

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.

摘要

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。

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