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硫/磷掺杂介导的氮化碳从棒状到具有优异光催化活性的多孔微管的形貌转变。

Sulfur/phosphorus doping-mediated morphology transformation of carbon nitride from rods to porous microtubes with superior photocatalytic activity.

作者信息

Jiao Yingying, Liu Mingquan, Qin Junchao, Li Yike, Wang Jianshe, He Zhanhang, Li Zhongjun

机构信息

College of Chemistry, Zhengzhou University, Zhengzhou 450001, PR China.

College of Chemistry, Zhengzhou University, Zhengzhou 450001, PR China.

出版信息

J Colloid Interface Sci. 2022 Feb 15;608(Pt 2):1432-1440. doi: 10.1016/j.jcis.2021.10.084. Epub 2021 Oct 20.

Abstract

Hetero-atoms doping or morphology controlling of carbon nitride (g-CN) can availably regulate its electronic band structure and optimize photocatalytic performance under visible light. Herein, sulful (S), phosphorus (P) co-doped porous carbon nitride microtubes (SPCN) was synthesized by using ammonium dihydrogen phosphate and melamine as precursors, in which ammonium dihydrogen phosphate can not only control the morphology of carbon nitride from nanorods to porous microtubes, but also provide a potential P source for P-doped CN. The prepared SPCN0.1 with the content of 0.1 g ammonium dihydrogen phosphate displayed the highest photocatalytic hydrogen generation rate of 4200.3 µmol gh, which was approximately 25 and 1.6 folds by bulk g-CN (CN) and sulphur doped g-CN microrods (SCN), respectively. Moreover, the apparent quantum efficiency of HER reached up to 10.3 % at 420 nm. The enhanced photocatalytic performance may be attributed to the synergistic effect of S, P doping and morphology structure of carbon nitride, which effectively accelerated the separation and transfer of photogenerated electron-hole pairs, proved by photoluminescence spectra, time-resolved PL spectra, electrochemical impedance spectrum and transient photocurrent responses. The novel synthetic method described in this paper is an effective approach to regulate the morphology of g-CNvia non-metal doping with superior photocatalytic performance.

摘要

对氮化碳(g-CN)进行杂原子掺杂或形貌调控能够有效调节其电子能带结构,并优化其在可见光下的光催化性能。在此,以磷酸二氢铵和三聚氰胺为前驱体合成了硫(S)、磷(P)共掺杂的多孔氮化碳微管(SPCN),其中磷酸二氢铵不仅能将氮化碳的形貌从纳米棒调控为多孔微管,还能为P掺杂的CN提供潜在的P源。制备的含有0.1 g磷酸二氢铵的SPCN0.1表现出最高的光催化产氢速率,为4200.3 μmol g h,分别约为体相g-CN(CN)和硫掺杂g-CN微棒(SCN)的25倍和1.6倍。此外,在420 nm处HER的表观量子效率高达10.3%。光催化性能的增强可能归因于S、P掺杂与氮化碳形貌结构的协同效应,这有效地加速了光生电子-空穴对的分离和转移,光致发光光谱、时间分辨PL光谱、电化学阻抗谱和瞬态光电流响应证明了这一点。本文所述的新型合成方法是一种通过非金属掺杂调控g-CN形貌并具有优异光催化性能的有效途径。

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