Interfacial coupled engineering of plasmonic amorphous MoO3-x nanodots/g-C3N4 nanosheets for photocatalytic water splitting and photothermal conversion
Interfacial coupled engineering of plasmonic amorphous MoO3-x nanodots/g-C3N4 nanosheets for photocatalytic water splitting and photothermal conversion
复制标题
DOI：
10.1016/j.cej.2022.139875
复制
发表时间：
2022-10
影响因子：
15.1
通讯作者：
Yumei Ren;Desheng Feng;Zhiming Yan;Zixu Sun;Zixuan Zhang;Dongwei Xu;C. Qiao;Zhonghui Chen;Yu Jia;Seong Chan Jun;Shude Liu;Y. Yamauchi
中科院分区：
文献类型：
--
作者：
Yumei Ren;Desheng Feng;Zhiming Yan;Zixu Sun;Zixuan Zhang;Dongwei Xu;C. Qiao;Zhonghui Chen;Yu Jia;Seong Chan Jun;Shude Liu;Y. Yamauchi
基于半导体的等离子体激元材料在光催化体系中引起了广泛的关注。然而，它们的光催化反应受到有限的光捕获能力和光生电子的转移速率的阻碍。在此，空位工程和相工程被合理地整合，以开发锚定在g-C3 N4上的非晶氧化钼（a-MoO 3 −x）纳米点作为高活性的光催化剂。通过a-MoO 3 − x纳米点的高局域表面等离子体共振（LSPR）效应和异质结构界面诱导的可调电学性质，Z型a-MoO 3 −x/g-C3 N4异质结构表现出宽带吸收和激发的光生电子。进一步的理论计算表明，光催化和光热性能的增强主要归因于a-MoO 3-x的高度局域化的安德森尾态。因此，a-MoO 3 −x/g-C3 N4异质结构表现出的光电流密度为136.5 μA cm−2，分别比纯g-C3 N4纳米片（13.5 μA cm−2）和a-MoO 3 − x纳米点（199 μA cm−2）高出约2.7和4.1倍。探索了a-MoO 3 −xin Z-结构异质结缺陷和长程无序对光催化性能的增强作用。
Semiconductor-based plasmonic materials have attracted extensive attention for photocatalytic systems. However, their photocatalytic reactions are hindered by limited light-harvesting ability and the transfer rate of photo-generated electrons. Herein, vacancy engineering and phase engineering are rationally integrated to develop amorphous molybdenum oxide (a-MoO3−x) nanodots anchored on g-C3N4as a highly active photocatalyst. Through high localized surface plasmon resonance (LSPR) effect of a-MoO3−xnanodots and tunable electrical properties induced by the heterostructural interface, the Z-scheme a-MoO3−x/g-C3N4heterostructure demonstrates broadband absorption and the excited photo-generated electrons. Further theoretical calculations demonstrate that the enhancement of photocatalytic and photothermal performance is mainly attributed to the highly localized Anderson tail states of a-MoO3−x. Consequently, the a-MoO3−x/g-C3N4heterostructure exhibits a photocurrent density of ∼36.5 μA cm−2, which is about 2.7 and 4.1 times higher than that of pure g-C3N4nanosheets (∼13.5 μA cm−2) and a-MoO3−xnanodots (∼9 μA cm−2), respectively. The photocatalytic performance enhancement relying on defects and long-range disorder of a-MoO3−xin Z-scheme heterostructure is explored.