Improving Charge Carrier Separation through S-Scheme-Based 2D–2D WS2/Sulfur-Doped g-C3N4 Heterojunctions for a Superior Photocatalytic O2 Reduction Reaction

IF 5.4 3区 材料科学 Q2 CHEMISTRY, PHYSICAL
Kundan Kumar Das, Upali Aparajita Mohanty, Ritik Mohanty, Preeti Prabha Sarangi, Dipti Prava Sahoo and Kulamani Parida*, 
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Abstract

Hydrogen peroxide (H2O2) generation via a photocatalytic O2 reduction reaction has been considered an economically efficient and environmentally friendly synthesis method. However, the productivity of H2O2 production is restricted because of sluggish reaction kinetics and fast recombination of photoinduced excitons. Therefore, a superior two-dimensional (2D)–2D WS2/sulfur-doped g-C3N4 (WSCN) hybrid material was successfully fabricated to address the associated limitations through a combination of wet impregnation and calcination techniques for H2O2 production. The effective anchoring of WS2 nanoplates onto sulfur-doped g-C3N4 (SCN) nanosheets facilitates effective separation of photoinduced excitons with sturdy redox properties, which is attributable to the establishment of S-scheme heterojunctions between WS2 and SCN through W–S bonding as substantiated by X-ray photoelectron spectroscopy (XPS) analysis. The W–S bond at the interface acts as a bridge for effective charge segregation pathways. Among all, 2.5 WSCN displays an exceptional H2O2 production of 817 μmol, which was 7.9- and 2.68-fold higher than those of pristine WS2 and SCN, respectively. The solar-to-chemical conversion efficiency was found to be 0.24%, whereas the apparent quantum yield was estimated to be 3.19% at 420 nm irradiation. The improved photocatalytic activity was figured out by a higher cathodic photocurrent of −1.51 mA cm–2 and delayed recombination of excitons, as supported by photoluminescence and electrochemical impedance spectroscopy measurements. The S-scheme charge-transfer pathway was well validated by a radical scavenging experiment and work function, which was evaluated from VB-XPS analysis and in situ XPS measurement. This research offers a paradigmatic idea for constructing an S-scheme photocatalyst for H2O2 generation.

Abstract Image

通过基于 S-Scheme 的 2D-2D WS2/掺硫 g-C3N4 异质结改善电荷载流子分离,实现卓越的光催化氧气还原反应
通过光催化氧化还原反应生成过氧化氢(H2O2)一直被认为是一种经济高效且环保的合成方法。然而,由于反应动力学迟缓以及光诱导激子的快速重组,H2O2 的生产率受到了限制。因此,为了解决相关的局限性,我们通过湿法浸渍和煅烧技术相结合的方法,成功制备了一种优异的二维(2D)-2D WS2/掺硫 g-C3N4 (WSCN)杂化材料,用于生产 H2O2。WS2 纳米板有效地锚定在掺硫 g-C3N4 (SCN) 纳米片上,促进了光诱导激子的有效分离,并具有坚固的氧化还原特性,这归功于 WS2 和 SCN 之间通过 W-S 键建立的 S 型异质结,X 射线光电子能谱 (XPS) 分析证实了这一点。界面上的 W-S 键充当了有效电荷隔离途径的桥梁。其中,2.5 WSCN 的 H2O2 生成量高达 817 μmol,分别是原始 WS2 和 SCN 的 7.9 倍和 2.68 倍。在 420 纳米波长的照射下,太阳能到化学物质的转化效率为 0.24%,而表观量子产率估计为 3.19%。光致发光和电化学阻抗光谱测量结果表明,阴极光电流为 -1.51 mA cm-2,激子延迟重组,从而提高了光催化活性。通过自由基清除实验和功函数,以及 VB-XPS 分析和原位 XPS 测量评估,S 型电荷转移途径得到了很好的验证。这项研究为构建用于生成 H2O2 的 S 型光催化剂提供了一个范例。
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来源期刊
ACS Applied Energy Materials
ACS Applied Energy Materials Materials Science-Materials Chemistry
CiteScore
10.30
自引率
6.20%
发文量
1368
期刊介绍: ACS Applied Energy Materials is an interdisciplinary journal publishing original research covering all aspects of materials, engineering, chemistry, physics and biology relevant to energy conversion and storage. The journal is devoted to reports of new and original experimental and theoretical research of an applied nature that integrate knowledge in the areas of materials, engineering, physics, bioscience, and chemistry into important energy applications.
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