Ionic liquid gating-induced defect passivation and enhanced photocatalytic performance in graphitic carbon nitride (g-C3N4) semiconductors.

IF 2.3 4区 物理与天体物理 Q3 PHYSICS, CONDENSED MATTER
Na Sa, Shanzhi Qu, Jinfeng Xu, Kaiqi Nie, Jia-Ou Wang, Junyong Kang, Jin-Cheng Zheng, Meng Wu, Shengli Huang, Hui-Qiong Wang
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Abstract

Ionic liquid gating (ILG) is an emergent technique for controlling multiple types of ionic doping and leads to numerous attractive physical properties in quantum materials. This study widens its intriguing applications in metal-free graphitic carbon nitride (g-C3N4) semiconductor which is distinct by various extrinsic defects (vacancies, interlayer defects, etc) and intrinsic defects (irregular melon chains, dangling bonds, etc.). Here, the efficient passivation of defects is realized in g-C3N4through combined electrostatic and electrochemical mechanisms. By optimizing the ionic liquid concentration and applying a negative electric field, the gated g-C3N4exhibit a changed local bonding environment, an increased bandgap, as well as a suppression of photoluminescence (PL) intensity over 80%. Our results demonstrate that the charged ions from the mixed electrolyte passivate the charged defect centers, redistribute the charges within the g-C3N4framework, leading to the improved photogenerated carries separation, which is verified by the enhanced photocatalytic efficiency of treated g-C3N4. In particular, the changes of the density of states near the Fermi level reflect ionic interaction induced defect passivation in g-C3N4, which plays a key role in regulating its PL properties. These findings provide novel insights in ILG mechanisms in layered porous materials and shed light on its potential prospects in other semiconductors with controlled defect engineering.

离子液体栅致缺陷钝化及增强石墨氮化碳(g-C₃N₄)半导体的光催化性能
离子液体门控(ILG)是一种新兴的控制多种类型离子掺杂的技术,它导致了量子材料中许多吸引人的物理性质。该研究扩大了其在无金属石墨氮化碳(g-C3N4)半导体中的有趣应用,该半导体具有各种外在缺陷(空位,层间缺陷等)和内在缺陷(不规则瓜链,悬空键等)。在这里,g-C3N4通过静电和电化学相结合的机制实现了缺陷的高效钝化。通过优化离子液体浓度和施加负电场,门控g-C3N4的局部成键环境发生改变,带隙增大,光致发光(PL)强度抑制80%以上。我们的研究结果表明,混合电解质中的带电离子钝化了带电缺陷中心,并在g-C3N4框架内重新分配了电荷,从而改善了光生载流子的分离,这一点通过处理后的g-C3N4的光催化效率得到了验证。特别是,在费米能级附近态密度的变化解决了g-C3N4在钝化缺陷和调节PL性能中的可能质子化作用。这些发现为层状多孔有机材料的ILG机制提供了新的见解,并揭示了其在其他有机半导体中具有控制缺陷工程的潜在前景。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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来源期刊
Journal of Physics: Condensed Matter
Journal of Physics: Condensed Matter 物理-物理:凝聚态物理
CiteScore
5.30
自引率
7.40%
发文量
1288
审稿时长
2.1 months
期刊介绍: Journal of Physics: Condensed Matter covers the whole of condensed matter physics including soft condensed matter and nanostructures. Papers may report experimental, theoretical and simulation studies. Note that papers must contain fundamental condensed matter science: papers reporting methods of materials preparation or properties of materials without novel condensed matter content will not be accepted.
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