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用于高效光催化产氢并同时降解抗生素的非晶态/晶态石墨相氮化碳同质结的静电自组装合成

Electrostatic Self-Assembled Synthesis of Amorphous/Crystalline g-CN Homo-Junction for Efficient Photocatalytic H Production with Simultaneous Antibiotic Degradation.

作者信息

Pan Yilin, Qiao Kai, Ning Chuangyu, Wang Xin, Liu Zhiquan, Chen Zhihong

机构信息

Key Laboratory for Water Quality and Conservation of the Pearl River Delta, Guangzhou University, Guangzhou 511370, China.

International Academy of Optoelectronics at Zhaoqing, South China Normal University, Liyuan Street, Zhaoqing 526238, China.

出版信息

Nanomaterials (Basel). 2023 Nov 17;13(22):2964. doi: 10.3390/nano13222964.

Abstract

g-CN has been regarded as a promising photocatalyst for photo-reforming antibiotics for H production but still suffers from its high charge recombination, which has been proven to be solvable by constructing a g-CN homo-junction. However, those reported methods based on uncontrollable calcination for preparing a g-CN homo-junction are difficult to reproduce. Herein, an amorphous/crystalline g-CN homo-junction (ACN/CCN) was successfully synthesized via the electrostatic self-assembly attachment of negatively charged crystalline g-CN nanorods (CCN) on positively charged amorphous g-CN sheets (ACN). All the ACN/CCN samples displayed much higher photo-reforming of antibiotics for H production ability than that of pristine ACN and CCN. In particular, ACN/CCN-2 with the optimal ratio exhibited the best photocatalytic performance, with a H evolution rate of 162.5 μmol·g·h and simultaneous consecutive ciprofloxacin (CIP) degradation under light irradiation for 4 h. The UV-vis diffuse reflectance spectra (DRS), photoluminescence (PL), and electrochemical results revealed that a homo-junction is formed in ACN/CCN due to the difference in the band arrangement of ACN and CCN, which effectively suppressed the charge recombination and then led to those above significantly enhanced photocatalytic activity. Moreover, H was generated from the water reduction reaction with a photogenerated electron (e), and CIP was degraded via a photogenerated hole (h). ACN/CCN exhibited adequate photostability and reusability for photocatalytic H production with simultaneous CIP degradation. This work provides a new idea for rationally designing and preparing homo-junction photocatalysts to achieve the dual purpose of chemical energy production and environmental treatment.

摘要

石墨相氮化碳(g-CN)被认为是一种有前途的光催化剂,可用于光重整抗生素以制氢,但仍存在高电荷复合问题,已证明通过构建g-CN同质结可解决该问题。然而,那些基于不可控煅烧制备g-CN同质结的报道方法难以重现。在此,通过带负电荷的结晶g-CN纳米棒(CCN)在带正电荷的非晶g-CN片(ACN)上的静电自组装附着,成功合成了非晶/结晶g-CN同质结(ACN/CCN)。所有ACN/CCN样品在光重整抗生素制氢能力方面均比原始ACN和CCN高得多。特别是,具有最佳比例的ACN/CCN-2表现出最佳的光催化性能,在光照4小时下,析氢速率为162.5 μmol·g·h,同时可连续降解环丙沙星(CIP)。紫外-可见漫反射光谱(DRS)、光致发光(PL)和电化学结果表明,由于ACN和CCN能带排列的差异,ACN/CCN中形成了同质结,有效抑制了电荷复合,进而导致上述光催化活性显著增强。此外,H是由光生电子(e)参与的水还原反应产生的,CIP是通过光生空穴(h)降解的。ACN/CCN在同时降解CIP的光催化制氢过程中表现出足够的光稳定性和可重复使用性。这项工作为合理设计和制备同质结光催化剂以实现化学能源生产和环境治理的双重目的提供了新思路。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/b720/10675752/99fcc779c154/nanomaterials-13-02964-g001.jpg

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