氮化碳接枝L-谷氨酰胺分子实现高效光催化产氢和降解性能

doi:10.16085/j.issn.1000-6613.2023-0191

摘要/Abstract

摘要：

将尿素和L-谷氨酰胺（Lg）作为前体材料，使用冷冻-煅烧法成功将Lg分子链接枝到了氮化碳（CN）的边缘，制备了具有优异光催化性能Lg接枝修饰的多孔氮化碳（LCN）光催化剂。通过X射线衍射光谱（XRD）、扫描电子显微镜（SEM）、傅里叶变换红外光谱（FTIR）、X射线光电子能谱（XPS）等表征测试方法对样品的形貌结构以及光催化性能进行了测试。结果表明，Lg分子链的引入不仅能够增加材料的比表面积，提供更多的活性位点，同时还可以有效促进光生电子的快速分离和转移，从而获得优异的光催化活性。在可见光的照射下，最优质量比的LCN-10光催化剂在析氢测试过程中产氢速率高达658µmol/(g·h)，约是纯相CN的3倍。并且在光降解盐酸四环素（TCH）和左氧氟沙星（LEV）的测试中，LCN-10也表现出良好的催化活性，在60min内对TCH和LEV的光降解率达到了98%及85%。这项工作为CN基光催化材料的表面修饰与性能优化提供了新的视角。

关键词: 光催化, 制氢, 降解, 氮化碳, L-谷氨酰胺

Abstract:

Using urea and L-glutamine (Lg) as precursor materials, Lg molecules were successfully linked to the edge of carbon nitride (CN) by freezing-calcination method, and Lg grafted porous carbon nitride (LCN) photocatalysts with excellent photocatalytic performance were prepared. The morphological structure and photocatalytic performance of the samples were tested by X-ray spectroscopy (XRD), scanning electron microscopy (SEM), Fourier transform infrared spectroscopy (FTIR) and X-ray photoelectron spectroscopy (XPS). The results showed that the introduction of Lg molecular chains could not only increase the specific surface area of the material and provide more active sites, but also effectively promote the rapid separation and transfer of photogenerated electrons, resulting in excellent photocatalytic activity. Under visible light irradiation, the hydrogen formation rate of LCN-10 photocatalyst with the optimal mass ratio during hydrogen evolution test was up to 658µmol/(g·h), about 3 times higher than that of pure phase CN. LCN-10 also indicated good catalytic activity in photodegradation tests of tetracycline hydrochloride (TCH) and levofloxacin (LEV), achieving 98% as well as 85% photodegradation of TCH and LEV within 60min. This work provided a new perspective on the surface modification and performance optimization of CN-based photocatalytic materials.

Key words: photocatalysis, hydrogen production, degradation, carbon nitride, L-glutamine

中图分类号:

刘飞, 陈哲, 陈峰. 氮化碳接枝L-谷氨酰胺分子实现高效光催化产氢和降解性能[J]. 化工进展, 2023, 42(12): 6372-6382.

LIU Fei, CHEN Zhe, CHEN Feng. Carbon nitride grafting of L-glutamine molecules for boosting the photocatalytic H₂ production and degradation activity[J]. Chemical Industry and Engineering Progress, 2023, 42(12): 6372-6382.

图/表 15

表1 LCN光催化剂不同配比用量

样品	尿素/g	L-谷氨酰胺/mg	水/mL
LCN-5	5	5	10
LCN-10	5	10	10
LCN-30	5	30	10
LCN-50	5	50	10

图1 样品FTIR光谱

图2 不同样品的XRD图以及局部放大图

图3 LCN-10样品的SEM、TEM以及元素Mapping图

图4 样品的XPS测试结果

图5 CN及LCN-10的BET测试结果

图6 样品析氢性能测试以及LCN-10析氢稳定性能测试结果

图7 TCH和LEV的降解曲线及动力学拟合曲线

图8 不同温度以及不同水质下LCN-10样品对TCH的降解性能

图9 UV-vis吸收光谱以及样品的Tauc图

图10 样品不同频率下的莫特肖特基曲线、XPS价带谱切线以及能带结构

图11 自由基捕获实验以及电化学测试

图12 样品光致发光光谱和时间分辨光致发光光谱

表2 CN及LCN-10样品瞬态荧光寿命

样品	常数A₁	指数成分寿命τ₁/ns	A₁τ₁/ns	常数A₂	指数成分寿命τ₂/ns	A₂τ₂/ns	τ_a/ns
CN	2306.23	0.86	2001.81	956.80	3.69	3530.61	2.07
LCN	2346.58	1.75	4106.51	955.18	6.42	6132.29	3.70

图13 LCN-10光催化机理

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