内源性衍生物对碳点化学传感性能的影响OA北大核心
Study on Influence of Endogenous Derivatives on Chemical Sensing Performance of Carbon Dots
以间苯二胺和1,2,3-丙烷三甲酸为原料,采用气流辅助的熔融态聚合法和一步水热法分别合成了蓝色荧光碳点(TMCDs)和青绿色荧光碳点(TMCDs-H2O).气流吹扫能够有效地抑制副反应,减少产物碳点(CDs)中的衍生结构.通过液体核磁共振、质谱和透射电镜等表征技术对这两种材料的结构与形貌进行了表征.与TMCDs-H2O的平均粒径((3.12±0.63)nm)相比,TMCDs的平均粒径更小((1.85±0.02)nm).采用核磁共振与质谱分析两种CDs的化学结构,发现二者虽然主体结构相似,但是TMCDs的结构更简单,聚合度相对较高.这些结果表明,在TMCDs-H2O的颗粒中可能通过超分子相互作用引入了大量的小分子衍生物,因此表现出低聚合度、多亚结构和大粒径的特点.将两种CDs用于金属离子的化学传感时,线性范围为1×10-5~5×10-4 mol/L,TMCDs和TMCDs-H2O对Fe3+的检出限分别为3.3×10-6 mol/L和3.8×10-6 mol/L.对自来水实际样品进行加标回收实验,结果表明,两种CDs的回收率相差不大,并且均与ICP-OES的回收率相近,但TMCDs的相对标准偏差较大.本研究结果表明,CDs中的内源性衍生结构可以提高其对金属离子的传感检测性能.
The blue fluorescent carbon dots(TMCDs)and cyan fluorescent carbon dots(TMCDs-H2O)were synthesized fromm-phenylenediamine and tricarballylic acid through air-assisted melting polymerization and one-step hydrothermal method,respectively.Air purging could effectively inhibit the side reactions and reduce the derivative structures in the carbon dots product.The structure and morphology of these two materials were systematically characterized using liquid nuclear magnetic resonance spectroscopy(NMR),mass spectrometry(MS),and transmission electron microscopy.Compared to TMCDs-H2O((3.12±0.63)nm),TMCDs showed a smaller average particle size(approximately(1.85±0.02)nm).The NMR and MS analysis revealed that although the main structure of both types of carbon dots was similar,TMCDs exhibited a simpler structure with higher degree of polymerization.These results suggested that supramolecular interactions might introduce numerous small molecule derivatives into TMCDs-H2O particles,resulting in lower polymerization degree,multiple substructures,and larger particle size characteristics for this material.When employed as chemical sensors for metal ion detection,in the linear range of 1×10-5-5×10-4 mol/L,the detection limits of Fe3+by TMCDs and TMCDs-H2O were 3.3×10-6 mol/L and 3.8×10-6 mol/L,respectively.The experimental results demonstrated that the recoveries of CDs and inductively coupled plasma optical emission spectrometer(ICP-OES)were similarity,whereas TMCDs displayed a considerable relative standard deviation.This study demonstrated that endogenously derived structures in CDs could enhance the performance of metal ion sensing.
覃迎喜;王昱;杨莉花;刘紫薇;覃爱苗;冯亮
桂林理工大学材料科学与工程学院,桂林 541004||中国科学院大连化学物理研究所,分离分析化学中国科学院重点实验室,大连 116023中国科学院大连化学物理研究所,分离分析化学中国科学院重点实验室,大连 116023桂林理工大学材料科学与工程学院,桂林 541004||中国科学院大连化学物理研究所,分离分析化学中国科学院重点实验室,大连 116023中国科学院大连化学物理研究所,分离分析化学中国科学院重点实验室,大连 116023桂林理工大学材料科学与工程学院,桂林 541004中国科学院大连化学物理研究所,分离分析化学中国科学院重点实验室,大连 116023
内源性衍生物碳点化学传感金属离子检测Fe3+传感机理
Endogenous derivativesCarbon dotsChemical sensingDetection of metal ionFe3+sensing mechanism
《分析化学》 2025 (1)
94-103,10
中国科学院青年创新促进会项目(No.2020185)、中国科学院大连清洁能源国家实验室榆林分院人工智能科技计划(No.DNL-YL A202203)、国家自然科学基金项目(No.22122307)和广西自然科学基金项目(No.2018JJA160029)资助. Supported by the Youth Innovation Promotion Association of Chinese Academy of Sciences(No.2020185),the AI S&T Program of Yulin Branch,Dalian National Laboratory for Clean Energy,CAS(No.DNL-YL A202203),the National Natural Science Foundation of China(No.22122307)and the Natural Science Foundation of Guangxi(No.2018JJA160029).
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