Mandal Tuhin, Ghosh Ashish Kumar, Mishra Shiv Rag, Pandey Sarvesh Kumar, Singh Vikram
Environment Emission and CRM Section, CSIR-Central Institute of Mining and Fuel Research Dhanbad Jharkhand 828108 India
Coal Quality and Value Addition Division, CSIR-Central Institute of Mining and Fuel Research Dhanbad Jharkhand 828108 India.
Nanoscale Adv. 2023 Jul 18;5(16):4269-4285. doi: 10.1039/d3na00289f. eCollection 2023 Aug 8.
Herein, blue-emitting carbon nanoparticles (CNPs) were synthesized using the flower for the highly selective and sensitive detection of Cr ions in aqueous media using a simple, green, and cost-effective approach, and computational experiments were also performed. The prepared CNPs were well-dispersed in water with an average diameter of 12 nm and functionalized with carbonyl, hydroxyl and carboxylic acid groups. The decrease in the fluorescence intensity of the CNPs with an increase in the content of Cr provided an important signal for the sensitive and selective detection of Cr in aqueous media. The limit of detection for Cr in an aqueous medium was found to be 103 ppb, which is more sensitive in comparison with the previously reported study. Furthermore, the validation of the proposed higher sensing feature and more selective nature of the CNPs towards Cr was also explained using an approach. The results from the theoretical calculations based on the DFT approach demonstrated that the binding energy (BE) of the CNPs with three transition metal (TM) cations (Cr, Fe, and Hg) follows the order of Cr > Fe > Hg, where the Cr TM cation associated with the CNPs possesses the highest valence state, showing the highest sensing feature and highest selectivity among the investigated ions, as expected. The metal ions associated with the CNPs having a higher charge and a smaller radius indicated a higher BE and larger degree of deformation of the CNPs. Moreover, to achieve new insights into the structural, stability/energetics, and electronic features, some useful tools, such as NCI-plot, HOMO-LUMO gap, MESP, and QTAIM analysis were employed, which facilitated noteworthy outcomes.
在此，使用花朵合成了发蓝光的碳纳米颗粒（CNPs），采用简单、绿色且经济高效的方法在水性介质中对Cr离子进行高选择性和灵敏检测，并且还进行了计算实验。制备的CNPs在水中分散良好，平均直径为12 nm，并被羰基、羟基和羧酸基团官能化。随着Cr含量增加，CNPs荧光强度降低，这为在水性介质中灵敏且选择性地检测Cr提供了重要信号。发现水性介质中Cr的检测限为103 ppb，与先前报道的研究相比更灵敏。此外，还使用一种方法解释了所提出的CNPs对Cr具有更高传感特性和更高选择性的验证。基于密度泛函理论（DFT）方法的理论计算结果表明，CNPs与三种过渡金属（TM）阳离子（Cr、Fe和Hg）的结合能（BE）遵循Cr > Fe > Hg的顺序，其中与CNPs相关的Cr TM阳离子具有最高价态，在所研究的离子中显示出最高的传感特性和最高的选择性，正如预期的那样。与CNPs相关的电荷更高且半径更小的金属离子表明CNPs具有更高的BE和更大程度的变形。此外，为了深入了解结构、稳定性/能量学和电子特性，采用了一些有用的工具，如NCI-plot、HOMO-LUMO能隙、分子静电势（MESP）和量子拓扑原子分子理论（QTAIM）分析，这些都促成了显著的成果。
