المجلة: Scientific Reports، المجلد: 14، العدد: 1
DOI: https://doi.org/10.1038/s41598-024-52688-y
PMID: https://pubmed.ncbi.nlm.nih.gov/38280908
تاريخ النشر: 2024-01-27
DOI: https://doi.org/10.1038/s41598-024-52688-y
PMID: https://pubmed.ncbi.nlm.nih.gov/38280908
تاريخ النشر: 2024-01-27
تحلل ضوئي فعال للملوثات الصبغية النسيجية باستخدام نيتريد الكربون الجرافيتي المعرض للحرارة (TE–g–C3N4)
نيتريد الكربون الجرافيتي
في السنوات الأخيرة، ساهمت العولمة، وتقدم التكنولوجيا، إلى جانب تطور تفضيلات الموضة لدى البشر، بشكل كبير في زيادة تصنيع المنسوجات والملابس.
تشير التقارير إلى أن الأصباغ السامة تسبب التهابات الجهاز التنفسي، وتهيج الجلد، وتهيج العينين.
نيتريد الكربون الجرافيتي
عملية التقشير الحراري لـ
قسم المواد التجريبية
ميلامين
الشكل 1. مخطط يوضح إعداد
أوكسالات
تركيب
تحضير الكمية الكبيرة
الجزء الأكبر
الجزء الأكبر
إعداد
تي-إي-جي-سي3
تي-إي-جي-سي3
توصيف
تم استخدام اختبارات حيود الأشعة السينية (XRD) للتحقق من إنتاج ونقاء المواد المُركبة باستخدام جهاز باناليتيكال X’Pert.
تجارب التحفيز الضوئي
النشاط الضوئي المحفز لـ TE-g-C
تم تقييم نسبة التحلل لكل صبغة وثابت معدل تفاعل المحفز الضوئي باستخدام المعادلات التالية.
أين،
القياسات الكهروكيميائية
تم إجراء تحليل موت-شوتكي لتأكيد قيمة نطاق التوصيل. باستخدام
النتائج والمناقشة
نتائج حيود الأشعة السينية البودرة
شكل 2أ أظهر نمط حيود الأشعة السينية لجميع العينات المحضرة
شكل 2أ أظهر نمط حيود الأشعة السينية لجميع العينات المحضرة
الشكل 2. (أ) نتائج حيود الأشعة السينية للمواد المسحوقة
ترتيب حلقات التري-س-ترازاين والتكرار الدوري لوحدات الهيبتازين داخل المستوى، على التوالي. أظهرت العينات التي تم تقشيرها حرارياً قممًا أوسع مع انخفاض في الشدة مقارنةً بنظيراتها الكتلية، مما قد يعكس تقليل المسافة بين الطبقات في العينات المقشرة.
تحليل FTIR
تمت دراسة المجموعات الوظيفية والترابط الكيميائي للمواد المحضرة بواسطة مطيافية الأشعة تحت الحمراء بتحويل فورييه (FTIR)، كما هو موضح في الشكل 2b. هنا، تمتلك جميع العينات المحضرة طيفًا مميزًا مشابهًا.
تحليل XPS
تم إجراء تحليل XPS لتحليل الحالة الكيميائية التفصيلية للمحفز المُعد. كما لوحظ من الشكل 3a، فإن طيف C 1 s للكتلة
| عينة | مساحة السطح
|
حجم المسام
|
حجم البلورات (نانومتر) | فجوة الطاقة (eV) | التركيب العنصري | |
| نسبة الكربون (وزن%) | N (نسبة الوزن%) | |||||
| ج-
|
٥.٠٣٥ | 0.028 | 9.0 | 2.54 | ٣٤.٠٦ | 65.94 |
|
|
9.189 | 0.08 | ٥.٧ | ٢.٥٩ | ٣٦.٠٠ | ٦٤.٠٠ |
|
|
١٣.٤٥ | 0.092 | 5.3 | 2.61 | ٣٧.٠٠ | ٦٣.٠٠ |
|
|
٤٨.٢٠٣ | 0.32 | ٤.٢ | 2.7 | ٣٩.٣ | 60.7 |
الجدول 1. المساحة السطحية، حجم المسام، حجم البلورات، فجوة الطاقة، والتركيب العنصري للمواد الكتلية والم exfoliated
الشكل 3. طيف XPS للكتلة
تم العثور عليها عند 288.34 إلكترون فولت و 285.341.
تحليل الشكل
توضح الشكل 4 الشكل البنيوي للعينات المحضرة التي أكدت تأثير درجة الحرارة على التقشر الحراري للمواد المحضرة. في حالة الكتلة
تحليل المساحة السطحية
تظهر الشكل 5
دراسة بصرية
تم فحص الخصائص البصرية للمواد المحفزة الضوئية المنتجة باستخدام مطيافية الانعكاس المنتشر للأشعة فوق البنفسجية (UV-DRS). تُظهر طيف الامتصاص البصري للعينات المحضرة في الشكل 6a. جميع الـ
الشكل 4. صور FESEM للعينات المُركبة: (أ)
الشكل 5. (أ)
الشكل 6. (أ) طيف الامتصاص للأشعة فوق البنفسجية والمرئية
أظهرت العينات المحضرة حافة امتصاص عند 450 نانومتر مما يدل على الخصائص الجوهرية (
علاوة على ذلك، تم جدولتها في الجدول 1 فجوات النطاق لجميع المحفزات الضوئية. تم حساب قيم فجوة النطاق باستخدام المعادلة التالية:
أين،
النشاط الضوئي التحفيزي
الأداء الضوئي المحفز لـ
أثر المحفز
تم تحليل الخصائص التحفيزية للمحفزات المحضرة من خلال إجراء التحلل الضوئي لجميع الأصباغ الثلاثة بشكل فردي تحت إشعاع الضوء فوق البنفسجي. في البداية، تم وضع جميع الأصباغ في غرفة التفاعل الضوئي وتم إشعاعها لمدة 60 دقيقة دون وجود محفز وتم تسجيل طيف الامتصاص المقابل كما هو موضح في الشكل 7a-f. أظهر الاختبار الفارغ (الخط الأسود في الشكل 7) عدم وجود تحلل للأصباغ. ومع ذلك، بعد إضافة المحفز الضوئي إلى محاليل الأصباغ، كان هناك انخفاض ملحوظ في تركيزات جميع محاليل الأصباغ.
الشكل 7. (أ-ج) حركيات التحلل المعتمدة على الزمن المقاسة كتركيز الصبغة عند الزمن t بالنسبة لتركيزها الابتدائي
علاوة على ذلك، فإن ثابت المعدل لـ
| محفز ضوئي | صبغة MB | صبغة RhB | صبغة MO |
| جملة
|
|
|
|
|
|
|
|
|
|
|
|
|
|
|
|
|
|
|
الجدول 2. قيم ثابت المعدل للكتلة والمستخرجة
تحقيق في آليات التفاعل الضوئي المحفز تحليل الطيف الضوئي (PL) وتحليل impedanc
من المتوقع أن يتمتع المحفز الضوئي الجيد بمعدل نقل شحنة مرتفع ومعدل إعادة تركيب منخفض للثقوب والإلكترونات المثارة ضوئيًا.
اختبارات امتصاص الجذور الحرة
في عملية التحلل الضوئي النموذجية، يتم تحفيز الفجوة الناتجة عن الضوء (
الشكل 8. (أ) طيف الفوتولومينسنس (PL) للمواد المحفزة الضوئية المُعدة، (ب) تحليل EIS للمواد المحفزة الضوئية المُعدة.
الشكل 9. (أ) دراسة امتصاص الجذور الحرة لتحديد آليات التفاعل لـ
| محفز ضوئي | فجوة الطاقة (eV) | جهد نطاق التوصيل (eV) [
|
جهد نطاق التكافؤ ( eV ) [
|
| جملة
|
2.54 | -1.05 | 1.49 |
|
|
٢.٥٩ | -1.075 | 1.51 |
|
|
2.61 | -1.085 | 1.52 |
|
|
2.7 | -1.13 | 1.57 |
الجدول 3. فجوة الطاقة (
أين،
بالإضافة إلى ذلك، تم إجراء تحليل موت-شوتكي أيضًا لأفضل محفز.
تقييم قابلية إعادة استخدام المحفزات الضوئية
الأفضل أداءً
الخاتمة
TE-
الشكل 10. آلية التفاعل الضوئي المقترحة
بعد 5 جولات متتالية. وبالتالي، TE-g-C-
توفر البيانات
جميع البيانات التي تدعم نتائج الدراسة متاحة من المؤلف المراسل عند الطلب المعقول.
تاريخ الاستلام: 15 نوفمبر 2023؛ تاريخ القبول: 22 يناير 2024
نُشر على الإنترنت: 27 يناير 2024
تاريخ الاستلام: 15 نوفمبر 2023؛ تاريخ القبول: 22 يناير 2024
نُشر على الإنترنت: 27 يناير 2024
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شكر وتقدير
يود المؤلفون أن يشكروا إدارة VIT على التسهيلات المطلوبة لتنفيذ هذا العمل. تم إنشاء الملخص الرسومي باستخدامبيوريندر.كوم (رقم الترخيص: TH268W5VVJ).
مساهمات المؤلفين
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معلومات إضافية
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معلومات إعادة الطباعة والتصاريح متاحة علىwww.nature.com/reprints.
ملاحظة الناشر: تظل شركة سبرينغر ناتشر محايدة فيما يتعلق بالمطالبات القضائية في الخرائط المنشورة والانتماءات المؤسسية.
الوصول المفتوح هذه المقالة مرخصة بموجب رخصة المشاع الإبداعي النسب 4.0 الدولية، التي تسمح بالاستخدام والمشاركة والتكيف والتوزيع وإعادة الإنتاج بأي وسيلة أو صيغة، طالما أنك تعطي الائتمان المناسب للمؤلفين الأصليين والمصدر، وتوفر رابطًا لرخصة المشاع الإبداعي، وتوضح ما إذا تم إجراء تغييرات. الصور أو المواد الأخرى من طرف ثالث في هذه المقالة مشمولة في رخصة المشاع الإبداعي الخاصة بالمقالة، ما لم يُشار إلى خلاف ذلك في سطر الائتمان للمواد. إذا لم تكن المادة مشمولة في رخصة المشاع الإبداعي الخاصة بالمقالة وكان استخدامك المقصود غير مسموح به بموجب اللوائح القانونية أو يتجاوز الاستخدام المسموح به، فستحتاج إلى الحصول على إذن مباشرة من صاحب حقوق الطبع والنشر. لعرض نسخة من هذه الرخصة، قم بزيارةhttp://creativecommons.org/licenses/by/4.0/.
© المؤلف(ون) 2024
© المؤلف(ون) 2024
قسم الكيمياء، مدرسة العلوم المتقدمة، معهد فيلور للتكنولوجيا، فيلور، تاميل نادو 632014، الهند. هندسة تصنيع الأعضاء البشرية (HOME)، مختبر، مركز المواد الحيوية، العلاج الخلوي والجزيئي (CBCMT)، معهد فيلور للتكنولوجيا، فيلور، تاميل نادو 632014، الهند. قسم الهندسة الكهروضوئية، جامعة تايبيه الوطنية للتكنولوجيا، تايبيه 106، تايوان. البريد الإلكتروني:arunkumar.p@vit.ac.in
Journal: Scientific Reports, Volume: 14, Issue: 1
DOI: https://doi.org/10.1038/s41598-024-52688-y
PMID: https://pubmed.ncbi.nlm.nih.gov/38280908
Publication Date: 2024-01-27
DOI: https://doi.org/10.1038/s41598-024-52688-y
PMID: https://pubmed.ncbi.nlm.nih.gov/38280908
Publication Date: 2024-01-27
Efficient photocatalytic degradation of textile dye pollutants using thermally exfoliated graphitic carbon nitride (
Graphitic carbon nitride (
In recent years, globalization, the advancement of technology, coupled with the evolving fashion preferences of humans, has significantly contributed to the augmentation of textile and garment manufacturing
toxic dyes is reported to trigger respiratory infections, skin, and eye irritations
Graphitic carbon nitride
The thermal exfoliation process of
Experimental section Materials
Melamine
Figure 1. Schematic showing the preparation of
oxalate
Synthesis
Preparation of bulk
The bulk
The bulk
Preparation of
TE-g-C3
TE-g-C3
Characterization
X-ray diffraction (XRD) tests were employed to verify the production and purity of the synthesized materials using Panalytical X’Pert
Photocatalytic experiments
The photocatalytic activity of the TE-g-C
The degradation percentage of each dye and the rate constant of the photocatalyst reaction were evaluated using the following equations.
where,
Electrochemical measurements
Mott-Schottky analysis was performed to confirm the conduction band value. Using
Results and Discussion
Powder XRD results
Figure 2a showed the XRD pattern of all the prepared
Figure 2a showed the XRD pattern of all the prepared
Figure 2. (a) Powder XRD results of
arrangement of tri-s-triazine heterocycles and the periodic repetition of heptazine units inside the plane, respectively. The thermally exfoliated samples showed broader peaks with reduced intensities when compared to their bulk counterparts, which probably depicted the reduced layer spacing in the exfoliated ones
FTIR analysis
Functional groups and chemical bonding of prepared materials were studied by Fourier transform infrared (FTIR) spectroscopy, as shown in Fig. 2b. Here all the prepared samples possess similar characteristics spectra of
XPS analysis
The XPS analysis was performed to analyze the detailed chemical status of the catalyst prepared. As observed from Fig. 3a, the C 1 s spectrum of bulk
| Sample | Surface area
|
Pore volume (
|
Crystallite size (nm) | Band gap (eV) | Elemental composition | |
| C (wt%) | N (wt%) | |||||
| g-
|
5.035 | 0.028 | 9.0 | 2.54 | 34.06 | 65.94 |
|
|
9.189 | 0.08 | 5.7 | 2.59 | 36.00 | 64.00 |
|
|
13.45 | 0.092 | 5.3 | 2.61 | 37.00 | 63.00 |
|
|
48.203 | 0.32 | 4.2 | 2.7 | 39.3 | 60.7 |
Table 1. Surface area, pore volume, crystallite size, band gap and, elemental composition of bulk and exfoliated
Figure 3. XPS spectrum of bulk
were found at 288.34 eV and 285.341.
Morphology analysis
Figure 4 illustrated the structural morphology of prepared samples which confirmed the effect of temperature on the thermal exfoliation of the prepared materials. In case of bulk
Surface area analysis
Figure 5 displays the
Optical study
The optical characteristics of the produced photocatalysts were examined using ultra-violet diffuse reflectance spectroscopy (UV-DRS). The optical absorption spectra of the prepared samples are shown in Fig. 6a. All the
Figure 4. FESEM images of the synthesized samples: (a)
Figure 5. (a)
Figure 6. (a) UV-Visible absorbance spectra of
prepared samples exhibited absorption edge at 450 nm depicting intrinsic (
Furthermore, the band gaps of all photocatalysts are tabulated in Table 1. The band gap values were calculated using the following equation:
where,
Photocatalytic activity
The photocatalytic performance of
Effect of catalyst
The catalytic properties of the prepared catalysts were analyzed by performing photodegradation of all three dyes individually under irradiation of UV light. Initially, all the dyes were kept in the photocatalytic reaction chamber and irradiated for 60 min without a catalyst and their corresponding absorbance spectrum was recorded as shown in Fig. 7a-f. The blank test (black line in Fig. 7) showed no degradation of dyes. However, after addition of photocatalyst to the dye solutions, there was a remarkable reduction in the concentrations of all dye solutions. Figure
Figure 7. (a-c) Time dependent degradation kinetics measured as the concentration of dye at time t with respect to initial concentration
Moreover, the rate constant for
| Photocatalyst | MB dye | RhB dye | MO dye |
| bulk
|
|
|
|
|
|
|
|
|
|
|
|
|
|
|
|
|
|
|
Table 2. Rate constant values for the bulk and exfoliated
Investigation of the photocatalytic reaction mechanisms Photoluminescence (PL) Spectroscopy and EIS analysis
A good photocatalyst are expected to have high charge transfer rate and low recombination rate of photoexcited holes and electrons
Radical scavenging tests
In a typical photocatalytic degradation process, the photo-induced hole (
Figure 8. (a) Photoluminescence (PL) spectra of prepared photocatalysts, (b) EIS analysis of the prepared photocatalysts.
Figure 9. (a) Radical scavenging study to determine the reaction mechanisms for
| Photocatalyst | Band gap (eV) | Conduction band potential (eV) [
|
Valance band potential ( eV ) [
|
| bulk
|
2.54 | -1.05 | 1.49 |
|
|
2.59 | -1.075 | 1.51 |
|
|
2.61 | -1.085 | 1.52 |
|
|
2.7 | -1.13 | 1.57 |
Table 3. Band gap (
where,
Additionally, Mott-Schottky analysis was also performed for the best catalyst
Evaluation of the reusability of the photocatalysts
The best-performing
Conclusion
The TE-
Figure 10. The proposed photocatalytic reaction mechanism of
after 5 consecutive runs. Thus, TE-g-C-
Data availability
All data that supports the findings of the study are available from the corresponding author on reasonable request.
Received: 15 November 2023; Accepted: 22 January 2024
Published online: 27 January 2024
Received: 15 November 2023; Accepted: 22 January 2024
Published online: 27 January 2024
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Acknowledgements
Authors would like to thank VIT management for required facilities to carry out this work. Graphical abstract was created with Biorender.com (License Number: TH268W5VVJ).
Author contributions
S.G: Synthesis, Methodology, Conceptualization, Data curation, Formal analysis, Investigation, Writing-original draft. T.K: Formal analysis, Visualization. S.S: Conceptualization, Resource, Formal analysis. A.P: Supervision, Resources, Data curation, Funding acquisition, Conceptualization, Validation, Writing-review & editing.
Competing interests
The authors declare no competing interests.
Additional information
Supplementary Information The online version contains supplementary material available at https://doi.org/ 10.1038/s41598-024-52688-y.
Correspondence and requests for materials should be addressed to A.P.
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© The Author(s) 2024
© The Author(s) 2024
Department of Chemistry, School of Advanced Sciences, Vellore Institute of Technology, Vellore, Tamil Nadu 632014, India. Human Organ Manufacturing Engineering (HOME), Lab, Centre for Biomaterials, Cellular and Molecular Theranostics (CBCMT), Vellore Institute of Technology, Vellore, Tamil Nadu 632014, India. Department of Electro-Optical Engineering, National Taipei University of Technology, Taipei 106, Taiwan. email: arunkumar.p@vit.ac.in