การย่อยสลายสีย้อมรีแอคทีฟเรด 120 บนตัวเร่งปฏิกิริยาเชิงแสง Fe-N-TiO2 โดยการดูดซับและการเกิดปฏิกิริยาภายใต้การฉายแสงวิซิเบิล
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ธ.ค. 26, 2020
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การเจือด้วยโลหะ การเจือด้วยอโลหะ การเจือร่วมกัน ไฮโดรเทอร์มอล ไททาเนียมไดออกไซด์ สีย้อมรีแอคทีฟเรด 120
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บทคัดย่อ
วัตถุประสงค์ของงานวิจัยนี้เพื่อปรับปรุงประสิทธิภาพของตัวเร่งปฏิกิริยาไนโตรเจนไททาเนียมไดออกไซด์โดยการเจือเหล็ก (Fe-N-TiO2) ต่อประสิทธิภาพในการย่อยสลายสีย้อมประเภทรีแอคทีฟเรด 120 ภายใต้แสงวิซิเบิล ตัวเร่งปฏิกิริยา Fe-N-TiO2 และ N-TiO2 ถูกสังเคราะห์ด้วยวิธีไฮโดรเทอร์มอล และไม่ผ่านกระบวนการแคลไซน์ ตัวเร่งปฏิกิริยาที่ศึกษาเพื่อเปรียบเทียบประสิทธิภาพ คือ ตัวเร่งปฏิกิริยาไททาเนียมไดออกไซด์ที่มีการเจือเหล็กร้อยละ 1 โดยน้ำหนัก (1.0%Fe-N-TiO2) ตัวเร่งปฏิกิริยาที่ไม่มีการเจือเหล็ก (N-TiO2) และตัวเร่งปฏิกิริยาทางการค้า (P25) คุณสมบัติทางกายภาพและทางเคมีของตัวเร่งปฏิกิริยา ได้แก่ โครงสร้างผลึก ขนาดผลึก ลักษณะสัณฐานวิทยา พื้นที่ผิวจำเพาะ สถานะออกซิเดชันของธาตุ ช่องว่างพลังงาน และค่าความเป็นแม่เหล็ก ได้ทำการวิเคราะห์ ด้วยเทคนิค X-ray diffraction (XRD) Field emission scanning electron microscope (FESEM) N2-adsorption-desorption X-ray photoemission spectroscopy (XPS) UV-vis diffuse reflectance spectroscopy (UV-DRs) และ Versalab (VSM) ตามลำดับ ผลการศึกษาพบว่าตัวเร่งปฏิกิริยา N-TiO2 และ P25 พบเฟสอนาเทสเป็นหลัก และเฟสรูไทล์พบเพียงเล็กน้อย ตัวเร่งปฏิกิริยา 1.0%Fe-N-TiO2 พบว่าความเป็นผลึกของเฟสอนาเทสลดลงและไม่พบเฟสรูไทล์ การเจือเหล็กทำให้ตัวเร่งปฏิกิริยามีขนาดผลึกขนาดเล็กประมาณ 10-11 นาโนเมตร ลักษณะสัณฐานวิทยาของตัวเร่งปฏิกิริยาที่สังเคราะห์ด้วยวิธีไฮโดรเทอร์มอล มีรูปร่างค่อนข้างเป็นทรงกลมที่มีขนาดอนุภาคนาโนเมตร และเมื่อมีการเจือเหล็กขนาดของอนุภาคเล็กลง พื้นที่ผิวจำเพาะของตัวเร่งปฏิกิริยาที่คำนวณโดยสมการของ Brunauer–Emmett–Teller (BET) พบว่าตัวเร่งปฏิกิริยา 1.0%Fe-N-TiO2 มีพื้นที่ผิวจำเพาะสูงสุดโดยมีค่าประมาณ 115 ตารางเมตรต่อกรัม สถานะออกซิเดชันของเหล็กในตัวเร่งปฏิกิริยา 1.0%Fe-N-TiO2 มีเลขออกซิเดชันเป็น Fe3+ ซึ่งการเจือเหล็กสามารถลดช่องว่างพลังงานจาก 2.94 อิเล็กตรอนโวลต์ (N-TiO2) เป็น 2.70 อิเล็กตรอนโวลต์ และค่าความเป็นแม่เหล็กของตัวเร่งปฏิกิริยา 1.0%Fe-N-TiO2 มีค่าความเป็นแม่เหล็กประมาณ 0.011 emuต่อกรัม ผลของการกำจัดสีย้อมรีแอคทีฟเรด 120 โดยการดูดซับและการเกิดปฏิกิริยาภายใต้แสงวิซิเบิล ผลพบว่าประสิทธิภาพการจำกัดสีย้อมของตัวเร่งปฏิกิริยา 1.0%Fe-N-TiO2 มีค่าสูงถึงร้อยละ 99 และมีประสิทธิภาพสูงสุดเมื่อเทียบกับตัวเร่งปฏิกิริยา N-TiO2 และ P25 สามารถสรุปได้ว่าตัวเร่งปฏิกิริยาไนโตรเจนไททาเนียมไดออกไซด์ที่ได้รับการปรับปรุงโดยการเจือเหล็กสามารถย่อยสลายมลพิษได้จริงภายใต้แสงวิซิเบิล
Article Details
ประเภทบทความ
บทความวิจัย (Research Article)
เอกสารอ้างอิง
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[2] Wu CH. Effects of operational parameters on the decolorization of C.I. Reactive Red 198 in UV/TiO2-based systems. Dyes and Pigments. 2008; 77(1): 31–38.
[3] Naghibi S, Faghihi Sani MA, Madaah Hosseini HR. Application of the statistical Taguchi method to optimize TiO2 nanoparticles synthesis by the hydrothermal assisted sol-gel technique. Ceramics International. 2014; 40(3): 4193–4201.
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[7] Komatsuda S, Asakura Y, Vequizo JJM, Yamakata A, Yin S. Enhanced photocatalytic NOx decomposition of visible-light responsive F-TiO2/(N,C)-TiO2 by charge transfer between F-TiO2 and (N,C)-TiO2 through their doping levels. Applied Catalysis B Environmental. 2018; 238(July): 358–364.
[8] Gar Alalm M, Samy M, Ookawara S, Ohno T. Immobilization of S-TiO2 on reusable aluminum plates by polysiloxane for photocatalytic degradation of 2,4-dichlorophenol in water. Journal of Water Process Engineering. 2018; 26(November): 329–335.
[9] Jaiswal R, Bharambe J, Patel N, Dashora A, Kothari DC, Miotello A. Copper and Nitrogen co-doped TiO2 photocatalyst with enhanced optical absorption and catalytic activity. Applied Catalysis B Environmental. 2015; 168–169: 333–341.
[10] Selvaraj A, Sivakumar S, Ramasamy AK, Balasubramanian V. Photocatalytic degradation of triazine dyes over N-doped TiO2 in solar radiation. Research on Chemical Intermediates. 2013; 39(6): 2287–2302.
[11] Ansari SA, Khan MM, Ansari MO, Cho MH. Nitrogen-doped titanium dioxide (N-doped TiO2) for visible light photocatalysis. New Journal of Chemistry. 2016; 40(4): 3000–3009.
[12] Barkul RP, Koli VB, Shewale VB, Patil MK, Delekar SD. Visible active nanocrystalline N-doped anatase TiO2 particles for photocatalytic mineralization studies. Materials Chemistry and Physics. 2016; 173(January): 42-51
[13] Asahi R, Morikawa T, Irie H, Ohwaki T. Nitrogen-doped titanium dioxide as visible-light-sensitive photocatalyst: Designs, developments, and prospects. Chemical Reviews. 2014; 114(19): 9824–9852.
[14] Razali NA, Othman SA. Synthesis and Characterization of Nitrogen Doped with Titanium Dioxide at Different Calcination Temperature by using Sol-Gel Method. Journal of Science and Technology. 2017; 9(3): 124–130.
[15] Majeed Khan MA, Siwach R, Kumar S, Alhazaa AN. Role of Fe doping in tuning photocatalytic and photoelectrochemical properties of TiO2 for photodegradation of methylene blue. Optics and Laser Technology. 2019; 118(March): 170–178.
[16] Hinojosa–Reyes M, Camposeco–Solis R, Ruiz F, Rodríguez–González V, Moctezuma E. Promotional effect of metal doping on nanostructured TiO2 during the photocatalytic degradation of 4-chlorophenol and naproxen sodium as pollutants. Materials Science in Semiconductor Processing. 2019; 100(December 2018): 130–139.
[17] Jaihindh DP, Verma A, Chen CC, Huang YC, Dong CL, Fu YP. Study of oxidation states of Fe- and Co-doped TiO2 photocatalytic energy materials and their visible-light-driven photocatalytic behavior. International of Journal Hydrogen Energy. 2019; 15892–15906.
[18] Karafas ES, Romanias MN, Stefanopoulos V, Binas V, Zachopoulos A, Kiriakidis G, et al. Effect of metal doped and co-doped TiO2 photocatalysts oriented to degrade indoor/outdoor pollutants for air quality improvement. A kinetic and product study using acetaldehyde as probe molecule. Journal of Photochemistry Photobiology A Chemistry. 2019; 371(November 2018): 255–263.
[19] Moradi H, Eshaghi A, Hosseini SR, Ghani K. Fabrication of Fe-doped TiO2 nanoparticles and investigation of photocatalytic decolorization of reactive red 198 under visible light irradiation. Ultrasonics Sonochemistry. 2016; 32: 314–319.
[20] Khan H, Swati IK. Fe3+-doped Anatase TiO2 with d-d Transition, Oxygen Vacancies and Ti3+ Centers: Synthesis, Characterization, UV-vis Photocatalytic and Mechanistic Studies. Industrial Engineering Chemistry Research. 2016; 55(23): 6619–6633.
[21] Rivera KKP, de Luna MDG, Suwannaruang T, Wantala K. Photocatalytic degradation of reactive red 3 and alachlor over uncalcined Fe–TiO2 synthesized via hydrothermal method. Desalination and Water Treatment. 2016; 57(46): 22017–22028.
[22] Zou M, Xiong F, Ganeshraja AS, Feng X, Wang C, Thomas T, et al. Visible light photocatalysts (Fe,N) : TiO2 from ammonothermally processed, solvothermal self-assembly derived Fe-TiO2 mesoporous microspheres. Materials Chemistry and Physics. 2017; 195: 259–267.
[23] Aphairaj D, Wirunmongkol T, Niyomwas S, Pavasupree S, Limsuwan P. Synthesis of anatase TiO2 nanotubes derived from a natural leucoxene mineral by the hydrothermal method. Ceramics International. 2014; 40(7 PART A): 9241–9247.
[24] Suwannaruang T, Wantala K. Single-step uncalcined N-TiO2 synthesis, characterizations and its applications on alachlor photocatalytic degradations. Applied Surface Science. 2016; 380(January): 257–267.
[25] Xu C, Zhang Y, Chen J, Lin J, Zhang X, Wang Z, et al. Enhanced mechanism of the photo-thermochemical cycle based on effective Fe-doping TiO2 films and DFT calculations. Applied Catalalysis B Environmental. 2017; 204(December 2018): 324–334.
[26] Yao Y, Sun M, Yuan X, Zhu Y, Lin X, Anandan S. One-step hydrothermal synthesis of N/Ti3+ co-doping multiphasic TiO2/BiOBr heterojunctions towards enhanced sonocatalytic performance. Ultrason Sonochem. 2018; 49(May): 69–78.
[27] Fiorenza R, Bellardita M, Scirè S, Palmisano L. Effect of the addition of different doping agents on visible light activity of porous TiO2 photocatalysts. Molecular Catalysis. 2018; 455(May): 108–120.
[28] Yun HJ, Lee DM, Yu S, Yoon J, Park HJ, Yi J. Effect of valence band energy on the photocatalytic performance of N-doped TiO2 for the production of O2 via the oxidation of water by visible light. Journal Molecular Catalysis A Chemical. 2013; 378(November 2013): 221–226.
[29] Safari M, Talebi R, Rostami MH, Nikazar M, Dadvar M. Synthesis of iron-doped TiO2 for degradation of reactive Orange16. Journal of Environmental Health Science Engineering. 2014; 12(1): 1–8.
[30] Sood S, Umar A, Mehta SK, Kansal SK. Highly effective Fe-doped TiO2 nanoparticles photocatalysts for visible-light driven photocatalytic degradation of toxic organic compounds. Journal of Colloid and Interface Science. 2015; 450: 213–223.
[31] Kalantari K, Kalbasi M, Sohrabi M, Royaee SJ. Enhancing the photocatalytic oxidation of dibenzothiophene using visible light responsive Fe and N co-doped TiO2 nanoparticles. Ceramics International. 2017; 43(1): 973–981.
[32] Thommes M, Kaneko K, Neimark A V, Olivier JP, Rodriguez-reinoso F, Rouquerol J, et al. Physisorption of gases , with special reference to the evaluation of surface area and pore size distribution. IUPAC Technical Report. 2015;87:1051–1069.
[33] Suwannaruang T, Kidkhunthod P, Chanlek N, Soontaranon S. Applied Surface Science High anatase purity of nitrogen-doped TiO2 nanorice particles for the photocatalytic treatment activity of pharmaceutical wastewater. Applied Surface Science. 2019; 478(October 2018): 1–14.
[34] Zhang K, Wang X, Guo X. Preparation of highly visible light active Fe–N co-doped mesoporous TiO2 photocatalyst by fast sol–gel method. Journal of Nanopartical Research. 2014; 16(2): (1-9)
[35] Abbas N, Shao GN, Haider MS, Imran SM, Park SS, Kim HT. Sol–gel synthesis of TiO2-Fe2O3systems: Effects of Fe2O3 content and their photocatalytic properties. Journal of Industrial and Engineering Chemistry. 2016; 39(2016): 112-120
[36] Liang R, Shen L, Jing F, Qin N, Wu L. Preparation of MIL−53 (Fe)−Reduced Graphene Oxide Nanocomposites by a Simple Self−Assembly Strategy for Increasing Interfacial Contact: Efficient Visible-Light Photocatalysts. Applied Materials Interfaces 2018; 53(April 2015): 9507-9515.
[37] Moura KO. Tuning the surface anisotropy in Fe-doped NiO nanoparticles. The Royal Society of Chemistry 2013; 6(November): 352-357.
[38] Bharti B, Kumar S, Lee H, Kumar R. Formation of oxygen vacancies and Ti3+ state in TiO2 thin film and enhanced optical properties by air plasma treatment. Nature Publishing Group. 2016; (August): 1-12.
[2] Wu CH. Effects of operational parameters on the decolorization of C.I. Reactive Red 198 in UV/TiO2-based systems. Dyes and Pigments. 2008; 77(1): 31–38.
[3] Naghibi S, Faghihi Sani MA, Madaah Hosseini HR. Application of the statistical Taguchi method to optimize TiO2 nanoparticles synthesis by the hydrothermal assisted sol-gel technique. Ceramics International. 2014; 40(3): 4193–4201.
[4] Liu G, Han C, Pelaez M, Zhu D, Liao S, Likodimos V, et al. Synthesis, characterization and photocatalytic evaluation of visible light activated C-doped TiO2 nanoparticles. Nanotechnology. 2012; 23(29): 294003.
[5] Suwannaruang T, Kamonsuangkasem K, Kidkhunthod P, Chirawatkul P, Saiyasombat C, Chanlek N, et al. Influence of nitrogen content levels on structural properties and photocatalytic activities of nanorice-like N-doped TiO2 with various calcination temperatures. Materials Research Bulletin. 2018; 105(May): 265–276.
[6] Hassan ME, Liu G, Omer EOM, Goja AM, Acharya S. Silver embedded C-TiO2 exhibits improved photocatalytic properties with potential application in waste water treatment. Arabian Journal of Chemistry. 2018; 0–6.
[7] Komatsuda S, Asakura Y, Vequizo JJM, Yamakata A, Yin S. Enhanced photocatalytic NOx decomposition of visible-light responsive F-TiO2/(N,C)-TiO2 by charge transfer between F-TiO2 and (N,C)-TiO2 through their doping levels. Applied Catalysis B Environmental. 2018; 238(July): 358–364.
[8] Gar Alalm M, Samy M, Ookawara S, Ohno T. Immobilization of S-TiO2 on reusable aluminum plates by polysiloxane for photocatalytic degradation of 2,4-dichlorophenol in water. Journal of Water Process Engineering. 2018; 26(November): 329–335.
[9] Jaiswal R, Bharambe J, Patel N, Dashora A, Kothari DC, Miotello A. Copper and Nitrogen co-doped TiO2 photocatalyst with enhanced optical absorption and catalytic activity. Applied Catalysis B Environmental. 2015; 168–169: 333–341.
[10] Selvaraj A, Sivakumar S, Ramasamy AK, Balasubramanian V. Photocatalytic degradation of triazine dyes over N-doped TiO2 in solar radiation. Research on Chemical Intermediates. 2013; 39(6): 2287–2302.
[11] Ansari SA, Khan MM, Ansari MO, Cho MH. Nitrogen-doped titanium dioxide (N-doped TiO2) for visible light photocatalysis. New Journal of Chemistry. 2016; 40(4): 3000–3009.
[12] Barkul RP, Koli VB, Shewale VB, Patil MK, Delekar SD. Visible active nanocrystalline N-doped anatase TiO2 particles for photocatalytic mineralization studies. Materials Chemistry and Physics. 2016; 173(January): 42-51
[13] Asahi R, Morikawa T, Irie H, Ohwaki T. Nitrogen-doped titanium dioxide as visible-light-sensitive photocatalyst: Designs, developments, and prospects. Chemical Reviews. 2014; 114(19): 9824–9852.
[14] Razali NA, Othman SA. Synthesis and Characterization of Nitrogen Doped with Titanium Dioxide at Different Calcination Temperature by using Sol-Gel Method. Journal of Science and Technology. 2017; 9(3): 124–130.
[15] Majeed Khan MA, Siwach R, Kumar S, Alhazaa AN. Role of Fe doping in tuning photocatalytic and photoelectrochemical properties of TiO2 for photodegradation of methylene blue. Optics and Laser Technology. 2019; 118(March): 170–178.
[16] Hinojosa–Reyes M, Camposeco–Solis R, Ruiz F, Rodríguez–González V, Moctezuma E. Promotional effect of metal doping on nanostructured TiO2 during the photocatalytic degradation of 4-chlorophenol and naproxen sodium as pollutants. Materials Science in Semiconductor Processing. 2019; 100(December 2018): 130–139.
[17] Jaihindh DP, Verma A, Chen CC, Huang YC, Dong CL, Fu YP. Study of oxidation states of Fe- and Co-doped TiO2 photocatalytic energy materials and their visible-light-driven photocatalytic behavior. International of Journal Hydrogen Energy. 2019; 15892–15906.
[18] Karafas ES, Romanias MN, Stefanopoulos V, Binas V, Zachopoulos A, Kiriakidis G, et al. Effect of metal doped and co-doped TiO2 photocatalysts oriented to degrade indoor/outdoor pollutants for air quality improvement. A kinetic and product study using acetaldehyde as probe molecule. Journal of Photochemistry Photobiology A Chemistry. 2019; 371(November 2018): 255–263.
[19] Moradi H, Eshaghi A, Hosseini SR, Ghani K. Fabrication of Fe-doped TiO2 nanoparticles and investigation of photocatalytic decolorization of reactive red 198 under visible light irradiation. Ultrasonics Sonochemistry. 2016; 32: 314–319.
[20] Khan H, Swati IK. Fe3+-doped Anatase TiO2 with d-d Transition, Oxygen Vacancies and Ti3+ Centers: Synthesis, Characterization, UV-vis Photocatalytic and Mechanistic Studies. Industrial Engineering Chemistry Research. 2016; 55(23): 6619–6633.
[21] Rivera KKP, de Luna MDG, Suwannaruang T, Wantala K. Photocatalytic degradation of reactive red 3 and alachlor over uncalcined Fe–TiO2 synthesized via hydrothermal method. Desalination and Water Treatment. 2016; 57(46): 22017–22028.
[22] Zou M, Xiong F, Ganeshraja AS, Feng X, Wang C, Thomas T, et al. Visible light photocatalysts (Fe,N) : TiO2 from ammonothermally processed, solvothermal self-assembly derived Fe-TiO2 mesoporous microspheres. Materials Chemistry and Physics. 2017; 195: 259–267.
[23] Aphairaj D, Wirunmongkol T, Niyomwas S, Pavasupree S, Limsuwan P. Synthesis of anatase TiO2 nanotubes derived from a natural leucoxene mineral by the hydrothermal method. Ceramics International. 2014; 40(7 PART A): 9241–9247.
[24] Suwannaruang T, Wantala K. Single-step uncalcined N-TiO2 synthesis, characterizations and its applications on alachlor photocatalytic degradations. Applied Surface Science. 2016; 380(January): 257–267.
[25] Xu C, Zhang Y, Chen J, Lin J, Zhang X, Wang Z, et al. Enhanced mechanism of the photo-thermochemical cycle based on effective Fe-doping TiO2 films and DFT calculations. Applied Catalalysis B Environmental. 2017; 204(December 2018): 324–334.
[26] Yao Y, Sun M, Yuan X, Zhu Y, Lin X, Anandan S. One-step hydrothermal synthesis of N/Ti3+ co-doping multiphasic TiO2/BiOBr heterojunctions towards enhanced sonocatalytic performance. Ultrason Sonochem. 2018; 49(May): 69–78.
[27] Fiorenza R, Bellardita M, Scirè S, Palmisano L. Effect of the addition of different doping agents on visible light activity of porous TiO2 photocatalysts. Molecular Catalysis. 2018; 455(May): 108–120.
[28] Yun HJ, Lee DM, Yu S, Yoon J, Park HJ, Yi J. Effect of valence band energy on the photocatalytic performance of N-doped TiO2 for the production of O2 via the oxidation of water by visible light. Journal Molecular Catalysis A Chemical. 2013; 378(November 2013): 221–226.
[29] Safari M, Talebi R, Rostami MH, Nikazar M, Dadvar M. Synthesis of iron-doped TiO2 for degradation of reactive Orange16. Journal of Environmental Health Science Engineering. 2014; 12(1): 1–8.
[30] Sood S, Umar A, Mehta SK, Kansal SK. Highly effective Fe-doped TiO2 nanoparticles photocatalysts for visible-light driven photocatalytic degradation of toxic organic compounds. Journal of Colloid and Interface Science. 2015; 450: 213–223.
[31] Kalantari K, Kalbasi M, Sohrabi M, Royaee SJ. Enhancing the photocatalytic oxidation of dibenzothiophene using visible light responsive Fe and N co-doped TiO2 nanoparticles. Ceramics International. 2017; 43(1): 973–981.
[32] Thommes M, Kaneko K, Neimark A V, Olivier JP, Rodriguez-reinoso F, Rouquerol J, et al. Physisorption of gases , with special reference to the evaluation of surface area and pore size distribution. IUPAC Technical Report. 2015;87:1051–1069.
[33] Suwannaruang T, Kidkhunthod P, Chanlek N, Soontaranon S. Applied Surface Science High anatase purity of nitrogen-doped TiO2 nanorice particles for the photocatalytic treatment activity of pharmaceutical wastewater. Applied Surface Science. 2019; 478(October 2018): 1–14.
[34] Zhang K, Wang X, Guo X. Preparation of highly visible light active Fe–N co-doped mesoporous TiO2 photocatalyst by fast sol–gel method. Journal of Nanopartical Research. 2014; 16(2): (1-9)
[35] Abbas N, Shao GN, Haider MS, Imran SM, Park SS, Kim HT. Sol–gel synthesis of TiO2-Fe2O3systems: Effects of Fe2O3 content and their photocatalytic properties. Journal of Industrial and Engineering Chemistry. 2016; 39(2016): 112-120
[36] Liang R, Shen L, Jing F, Qin N, Wu L. Preparation of MIL−53 (Fe)−Reduced Graphene Oxide Nanocomposites by a Simple Self−Assembly Strategy for Increasing Interfacial Contact: Efficient Visible-Light Photocatalysts. Applied Materials Interfaces 2018; 53(April 2015): 9507-9515.
[37] Moura KO. Tuning the surface anisotropy in Fe-doped NiO nanoparticles. The Royal Society of Chemistry 2013; 6(November): 352-357.
[38] Bharti B, Kumar S, Lee H, Kumar R. Formation of oxygen vacancies and Ti3+ state in TiO2 thin film and enhanced optical properties by air plasma treatment. Nature Publishing Group. 2016; (August): 1-12.
