Sustainable degradation of carbon tetrafluoride to non-corrosive useful products by incorporating reduced electron mediator within electro-scrubbing

G. Muthuraman; A.G. Ramu; Y.H. Cho; E.J. McAdam; I.S. Moon

Journal of Industrial and Engineering Chemistry, Vol.63, 275-280, July, 2018

DOI10.1016/j.jiec.2018.02.025 Export Citation

Sustainable degradation of carbon tetrafluoride to non-corrosive useful products by incorporating reduced electron mediator within electro-scrubbing

G. Muthuraman, A.G. Ramu, Y.H. Cho¹, E.J. McAdam², and I.S. Moon^†

Department of Chemical Engineering, Sunchon National University, #255 Jungangno, Suncheon 57922, Jeollanam-do, Republic of Korea
¹Korea Atomic Energy Research Institute, Yuseong P.O. Box 105, Daejeon, Republic of Korea
²Cranfield Water Science Institute, Cranfield University, Building 39, MK43 0AL, UK

E-mail:

The degradation of CF4 gas using existing technologies produces other types of greenhouse gas (CO2) and corrosive side products. The main aim of this study is to degrade CF4 gas at room temperature into useful products without producing corrosive side products by mediated electrochemical reduction (MER) process using an electrogenerated Cu1+[Ni2+(CN)4]1- mediator. Initial studies on the electrolytic reduction of the hetero-bimetallic complex in catholyte solution at anodized Ti cathode was monitored by oxidation/reduction potential (ORP) variation whether the Cu2+ or Ni2+ was reduced in the Cu2+[Ni2 +(CN)4] and confirmed by electron spin resonance (ESR) spectroscopy the Cu1+[Ni2+(CN)4]1- formation. The concentration variation of Cu1+[Ni2+(CN)4]1- during CF4 injection demonstrated the degradation of CF4 followed the MER by electrogenerated Cu1+[Ni2+(CN)4]1-. Maximum removal efficiency of CF4 using electroscrubbing process was 96% at room temperature. Through the variation in gas phase parameters, the gas phase mass transfer coefficient was calculated that can facilitate scale up the developed process. Fourier transform infrared spectroscopy analysis in both the gas and solution phases showed that CH3CH2OH was the main product that formed during the removal of CF4 by electrogenerated Cu1+[Ni2 +(CN)4]1- at electroscrubber along with a small amount of CF3CH3 intermediate. Importantly, this mechanism also avoided formation of the corrosive product HF.

Keywords:Hetero-bimetal;MER;CF4 degradation;Ethanol formation

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[1] Ravishankara AR, Solomon S, Turnipseed AA, Warren RF, Science, 259, 194 (1993)

[2] Tsai WT, Chen HP, Hsien WY, J. Loss Prev. Process Ind., 15(2), 65 (2002)

[3] Rittmeyer C, Vehlow J, Chemosphere, 26, 2129 (1993)

[4] Lee CW, Ryan JV, Hall RE, Kryder GD, Springsteen BR, Combust. Sci. Technol., 116-117, 455 (1996)

[5] Lee HM, Chang MB, Lu RF, Ind. Eng. Chem. Res., 44(15), 5526 (2005)

[6] Gal' A, Ogata A, Futamura S, Mizuno K, J. Phys. Chem. A, 107(42), 8859 (2003)

[7] Xu XF, Jeon JY, Choi MH, Kim HY, Choi WC, Park YK, J. Mol. Catal. A-Chem., 266(1-2), 131 (2007)

[8] Gandhi MS, Mok YS, Environ J, J. Environ. Sci., 24, 1234 (2012)

[9] Narengerile, Saito H, Watanabe T, Plasma Chem. Plasma Process., 30(6), 813 (2010)

[10] Zhang HX, Ng CF, Lai SY, Appl. Catal. B: Environ., 55(4), 301 (2005)

[11] Xu X, Niu X, Fan J, Wang Y, Feng M, J. Nat. Gas Chem., 20, 543 (2011)

[12] Takita Y, Ninomiya M, Miyake H, Wakamatsu H, Yoshinaga Y, Ishihara T, Phys. Chem. Chem. Phys., 1, 4501 (1999)

[13] Farris MM, Klinghoffer AA, RosSnl JA, Tevault DE, Catal. Today, 11, 501 (1992)

[14] Sonoyama N, Sakata T, Environ. Sci. Technol., 32, 375 (1998)

[15] Cabot PL, Segarra L, Casado J, J. Electrochem. Soc., 151(2), B98 (2004)

[16] Wagoner ER, Peters DG, J. Electrochem. Soc., 160(10), G135 (2013)

[17] Schizodimou A, Kyriacou G, Lambrou C, J. Electroanal. Chem., 471(1), 26 (1999)

[18] Wagoner ER, Hayes JL, Karty JA, Peters DG, J. Electroanal. Chem., 676, 6 (2012)

[19] Cabot PL, Segarra L, Casado J, Electrochem. Solid State Lett., 6(3), B15 (2003)

[20] Taylor-Smith RE, Sayres D, Proc. Electrochem. Soc., 99-8, 116 (1999)

[21] Muthuraman G, Moon IS, J. Hazard. Mater., 325, 157 (2017)

[22] El-Bahy ZM, Ohnishi R, Ichikawa M, Appl. Catal. B: Environ., 40(2), 81 (2003)

[23] Takita Y, Morita C, Ninomiya M, Wakamatsu H, Nishiguchi H, Ishihara T, Chem. Lett., 417 (1999).

[24] Song JY, Chung SH, Kim MS, Seo MG, Lee YH, Lee KY, Kim JS, J. Mol. Catal. A-Chem., 370, 50 (2013)

[25] Chippindale AM, Hibble SJ, Marelli E, Bilbe EJ, Hannon AC, Zbiri M, Dalton Trans., 44, 12502 (2015)

[26] Fernelius WC, Burbage JJ, Ballou NE, Potassium tetracyanonickelate(II), Inorganic Syntheses, John Wiley & Sons Inc., pp.227 2007.

[27] Savelieff MG, Wilson TD, Elias Y, Nilges MJ, Garner DK, Lu Y, Proc. Natl. Acad. Sci. U. S. A., 105, 7919 (2008)

[28] Scharlin P, Battino R, J. Solut. Chem., 21, 67 (1992)

[29] Song Y, Peng R, Hensley DK, Bonnesen PV, Liang L, Wu Z, Meyer HM, Chi M, Ma C, Sumpter BG, Rondinone AJ, Chem. Sel., 1, 6055 (2016)

[30] Kuhl KP, Cave ER, Abram DN, Jaramillo TF, Energy Environ. Sci., 5, 7050 (2012)