Pyrolytic Temperature Dependent and Ash Catalyzed Formation of Sludge Char. Xiao-Qing Liu, Hong-Sheng Ding, Yuan-Ying Wang, Wu-Jun Liu, Hong Jiang*

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Pyrolytic Temperature Dependent and Ash Catalyzed Formation of Sludge Char with Ultra-High Adsorption to 1-Naphthol Xiao-Qing Liu, Hong-Sheng Ding, Yuan-Ying Wang, Wu-Jun Liu, Hong Jiang* CAS Key Laboratory of Urban Pollutant Conversion, Department of Chemistry, University of Science and Technology of China, Hefei 230026, China * Corresponding author: Dr. Hong Jiang Fax: 86-551-63607482; E-mail: jhong@ustc.edu.cn

Table S1 Comparison of the 1-Naphthol Adsorption Capacities of Adsorbents in this Work and Other Adsorbents in the Literature Adsorbent Commercial activated carbon Carbon nanotubes Preparation method Chemical vapor deposition (CVD) of acetylene in hydrogen flow at 760 o C q max (mg Adsorption g 1 ) temperature(k) Referances 72.08 298 S1 54.35 298 S2 XC-72 83.54 293 S3 OP700 sulfonated graphene sulfonated graphene Orange peels pyrolysis at 700 o C 47.97 S4 prepared from graphite 331 293 S5 prepared from graphite 922 313 S5 h-rgo GO reacted with hydrazine 799 303 S6 l-rgo GO reacted with hydrazine 514 303 S6 SC500 DA800 DC800 Sewage sludge pyrolysis at 500 o C SC800 washed with HF and HCl Sludge washed with HF and HCl, then pyrolysis at 800 o C 67.11 298 This work 666.67 298 This work 231 298 This work S1. Anbia, M.; Moradi, S. E., The examination of surface chemistry and porosity of carbon nanostructured adsorbents for 1-naphthol removal from petrochemical wastewater streams. Korean J. Chem. Eng. 2012, 29, 743-749. S2. Sheng, G., Shao, D., Ren, X., Wang, X., Li, J., Chen, Y., Wang, X.. Kinetics and thermodynamics of adsorption of ionizable aromatic compounds from aqueous solutions by as-prepared and oxidized multiwalled carbon nanotubes. J. Hazard. Mat. 2010, 178, 505-516. S3. Zuo, L., Yu, S., Cheng, L., Du, E. Adsorption of phenol and 1-naphthol onto XC-72 carbon. Korean J. Chem. Eng. 2013, 30, 714-723.

S4. Chen, B.; Chen, Z., Sorption of naphthalene and 1-naphthol by biochars of orange peels with different pyrolytic temperatures. Chemosphere 2009, 76, 127-33. S5. Zhao, G.; Li, J.; Wang, X., Kinetic and thermodynamic study of 1-naphthol adsorption from aqueous solution to sulfonated graphene nanosheets. Chem. Eng. J. 2011, 173, 185-190. S6. Ali, M. M.; Sandhya, K., Reduced graphene oxide as a highly efficient adsorbent for 1-naphthol and the mechanism thereof. RSC Adv. 2014, 4, 51624-51631.

Table S2 Adsorption Capacity of Adsorbents, results of 4d batch experiments Adsorbent Ash Ash(%) Wt% Adsorption Q 1 (mg g 1 ) Adsorbent Sludge char Adsorption Qs e (mg g 1 ) Adsorbent Adsorption Qd e (mg g 1 ) Ash200 50.3 9.87 Ash300 63.3 8.92 SC300 18.21 DA300 81.20 Ash400 71.8 8.42 SC400 59.69 DA400 124.29 Ash500 73.4 8.44 SC500 67.11 DA500 387.49 Ash800 82.0 8.25 SC800 66.47 DA800 530.4 Table S3 The Percent of Peak Area Determined by XPS Chars C=C/C-C C-N C-O C=O DA300 39.2 28.8 22.5 9.6 DA400 41.5 27.7 21.2 10.6 DA500 43.0 28.3 22.7 DA800 58.2 26.3 15.6 DC300 41.8 27.7 17.2 13.3 DC400 39.2 27.2 19.4 14.2 DC500 36.1 26.5 20.4 16.9 DC800 40.9 26.9 19.6 12.6 Table S4 Raman Fitting Results of SCs and DAs SC400 SC500 SC800 DA300 DA400 DA500 DA800 DC300 DC400 DC500 DC800 I D1 /I G 2.49 2.74 2.26 3.25 3.21 3.10 2.60 2.55 3.42 2.57 3.17 I D2 /I G 0.24 0.13 0.06 0.75 0.43 0.24 0.12 0.03 0.20 0.05 0.03 I D3 /I G 0.24 0.22 0.18 0.39 0.24 0.38 0.21 0.22 0.32 0.30 0.66 I D4 /I G 0.22 0.17 0.14 0.21 0.19 0.20 0.14 0.15 0.27 0.22 0.44 I G /I all 0.24 0.24 0.28 0.18 0.20 0.20 0.25 0.25 0.19 0.24 0.19 I D1, I D2, I D3, I D4 and I G represent the fitting area of band D1, D2, D3, D4 and G respectively.

Table S5 The Composition of Sewage Sludge Ash Material SiO 2 Al 2 O 3 P 2 O 5 Fe 2 O 3 K 2 O MgO CaO NaO TiO 2 SO 3 Mn Content (%) 50.20 16.62 9.52 6.59 3.89 3.70 3.21 1.16 0.94 0.50 0.11 Table S6 The Yields of DAs DA300 DA400 DA500 DA800 Yields (%) 21.9 23.6 22.9 19.8 Table S7 TCLP Results chars Pb Cd Cu Zn(mg/L) SC300 ND ND ND 0.505 SC400 ND ND ND 0.4775 SC500 ND ND ND 0.8225 SC800 ND ND ND 0.6

Figure S1 TGA analysis of sludge

Figure S2 The N 2 stripping and adsorption isotherm of sludge chars.

Figure S3 Adsorption isotherm of 1-naphthol on DA800. ( initial 1-naphthol concentration 50-800 mg L 1, sorbent 0.3 g L 1 ).

Figure S4 XPS analysis of DCs

Figure S5 FTIR analysis of DCs

Figure S6 Fitting results of Raman.

Figure S7 Raman spectroscopy of DCs

Figure S8 Adsorption kinetics of 1-naphthol on deashed sludge chars ( initial 1-naphthol concentration 200 mg L 1, sorbent 0.5 g L 1 ).

Figure S9 SEM images of sludge (a), DA800 (b), deashed sludge (c), and DC800 (d).

a1 a2 a3 a4 b1 b2 b3 b4 c1 c2 c3 c4 d1 d2 d3 d4 e1 e2 e3 e4 Figure S10 SEM-EDS line spectra of SC300 (a1-a5), SC400 (b1-b5), SC500 (c1-c5), SC800 (d1-d5), DA800 (e1-e5).

a b Figure. S11 Effect of ph and temperature on the 1-naphthol adsorption capacity of DA800 To investigate the effect of ph on the 1-naphthol adsorption capacity of DA800, experiments were carried out using 200 mg L 1 1-naphthol aqueous solution with initial ph values ranging from 5.0 to 9.0.