# H Currently, there are several effective techniques for removal of heavy metal ions: chemical precipitation (Fu et al., 2011), ion exchange (Zewail et al., 2015), adsorption (Kumar et al., 2016), membrane filtration (Yurekli et al., 2017), electrodialysis (Nemati et al., 2017), reverse osmosis (Li et al., 2017), etc. Among them, the adsorption seems to be the most attractive technique due to its recovery merit, low cost, easy handling and simple design requirement (Kurniawan et al., 2006). However, it is difficult to remove the total metal ions by the only adsorption because of the physicochemical limitation of adsorptive rate particularly at the low concentration range of target metals. In contrast, a coupling method of the adsorption and the photoelectrodeposition is a more effective technique for the removing heavy metal ions at low concentrations due to utilizing irreversible photocatalytic redox reaction. Commonly, semiconductor photocatalysts have been used as an adsorbent to occur the photoelectrodeposition (Kobayashi et al., 2017;Nozaki et al., 2018). The wide band gap semiconductors such as TiO 2 , WO 3 , SnO 2 , and CeO 2 have mostly been used as a photocatalyst due to their thermal and chemical stability, low cost and environmental-friendly (Ji et al., 2009;Zhang et al., 2018). Among them, the CeO 2 has received much attention for the unique characteristics. The CeO 2 possesses large oxygen storage and releasing ability derived from the redox cycle between Ce 3+ and Ce 4+ , and the CeO 2 is often utilized for the catalytic oxidation reaction. The CeO 2 therefore plays an important role as a photocatalyst for photo-oxidation and photo-reduction against adsorbed substances (Ke et al., 2014;Qiang et al., 2015). Furthermore, the CeO 2 shows a strong UV absorption and does not cause the photolysis during the photocatalysis (Magesh et al., 2009), while only CeO 2 nanoparticles show low adsorption capacity of heavy metal ions. In the pioneering reports, improvement on the adsorption capacity was attempted by loading heterogeneous semiconductor materials possessing the high adsorption capacity and the high carrier conductivity for the surface photoelectrodeposition such as Gd 2 O 3 (Ayawanna et al., 2015), La 2 O 3 (Ayawanna et al., 2017), ZnO (Nozaki et al., 2018), etc., on the CeO 2 as an auxiliary catalyst. However, these metal oxides easily eluted instead of the adsorption of heavy metal ions as an ion-exchange manner because of their higher ionization tendency (Ayawanna et al., 2015;Ayawanna et al., 2017;Nozaki et al., 2018). Thus, an excellent loading material possessing high adsorption capacity, high carrier conductivity and chemical stability was desired. Tin-oxide compounds (SnO x ) are focused in this study. The SnO x has prominent superiorities such as high abundance, non-toxicity, low ionization tendency, high adsorption capacity of heavy metal ions, and fast carrier mobility between band structure and surface (Hamdi et al., 2017;Dey, 2018). Thus, the SnO x offers many technological applications such as photocatalysts (Zhao et al., 2018), solid-state gas sensors, and adsorbents for the removal of heavy metal ions (Kumar et al., 2016;Dey, 2018). Motivated by these factors, the SnO x was loaded on the CeO 2 surface to prepare a new photocatalyst for the adsorption and the photoelectrodeposition of heavy metal ions. The primary purpose of this study was to synthesize the SnO x /CeO 2 photocatalysts and evaluate its removal ability of heavy metal ions especially lead ion (Pb 2+ ). In addition, it was also a major purpose to obtain further knowledge of the photoelectrodeposition phenomenon which detailed mechanism has not been elucidated yet. # II. # Materials and Methods # a) Chemicals and reagents Ce(NO 3 ) O, and L(+)-ascorbic acid were all purchased from Wako Pure Chemical Industries Co., Ltd. 4-(2-pyridylazo)-resorcinol was purchased from Dojindo Molecular Technologies Co., Ltd. 2,3diaminonaphthalene and 1,5-diphenylcarbazide were purchased from Tokyo Chemical Industry Co., Ltd. All other reagents were at least of reagent grade and used without further purification. Milli-Q water was used for the preparation of all aqueous solutions. # b) Synthesis of SnO x /CeO 2 CeO 2 was prepared by the polymerized complex method. Firstly, 10.0 g of citric acid was dissolved in 11.8 g of ethylene glycol with heating at 50 ?C for 30 min under stirring at 600 rpm by a hot magnetic stirrer. Then, 5.0 g of Ce(NO 3 ) 3 ? 6H 2 O were added to the solution and heated at 200 ?C for 1 h under stirring at 600 rpm. Finally, the obtained precursor gel was calcined at 350 ?C for 1 h and then at 1000 ?C for 5 h with a heating rate of 10 ?C/min (Kakihana et al., 1992). SnO x /CeO 2 were prepared by the impregnation method. The prepared nanoparticles the abovewere impregnated in an aqueous solution of SnCl 2 ? 2H 2 O, and the solution was heated at 150 ?C under stirring at 400 rpm. After the evaporation of water, the obtained sample was calcined at 650 ?C for 3 h with a heating rate of 10 ?C/min (Murayama et al., 2017). # c) Characterization The crystal phase and structure of the obtained photocatalysts were analyzed by the powder X-ray diffraction (XRD, D8 ADVANCE, Bruker AXS) with CuK? radiation. The chemical states and composition of the photocatalyst surface were identified using the X-ray photoelectron spectroscopy (XPS, PHI X-tool, ULVAC-PHI) operated with AlK ? were calibrated by fixing the C 1s peak of the surface carbonaceous contaminants at 284.8 eV. The Brunauer-Emmett-Teller (BET) specific surface area of the photocatalysts were elucidated using a BET surface area analyzer (Flowsorb ?, d) Removal of Pb 2+ An aqueous solution including 20.0 mg/L Pb 2+ was prepared. Then, 0.130 g or 0.200 g of the SnO x /CeO 2 photocatalyst particles were added into a 20.0 mL of the prepared aqueous solution in a 30 mL beaker. The suspension was stirred at 500 rpm for 150 min by a magnetic stirrer and was also being irradiated with a UV-LED light (NCSU033B, 7.8 mW/cm 2 , 360-370 nm, NICHIA). Another similar experimental set was carried out on the same suspension under stirring in dark condition. After the experiments, the reaction suspension was sampled and filtered, and the pH of the filtrate was measured using a pH meter (PH-201, SAGA). The residual concentrations of Pb 2+ in the filtrate was measured by the colorimetry with 4-(2-pyridylazo)resorcinol at 520 nm (Kocy?a et al., 2015). The effect of different initial pH on Pb 2+ removal was examined. The pH was adjusted using either 0.10 M HCl or 0.10 M NaOH solutions. In the time-course removal experiments of Pb 2+ , 1.000 g of the SnO x /CeO 2 photocatalysts were added into a 100.0 mL of the aqueous solution including 20.0 mg/L Pb 2+ in a 100 mL beaker due to sampling 5.0 mL of the reaction suspension at designated times (10, 30, 60, 105 and 150 min). The obtained data were fitted to the pseudo first-order model (Equation ( 1)) and pseudo second-order model (Equation ( 2)) (Lagergren et al., 1898;Ho et al., 1999): ?? ?? = ?? ?? (1 ? ??????(??? 1 ??))(1)?? ?? = ?? ?? 2 ?? 2 ?? (1+?? ?? ?? 2 ??)(2) Adsorption and Photoelectrodeposition of Heavy Metal Ions from Wastewater using SnO x(1