Oxidation of As（Ⅲ） by three types of manganese oxides and the effects ofpH, ion strength and tartaric acid on the oxidation were investigated by means of chemical analysis, equilibrium redox, X-ray diffraction （XR...Oxidation of As（Ⅲ） by three types of manganese oxides and the effects ofpH, ion strength and tartaric acid on the oxidation were investigated by means of chemical analysis, equilibrium redox, X-ray diffraction （XRD） and transmission electron microscopy （TEM）. Three synthesized Mn oxide minerals, bimessite, cryptomelane, and hausmannite, which widely occur in soil and sediments, could actively oxidize As（Ⅲ） to As（Ⅴ）. However, their ability in As（Ⅲ）-oxidation varied greatly depending on their structure, composition and surface properties. Tunnel structured cryptomelane exhibited the highest ability of As （Ⅲ） oxidation, followed by the layer structured birnessite and the lower oxide hausmannite. The maximum amount of As （Ⅴ） produced by the oxidation was in the order （mmol/kg） of cryptomelane （824.2） 〉 bimessite （480.4） 〉 hausmannite （117.9）, As pH increased from the very low value（pH 2.5）, the amount of As（Ⅲ） oxidized by the tested Mn oxides was firstly decreased, then negatively peaked in pH 3.0 6.5, and eventually increased remarkably. Oxidation of As（Ⅲ） by the Mn oxides had a buffering effects on the pH variation in the solution. It is proposed that the oxidative reaction processes between As （Ⅲ） and biruessite（or cryptomelane） are as follows： （1） at lower pH condition： （MnO2）x＋ H3AsO3 ＋ 0.5H^＋=0.5H2AsO4^- ＋ 0.5HAsO4^2- ＋Mn〉^2＋ （MnO2）x-1 ＋ H2O; （2） at higher pH condition： （MnO2）x ＋ H3AsO3 = 0.5H2AsO4^- ＋ 0.5HAsO4^2- ＋ 1.5H^＋ ＋ （MnO2）x-1. MnO. With increase of ion strength, the As（Ⅲ） oxidized by bimessite and cryptomelane decreased and was negatively correlated with ion strength. However, ion strength had little influence on As （Ⅲ） oxidation by the hausmarmite. The presence of tartaric acid promoted oxidation of As（Ⅲ） by birnessite. As for cryptomelane and hansmannite, the same effect was observed when the concentration of tartaric acid was below 4 mmol展开更多
Cadmium (Cd) and arsenic (As) are two of the most toxic elements.However,the chemical behaviors of these two elements are different,making it challenging to utilize a single adsorbent with high adsorption capacity for...Cadmium (Cd) and arsenic (As) are two of the most toxic elements.However,the chemical behaviors of these two elements are different,making it challenging to utilize a single adsorbent with high adsorption capacity for both Cd(Ⅱ) and As(Ⅴ) removal.To solve this problem,we synthesized HA/Fe-Mn oxides-loaded biochar (HFMB),a novel ternary material,to perform this task,wherein scanning electron microscopy (SEM) combined with EDS (SEM-EDS) was used to characterize its morphological and physicochemical properties.The maximum adsorption capacity of HFMB was 67.11 mg/g for Cd(Ⅱ) and 35.59 mg/g for As(Ⅴ),which is much higher compared to pristine biochar (11.06 mg/g,0 mg/g for Cd(Ⅱ) and As(Ⅴ),respectively).The adsorption characteristics were investigated by adsorption kinetics and the effects of the ionic strength and pH of solutions.X-ray photoelectron spectroscopy (XPS) and Fourier-transform infrared spectroscopy (FT-IR) revealed that chelation and deposition were the adsorption mechanisms that bound Cd(Ⅱ) to HFMB,while ligand exchange was the adsorption mechanism that bound As(Ⅴ).展开更多
文摘Oxidation of As（Ⅲ） by three types of manganese oxides and the effects ofpH, ion strength and tartaric acid on the oxidation were investigated by means of chemical analysis, equilibrium redox, X-ray diffraction （XRD） and transmission electron microscopy （TEM）. Three synthesized Mn oxide minerals, bimessite, cryptomelane, and hausmannite, which widely occur in soil and sediments, could actively oxidize As（Ⅲ） to As（Ⅴ）. However, their ability in As（Ⅲ）-oxidation varied greatly depending on their structure, composition and surface properties. Tunnel structured cryptomelane exhibited the highest ability of As （Ⅲ） oxidation, followed by the layer structured birnessite and the lower oxide hausmannite. The maximum amount of As （Ⅴ） produced by the oxidation was in the order （mmol/kg） of cryptomelane （824.2） 〉 bimessite （480.4） 〉 hausmannite （117.9）, As pH increased from the very low value（pH 2.5）, the amount of As（Ⅲ） oxidized by the tested Mn oxides was firstly decreased, then negatively peaked in pH 3.0 6.5, and eventually increased remarkably. Oxidation of As（Ⅲ） by the Mn oxides had a buffering effects on the pH variation in the solution. It is proposed that the oxidative reaction processes between As （Ⅲ） and biruessite（or cryptomelane） are as follows： （1） at lower pH condition： （MnO2）x＋ H3AsO3 ＋ 0.5H^＋=0.5H2AsO4^- ＋ 0.5HAsO4^2- ＋Mn〉^2＋ （MnO2）x-1 ＋ H2O; （2） at higher pH condition： （MnO2）x ＋ H3AsO3 = 0.5H2AsO4^- ＋ 0.5HAsO4^2- ＋ 1.5H^＋ ＋ （MnO2）x-1. MnO. With increase of ion strength, the As（Ⅲ） oxidized by bimessite and cryptomelane decreased and was negatively correlated with ion strength. However, ion strength had little influence on As （Ⅲ） oxidation by the hausmarmite. The presence of tartaric acid promoted oxidation of As（Ⅲ） by birnessite. As for cryptomelane and hansmannite, the same effect was observed when the concentration of tartaric acid was below 4 mmol
基金supported by the National Key Research and Development Project of China(No.2016YFD0800706)the Science and Technology Project of Fujian Province of China(No.2018Y0080)the Science and Technology Project of Xiamen(No.3502Z20172026)
文摘Cadmium (Cd) and arsenic (As) are two of the most toxic elements.However,the chemical behaviors of these two elements are different,making it challenging to utilize a single adsorbent with high adsorption capacity for both Cd(Ⅱ) and As(Ⅴ) removal.To solve this problem,we synthesized HA/Fe-Mn oxides-loaded biochar (HFMB),a novel ternary material,to perform this task,wherein scanning electron microscopy (SEM) combined with EDS (SEM-EDS) was used to characterize its morphological and physicochemical properties.The maximum adsorption capacity of HFMB was 67.11 mg/g for Cd(Ⅱ) and 35.59 mg/g for As(Ⅴ),which is much higher compared to pristine biochar (11.06 mg/g,0 mg/g for Cd(Ⅱ) and As(Ⅴ),respectively).The adsorption characteristics were investigated by adsorption kinetics and the effects of the ionic strength and pH of solutions.X-ray photoelectron spectroscopy (XPS) and Fourier-transform infrared spectroscopy (FT-IR) revealed that chelation and deposition were the adsorption mechanisms that bound Cd(Ⅱ) to HFMB,while ligand exchange was the adsorption mechanism that bound As(Ⅴ).
