Ying Xue, Yiming Tang, Xukai Li, Weirui Chen, Ying Wu, Guiquan Che, Laisheng Li
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Compared with 0.5 K min-1 and 2 K min-1, Mn-MCM-41 with 1 K min-1 showed much better performance in bromate inhibition process, Mn100-MCM-41 (molar ratio of Si/Mn=100) achieved 96.7% inhibition efficiency at pH 6.5, which was attributed to higher fraction of Mn(II)/Mn(III) and oxygen vacancies. The influence of pH, TBA and intermediate HOBr/OBr- were explored to investigate the mechanism. The results showed that more H2O2 generation and decreased O3 exposure to Br- in Mn-MCM-41 catalytic ozonation process, the oxidative transformation from Br- to HOBr/OBr- was blocked, resulting to less bromate formation. Highlights: • Temperature ramping rate during calcination of Mn-MCM-41 was crucial. • Oxygen vacancy and variation Mn state are responsible for catalytic performance. • Mn-MCM-41 achieved high bromate inhibition efficiency (96.7%) at pH 6.5. • Mn-MCM-41 inhibited BrO3 - by reducing HOBr/OBr-.","PeriodicalId":16326,"journal":{"name":"Journal of Material Sciences & Engineering","volume":"124 1","pages":"1-7"},"PeriodicalIF":0.0000,"publicationDate":"2018-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"2","resultStr":"{\"title\":\"Bromate Inhibition during Ozonation of Bromide-Containing Water by the Presence of Mn Incorporated MCM-41\",\"authors\":\"Ying Xue, Yiming Tang, Xukai Li, Weirui Chen, Ying Wu, Guiquan Che, Laisheng Li\",\"doi\":\"10.4172/2169-0022.1000460\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"The mesoporous Mn incorporated MCM-41 was employed to inhibit bromate formation during catalytic ozonation of bromide-containing water, Mn-MCM-41 was synthesized via hydrothermal method and the influences of temperature ramping rate (0.5, 1 and 2 K min-1) during calcination were investigated. It was characterized by XRD, TEM, SEM, XPS and H2-TPR, indicating that temperature ramping rate could affect the valence states of active Mn species, the dispersion of Mn on the surface of catalyst and the formation of oxygen vacancies, which could increase surface hydroxyl groups on Mn-MCM-41 and accelerated ozone decomposition to generate oxygen species. Compared with 0.5 K min-1 and 2 K min-1, Mn-MCM-41 with 1 K min-1 showed much better performance in bromate inhibition process, Mn100-MCM-41 (molar ratio of Si/Mn=100) achieved 96.7% inhibition efficiency at pH 6.5, which was attributed to higher fraction of Mn(II)/Mn(III) and oxygen vacancies. The influence of pH, TBA and intermediate HOBr/OBr- were explored to investigate the mechanism. The results showed that more H2O2 generation and decreased O3 exposure to Br- in Mn-MCM-41 catalytic ozonation process, the oxidative transformation from Br- to HOBr/OBr- was blocked, resulting to less bromate formation. 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引用次数: 2
摘要
采用介孔Mn掺入MCM-41抑制含溴化物水催化臭氧化过程中溴酸盐的生成,采用水热法合成了Mn-MCM-41,考察了焙烧过程中升温速率(0.5、1和2 K min-1)对溴酸盐生成的影响。通过XRD、TEM、SEM、XPS和H2-TPR对其进行表征,结果表明升温速率会影响活性Mn的价态,影响Mn在催化剂表面的分散和氧空位的形成,使Mn- mcm -41表面羟基增加,加速臭氧分解生成氧。与0.5 K min-1和2 K min-1相比,1 K min-1的Mn- mcm -41在溴酸盐缓蚀过程中表现出更好的缓蚀性能,在pH为6.5时,Mn- mcm -41 (Si/Mn摩尔比为100)的缓蚀效率达到96.7%,这主要归功于更高的Mn(II)/Mn(III)比例和氧空位。探讨了pH、TBA和中间HOBr/OBr-的影响机理。结果表明,在Mn-MCM-41催化臭氧化过程中,H2O2生成增多,O3暴露量减少,Br-向HOBr/OBr-的氧化转化被阻断,溴酸盐生成减少。•Mn-MCM-41煅烧过程中的升温速率至关重要。•氧空位和Mn态的变化对催化性能有影响。•Mn-MCM-41在pH 6.5时具有较高的溴酸盐抑制效率(96.7%)。Mn-MCM-41通过降低HOBr/OBr-抑制BrO3 -。
Bromate Inhibition during Ozonation of Bromide-Containing Water by the Presence of Mn Incorporated MCM-41
The mesoporous Mn incorporated MCM-41 was employed to inhibit bromate formation during catalytic ozonation of bromide-containing water, Mn-MCM-41 was synthesized via hydrothermal method and the influences of temperature ramping rate (0.5, 1 and 2 K min-1) during calcination were investigated. It was characterized by XRD, TEM, SEM, XPS and H2-TPR, indicating that temperature ramping rate could affect the valence states of active Mn species, the dispersion of Mn on the surface of catalyst and the formation of oxygen vacancies, which could increase surface hydroxyl groups on Mn-MCM-41 and accelerated ozone decomposition to generate oxygen species. Compared with 0.5 K min-1 and 2 K min-1, Mn-MCM-41 with 1 K min-1 showed much better performance in bromate inhibition process, Mn100-MCM-41 (molar ratio of Si/Mn=100) achieved 96.7% inhibition efficiency at pH 6.5, which was attributed to higher fraction of Mn(II)/Mn(III) and oxygen vacancies. The influence of pH, TBA and intermediate HOBr/OBr- were explored to investigate the mechanism. The results showed that more H2O2 generation and decreased O3 exposure to Br- in Mn-MCM-41 catalytic ozonation process, the oxidative transformation from Br- to HOBr/OBr- was blocked, resulting to less bromate formation. Highlights: • Temperature ramping rate during calcination of Mn-MCM-41 was crucial. • Oxygen vacancy and variation Mn state are responsible for catalytic performance. • Mn-MCM-41 achieved high bromate inhibition efficiency (96.7%) at pH 6.5. • Mn-MCM-41 inhibited BrO3 - by reducing HOBr/OBr-.