It is crucial to develop arsenic removal adsorbents with strong sulfur resistance under middle-low-temperature flue gas conditions(<400℃).In this work,five Fe-Ce-La oxides were prepared by co-precipitation method,...It is crucial to develop arsenic removal adsorbents with strong sulfur resistance under middle-low-temperature flue gas conditions(<400℃).In this work,five Fe-Ce-La oxides were prepared by co-precipitation method,and FeCeLaO/SiO_(2)-Al_(2)O_(3) composite adsorbents were prepared by coupling fly ash-based Si-Al carriers.The active components Fe-Ce-La oxides and Si-Al carriers were characterized by TPD,TG,XRF,BET and XPS,respectively.The effects of temperature,Si/Al ratio and FeCeLaO loading rate on the sulfur resistance were investigated.Results show that the SO_(2) promotes the arsenic removal of Fe_(2)O_(3),CeLaO and FeCeLaO.At 400℃,the arsenic removal efficiencies of the three oxides increase from 45.3%,72.5% and 81.3% without SO_(2) to 62.6%,80.5%and 91.0%,respectively.The SO_(2) inhibits the arsenic removal of La_(2)O_(2)CO_(3) and FeLaO,and the inhibition effect is pronounced at high temperatures.The sulfur poisoning resistance of Si-Al carriers increases with the increase of Si/Al ratio.When the Si/Al ratio is increased to 9.74,the arsenic removal efficiency in the SO_(2) environment is 13.9% higher than that in the absence of SO_(2).Introducing FeCeLaO active components is beneficial for enhancing the SO_(2) poisoning resistance of Si-Al carriers.The strong sulfur resistance of the FeCeLaO/SiO_(2)-Al_(2)O_(3) composite adsorbent results from multiple factors:protective effects of Ce on Fe,La and Al;sulfation-induced generation of Ce^(3+)and surface-adsorbed oxygen;and strong surface acidity of SiO_(2).展开更多
以硝酸铈和尿素为原料,1,3,5苯三甲酸为配体,采用简单的静电自组装法合成了铈金属有机框架(Ce-BTC)和石墨相氮化碳(g-C_(3)N_(4))的复合材料(Ce-BTC/g-C_(3)N_(4)),用于二氧化碳还原制一氧化碳的研究,并探索Ce-BTC的复合对g-C_(3)N_(4)...以硝酸铈和尿素为原料,1,3,5苯三甲酸为配体,采用简单的静电自组装法合成了铈金属有机框架(Ce-BTC)和石墨相氮化碳(g-C_(3)N_(4))的复合材料(Ce-BTC/g-C_(3)N_(4)),用于二氧化碳还原制一氧化碳的研究,并探索Ce-BTC的复合对g-C_(3)N_(4)性能的影响机制。利用X射线衍射、红外光谱、扫描电子显微镜、紫外-可见光吸收光谱、荧光光谱、阻抗、光电流测试和CO_(2)还原性能测试对复合材料的结构、形貌、光电学性能及催化性能进行研究。结果表明Ce-BTC与g-C_(3)N_(4)的复合可能使得g-C_(3)N_(4)层间距发生改变,在细化晶体颗粒的同时提高样品比表面积,使复合样品获得更高的可见光捕获能力且载流子的分离效率更高;在仅加入1 mL H2O作为质子提供源的前提下,Ce-BTC/g-C_(3)N_(4)-3拥有最优光催化性能。CO产率为19.02μmol/(h·g),是g-C_(3)N_(4)的2.25倍,循环测试后催化性能基本保持稳定。展开更多
文摘It is crucial to develop arsenic removal adsorbents with strong sulfur resistance under middle-low-temperature flue gas conditions(<400℃).In this work,five Fe-Ce-La oxides were prepared by co-precipitation method,and FeCeLaO/SiO_(2)-Al_(2)O_(3) composite adsorbents were prepared by coupling fly ash-based Si-Al carriers.The active components Fe-Ce-La oxides and Si-Al carriers were characterized by TPD,TG,XRF,BET and XPS,respectively.The effects of temperature,Si/Al ratio and FeCeLaO loading rate on the sulfur resistance were investigated.Results show that the SO_(2) promotes the arsenic removal of Fe_(2)O_(3),CeLaO and FeCeLaO.At 400℃,the arsenic removal efficiencies of the three oxides increase from 45.3%,72.5% and 81.3% without SO_(2) to 62.6%,80.5%and 91.0%,respectively.The SO_(2) inhibits the arsenic removal of La_(2)O_(2)CO_(3) and FeLaO,and the inhibition effect is pronounced at high temperatures.The sulfur poisoning resistance of Si-Al carriers increases with the increase of Si/Al ratio.When the Si/Al ratio is increased to 9.74,the arsenic removal efficiency in the SO_(2) environment is 13.9% higher than that in the absence of SO_(2).Introducing FeCeLaO active components is beneficial for enhancing the SO_(2) poisoning resistance of Si-Al carriers.The strong sulfur resistance of the FeCeLaO/SiO_(2)-Al_(2)O_(3) composite adsorbent results from multiple factors:protective effects of Ce on Fe,La and Al;sulfation-induced generation of Ce^(3+)and surface-adsorbed oxygen;and strong surface acidity of SiO_(2).
文摘以硝酸铈和尿素为原料,1,3,5苯三甲酸为配体,采用简单的静电自组装法合成了铈金属有机框架(Ce-BTC)和石墨相氮化碳(g-C_(3)N_(4))的复合材料(Ce-BTC/g-C_(3)N_(4)),用于二氧化碳还原制一氧化碳的研究,并探索Ce-BTC的复合对g-C_(3)N_(4)性能的影响机制。利用X射线衍射、红外光谱、扫描电子显微镜、紫外-可见光吸收光谱、荧光光谱、阻抗、光电流测试和CO_(2)还原性能测试对复合材料的结构、形貌、光电学性能及催化性能进行研究。结果表明Ce-BTC与g-C_(3)N_(4)的复合可能使得g-C_(3)N_(4)层间距发生改变,在细化晶体颗粒的同时提高样品比表面积,使复合样品获得更高的可见光捕获能力且载流子的分离效率更高;在仅加入1 mL H2O作为质子提供源的前提下,Ce-BTC/g-C_(3)N_(4)-3拥有最优光催化性能。CO产率为19.02μmol/(h·g),是g-C_(3)N_(4)的2.25倍,循环测试后催化性能基本保持稳定。