TiO_(2)-supported V_(2)O_(5)catalysts are commonly used in NO_(x)reduction with ammonia due to their robust catalytic performance.Over these catalysts,it is generally considered that the active species are mainly deri...TiO_(2)-supported V_(2)O_(5)catalysts are commonly used in NO_(x)reduction with ammonia due to their robust catalytic performance.Over these catalysts,it is generally considered that the active species are mainly derived from the vanadia species rather than the intrinsic structure of V-O-Ti entities,namely the interface sites.To reveal the role of V-O-Ti entities in NH_(3)-SCR,herein,we prepared TiO_(2)/V_(2)O_(5)catalysts and demonstrated that V-O-Ti entities were more active for NO_(x)reduction under wet conditions than the V sites(V=O)working alone.On the V-O-Ti entities,kinetic measurements and first principles calculations revealed that NH_(3)activation exhibited a much lower energy barrier than that on V=O sites.Under wet conditions,the V-O-Ti interface significantly inhibited the transformation of V=O to V-OH sites thus benefiting NH_(3)activation.Under wet conditions,meanwhile,the migration of NH_(4)^(+)from Ti site neighboring the V-O-Ti interface to Ti site of the V-O-Ti interface was exothermic;thus,V-O-Ti entities together with neighboring Ti sites could serve as channels linking NH_(3)pool and active centers for activation of NH_(4)^(+).This finding reveals that the V-O-Ti interface sites on V-based catalysts play a crucial role in NO_(x)removal under realistic conditions,providing a new perspective on NH_(3)-SCR mechanism.展开更多
NH_(3)-SCR(SCR:Selective catalytic reduction)is an effective technology for the de-NO_(x)process from both mobile and stationary pollution sources,and the most commonly used catalysts are the vanadia-based catalysts.A...NH_(3)-SCR(SCR:Selective catalytic reduction)is an effective technology for the de-NO_(x)process from both mobile and stationary pollution sources,and the most commonly used catalysts are the vanadia-based catalysts.An innovative V_(2)O_(5)-CeO_(2)/TaTiO_(x)catalyst for NO_(x)removal was prepared in this study.The influences of Ce and Ta in the V_(2)O_(5)-CeO_(2)/TaTiO_(x)catalyst on the SCR performance and physicochemical properties were investigated.The V_(2)O_(5)-CeO_(2)/TaTiO_(x)catalyst not only exhibited excellent SCR activity in a wide temperature window,but also presented strong resistance to H_(2)Oand SO_(2)at 275◦C.A series of characterizationmethods was used to study the catalysts,including H2-temperature programmed reduction,X-ray photoelectron spectroscopy,NH_(3)-temperature programmed desorption,etc.It was discovered that a synergistic effect existed between Ce and Ta species.The introduction of Ce and Ta enlarged the specific surface area,increased the amount of acid sites and the ratio of Ce^(3+),(V^(3+)+V^(4+))and Oα,and strengthened the redox capability which were related to synergistic effect between Ce and Ta species,significantly improving the NH_(3)-SCR activity.展开更多
基金supported by the National Natural Science Foundation of China (Nos.U20B6004,22072179,and 22276202)the Strategic Priority Research Program of the Chinese Academy of Sciences (No.XDA23010200)+1 种基金the Special project of eco-environmental technology for peak carbon dioxide emissions and carbon neutrality (No.RCEES-TDZ2021-2)the Youth Innovation Promotion Association of the Chinese Academy of Sciences (No.2019045)。
文摘TiO_(2)-supported V_(2)O_(5)catalysts are commonly used in NO_(x)reduction with ammonia due to their robust catalytic performance.Over these catalysts,it is generally considered that the active species are mainly derived from the vanadia species rather than the intrinsic structure of V-O-Ti entities,namely the interface sites.To reveal the role of V-O-Ti entities in NH_(3)-SCR,herein,we prepared TiO_(2)/V_(2)O_(5)catalysts and demonstrated that V-O-Ti entities were more active for NO_(x)reduction under wet conditions than the V sites(V=O)working alone.On the V-O-Ti entities,kinetic measurements and first principles calculations revealed that NH_(3)activation exhibited a much lower energy barrier than that on V=O sites.Under wet conditions,the V-O-Ti interface significantly inhibited the transformation of V=O to V-OH sites thus benefiting NH_(3)activation.Under wet conditions,meanwhile,the migration of NH_(4)^(+)from Ti site neighboring the V-O-Ti interface to Ti site of the V-O-Ti interface was exothermic;thus,V-O-Ti entities together with neighboring Ti sites could serve as channels linking NH_(3)pool and active centers for activation of NH_(4)^(+).This finding reveals that the V-O-Ti interface sites on V-based catalysts play a crucial role in NO_(x)removal under realistic conditions,providing a new perspective on NH_(3)-SCR mechanism.
基金supported by the National Natural Science Foundation of China(Nos.22276182 and 22188102)the Natural Science Foundation of Fujian Province,China(No.2023J06048)the Youth Innovation Promotion Association of Chinese Academy of Sciences(No.2021303).
文摘NH_(3)-SCR(SCR:Selective catalytic reduction)is an effective technology for the de-NO_(x)process from both mobile and stationary pollution sources,and the most commonly used catalysts are the vanadia-based catalysts.An innovative V_(2)O_(5)-CeO_(2)/TaTiO_(x)catalyst for NO_(x)removal was prepared in this study.The influences of Ce and Ta in the V_(2)O_(5)-CeO_(2)/TaTiO_(x)catalyst on the SCR performance and physicochemical properties were investigated.The V_(2)O_(5)-CeO_(2)/TaTiO_(x)catalyst not only exhibited excellent SCR activity in a wide temperature window,but also presented strong resistance to H_(2)Oand SO_(2)at 275◦C.A series of characterizationmethods was used to study the catalysts,including H2-temperature programmed reduction,X-ray photoelectron spectroscopy,NH_(3)-temperature programmed desorption,etc.It was discovered that a synergistic effect existed between Ce and Ta species.The introduction of Ce and Ta enlarged the specific surface area,increased the amount of acid sites and the ratio of Ce^(3+),(V^(3+)+V^(4+))and Oα,and strengthened the redox capability which were related to synergistic effect between Ce and Ta species,significantly improving the NH_(3)-SCR activity.
