In part Ⅰ of this paper series, the application of an incomplete adjoint operator to calculate the optimal reduction of the total emissions S was suggested. This paper, part Ⅱ of the series, focuses on calculating t...In part Ⅰ of this paper series, the application of an incomplete adjoint operator to calculate the optimal reduction of the total emissions S was suggested. This paper, part Ⅱ of the series, focuses on calculating the reduction of the anthropogenic emission source S. As aSc(the source term due to the chemical reaction in the atmosphere) is a complex function of the pollutant concentration, we propose an iterative optimization method using a positive-negative discriminant to obtain Sfrom he aS. Tconvergence of the iterations is also proven in this paper.展开更多
Activated red mud(RM)has been proved to be a promising base material for the selective catalysis reduction(SCR)of NOx.The inherent low reducibility and acidity limited its low-temperature activity.In this work,molybde...Activated red mud(RM)has been proved to be a promising base material for the selective catalysis reduction(SCR)of NOx.The inherent low reducibility and acidity limited its low-temperature activity.In this work,molybdenum oxide,tungsten oxide,and cerium oxide were used to reconfigure the redox sites and acid sites of red mud based catalyst.When activated red mud was reconfigured by cerium-tungsten oxide(Ce-W@RM),the NOx conversion kept above 90%at 219-480℃.The existence of Ce^(3+)/Ce^(4+) redox electron pairs provided more surface adsorbed oxygen(O_(α)) and served as a redox cycle.Positive interactions between Ce,W species and Fe oxide in red mud occurred,which led to the formation of unsaturated chemical bond and promoted the activation of adsorbed NH_(3) species.WO_(3) and Ce_(2)(WO_(4))_(3)(formed by solid-state reaction between Ce and W species)could provide more Brønsted acid sites(W-O modes of WO_(3),W=O or W-O-W modes of Ce_(2)(WO_(4))_(3)).CeO_(2) species could provide more Lewis acid sites.The Langmuir-Hinshelwood(L-H)routes and Eley-Rideal(E-R)routes occurred in the low-temperature SCR reaction on the Ce-W@RM surface.NH_(4)^(+) species on Brønsted acid sites,NH_(3) species on Lewis acid sites,bidentate nitrate and bridging nitrate species were key active intermediates species.展开更多
Commercial V_(2)O_(5)-based catalysts have been successfully applied in NH_(3) selective catalytic reduction(NH_(3)-SCR)of NO_(x) from power stations,but their poor alkali-resistance restrains the wider application in...Commercial V_(2)O_(5)-based catalysts have been successfully applied in NH_(3) selective catalytic reduction(NH_(3)-SCR)of NO_(x) from power stations,but their poor alkali-resistance restrains the wider application in nonelectrical industries.In this study,NO_(x) reduction against alkali poisoning over V_(2)O_(5)/TiO_(2) is greatly improved via Ce(SO_(4))_(2) modification.It has been originally demonstrated that Ce^(4+)-SO_(4)^(2−)pair sites play crucial roles in improving NO_(x) reduction against alkali poisoning over V_(2)O_(5)/TiO_(2) catalysts.The strong interaction between V species and Ce sites of Ce^(4+)-SO_(4)^(2−)pairs triggers the reaction between NH_(4)^(+) species and gaseous NO via Eley-Rideal(E-R)reaction pathway.After K-poisoning,the SO_(4)^(2−)sites of Ce^(4+)-SO_(4)^(2−)pairs as protective sites strongly bond with K and thus maintain the high reaction efficiency via the E-R reaction pathway.This work demonstrates an effective strategy to enhance NO_(x) reduction against alkali poisoning over catalysts via constructing Ce^(4+)-SO_(4)^(2−)pair sites,contributing to developing alkali-resistant SCR catalysts for practical application in nonelectrical industries.展开更多
基金supported by the National Key R&D Program of China(Grant No.2016YFC0209000)the National Natural Science Foundation of China(Grant Nos.41630530&41877316).
文摘In part Ⅰ of this paper series, the application of an incomplete adjoint operator to calculate the optimal reduction of the total emissions S was suggested. This paper, part Ⅱ of the series, focuses on calculating the reduction of the anthropogenic emission source S. As aSc(the source term due to the chemical reaction in the atmosphere) is a complex function of the pollutant concentration, we propose an iterative optimization method using a positive-negative discriminant to obtain Sfrom he aS. Tconvergence of the iterations is also proven in this paper.
基金supported by the National Natural Science Foundation of China(21906090)the National Key Research and Development Program(2017YFC0210200,2017YFC0212800)Primary Research&Development Project of Shandong Province(2018GSF117034,2019JZZY020305).
文摘Activated red mud(RM)has been proved to be a promising base material for the selective catalysis reduction(SCR)of NOx.The inherent low reducibility and acidity limited its low-temperature activity.In this work,molybdenum oxide,tungsten oxide,and cerium oxide were used to reconfigure the redox sites and acid sites of red mud based catalyst.When activated red mud was reconfigured by cerium-tungsten oxide(Ce-W@RM),the NOx conversion kept above 90%at 219-480℃.The existence of Ce^(3+)/Ce^(4+) redox electron pairs provided more surface adsorbed oxygen(O_(α)) and served as a redox cycle.Positive interactions between Ce,W species and Fe oxide in red mud occurred,which led to the formation of unsaturated chemical bond and promoted the activation of adsorbed NH_(3) species.WO_(3) and Ce_(2)(WO_(4))_(3)(formed by solid-state reaction between Ce and W species)could provide more Brønsted acid sites(W-O modes of WO_(3),W=O or W-O-W modes of Ce_(2)(WO_(4))_(3)).CeO_(2) species could provide more Lewis acid sites.The Langmuir-Hinshelwood(L-H)routes and Eley-Rideal(E-R)routes occurred in the low-temperature SCR reaction on the Ce-W@RM surface.NH_(4)^(+) species on Brønsted acid sites,NH_(3) species on Lewis acid sites,bidentate nitrate and bridging nitrate species were key active intermediates species.
基金the National Natural Science Foundation of China(Nos.22125604,22106100,21976117)Shanghai Rising-Star Program(No.22QA1403700)+1 种基金Chenguang Program supported by Shanghai Education Development FoundationShanghai Municipal Education Commission(No.22Z00354).
文摘Commercial V_(2)O_(5)-based catalysts have been successfully applied in NH_(3) selective catalytic reduction(NH_(3)-SCR)of NO_(x) from power stations,but their poor alkali-resistance restrains the wider application in nonelectrical industries.In this study,NO_(x) reduction against alkali poisoning over V_(2)O_(5)/TiO_(2) is greatly improved via Ce(SO_(4))_(2) modification.It has been originally demonstrated that Ce^(4+)-SO_(4)^(2−)pair sites play crucial roles in improving NO_(x) reduction against alkali poisoning over V_(2)O_(5)/TiO_(2) catalysts.The strong interaction between V species and Ce sites of Ce^(4+)-SO_(4)^(2−)pairs triggers the reaction between NH_(4)^(+) species and gaseous NO via Eley-Rideal(E-R)reaction pathway.After K-poisoning,the SO_(4)^(2−)sites of Ce^(4+)-SO_(4)^(2−)pairs as protective sites strongly bond with K and thus maintain the high reaction efficiency via the E-R reaction pathway.This work demonstrates an effective strategy to enhance NO_(x) reduction against alkali poisoning over catalysts via constructing Ce^(4+)-SO_(4)^(2−)pair sites,contributing to developing alkali-resistant SCR catalysts for practical application in nonelectrical industries.
