Alkali-resistant NO_(x) reduction over FeVO_(4)/TiO_(2)catalysts via regulating the electron transfer between Fe and V

The presence of alkali metals in exhaust gas from stationary resources causes a grand challenge for the practical application of selective catalytic reduction(SCR)of NO_(x) with NH_(3).Here,alkali-resistant NO_(x) reduction has been successfully implemented via tailoring the electron transfer over Fe and V species on FeVO_(4)/TiO_(2)catalysts.The strong interaction between Fe and V induced electron transfer from V to Fe and strengthened the adsorption and activation of NH_(3)and NO over active VO_(x) sites.In the presence of K_(2)O,the strong electron withdrawing effect of Fe offset the electron donating effect of K on the VO_(x) species,thus protecting the active species VO_(x) to maintain the NO_(x) reduction ability.The enhanced adsorption and activation of NH_(3) allowed SCR reaction to proceed via E-R mechanism even after K_(2)O poisoning.This work elucidated the electronic effects on the alkali metals resistance of traditional ferric vanadate SCR catalysts and provided a promising strategy to design SCR catalysts with superior alkali resistance.

NO_(x) reduction against alkali poisoning over Ce(SO_(4))_(2)-V_(2)O_(5)/TiO_(2) catalysts by constructing the Ce^(4+)-SO_(4)^(2−)pair sites

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.

Deactivation mechanisms and anti-deactivation strategies of molecular sieve catalysts for NO_(x)reduction

Molecular sieve catalysts,owing to their unique chemical properties,are widely used as catalysts among various catalytic reactions.Abundant Br?nsted acid sites in molecular sieve catalysts usually enable active components to disperse well on the catalyst surface,and help to adsorb a large number of gas molecules to achieve maximum catalytic performance.Therefore,a variety of molecular sieve catalysts have been developed and used in the selective catalytic reduction of NO_(x)by NH_(3)(NH_(3)-SCR).For example,Cu molecular sieve catalysts such as Cu-SSZ-13 and Cu-SAPO-34 with wide temperature windows and stable structure are considered and applied as commercial catalysts for NO_(x)removal in diesel vehicles for a long time.Although molecular sieve catalysts possess many advantages,they still cannot avoid the serious deactivation caused by various factors in practical applications.In this review,reasons leading to the deactivation of molecular sieve catalysts for NO_(x)reduction in actual working conditions were concluded.The deactivation mechanisms of molecular sieve catalysts for NO_(x)reduction were analyzed and the corresponding anti-deactivation strategies were summarized.Finally,challenges and prospects of molecular sieve catalysts for NO_(x)reduction were also proposed.

Unravelling the Anomalous Coking Resistance over Boron Nitride-Supported Ni Catalysts for Dry Reforming of Methane

Metal oxides have been used as the supports for heterogeneous catalysis formany years,but they still suffer from coking in some high-temperature applications.The main reasons for coking are the uncontrollable dissociation of C-H and the overbalance between carbon deposition and removal.Herein,we find a boron nitride(BN)-immobilized Ni catalyst shows unprecedented coking resistance in dry reforming of methane via the incomplete decomposition of methane.Unlike the Ni-based catalysts supported by traditional metal oxides,BN-supported Ni accelerates the first C-H dissociation while inhibiting the breaking of the final C-H bond;hence,the suppression of the complete decomposition of methane thoroughly addresses the coking issue.This work reveals the fundamental reason for the coking resistance over BN-supported Ni catalysts is selective activation of the C-H bond,which can provide an inspiring idea for other applications.

Hydrothermally stable metal oxide-zeolite composite catalysts for low-temperature NO_(x) reduction with improved N_(2) selectivity

Development of hydrothermally stable,low-temperature catalysts for controlling nitrogen oxides emissions from mobile sources remains an urgent challenge.We have prepared a metal oxide-zeolite composite catalyst by depositing Mn active species on a mixture support of CeO_(2)/Al_(2)O_(3) and ZSM-5.This composite catalyst is hydrothermally stable and shows improved low-temperature SCR activity and significantly reduced N_(2)O formation than the corresponding metal oxide catalyst.Comparing with a Cu-CHA catalyst,the composite catalyst has a faster response to NH_(3) injection and less NH_(3) slip.Our characterization results reveal that such an oxide-zeolite composite catalyst contains more acidic sites and Mn^(3+)species as a result of oxide-zeolite interaction,and this interaction leads to the generation of more NH_(4)^(+)species bound to the Br?nsted acid sites and more reactive NOxspecies absorbed on the Mn sites.Herein,we report our mechanistic understanding of the oxide-zeolite composite catalyst and its molecular pathway for improving the low-temperature activity and N_(2) selectivity for NH_(3)-SCR reaction.Practically,this work may provide an alternative methodology for low-temperature NO_(x) control from diesel vehicles.

Unraveling SO_(2)-tolerant mechanism over Fe_(2)(SO_(4))_(3)/TiO_(2) catalysts for NO_(x) reduction

Developing low-temperature SO_(2)-tolerant catalysts for the selective catalytic reduction of NO_(x) is still a challenging task.The sulfation of active metal oxides and deposition of ammonium bisulfate deactivate catalysts,due to the difficult decomposition of the as-formed sulfate species at low temperatures(<300℃).In recent years,metal sulfate catalysts have attracted increasing attention owing to their good catalytic activity and strong SO_(2) tolerance at higher temperatures(>300℃);however,the SO_(2)-tolerant mechanism of metal sulfate catalysts is still ambiguous.In this study,Fe_(2)(SO_(4))_(3)/TiO_(2) and Ce_(2)(SO_(4))_(3)/TiO_(2) catalysts were prepared using the corresponding metal sulfate salt as the precursor.These catalysts were tested for their low-temperature activity and SO_(2) tolerance activity.Compared to Ce_(2)(SO_(4))_(3)/TiO_(2),Fe_(2)(SO_(4))_(3)/TiO_(2) showed significantly better low-temperature activity and SO_(2) tolerance.It was demonstrated that less surface sulfate species formed on Fe_(2)(SO_(4))_(3)/TiO_(2) and Ce_(2)(SO_(4))_(3)/TiO_(2).However,the presence of NO and O_(2) could assist the decomposition of NH_(4)HSO_(4) over Fe_(2)(SO_(4))_(3)/TiO_(2) at a lower temperature,endowing Fe_(2)(SO_(4))_(3)/TiO_(2) with better low-temperature SO_(2) tolerance than Ce_(2)(SO_(4))_(3)/TiO_(2).This study unraveled the SO_(2)-tolerant mechanism of Fe_(2)(SO_(4))_(3)/TiO_(2)at lower temperatures(<300℃),and a potential strategy is proposed for improving the low-temperature SO_(2)-tolerance of catalysts with Fe_(2)(SO_(4))_(3) as the main active component or functional promoter.

Shape and size effects of ceria nanoparticles on the impact strength of ceria/epoxy resin composites

Ceria nanoparticles with various shapes （rods, cubes, and plates） and sizes were controllably synthesized and then introduced into epoxy resin. Subsequently, we investigated correlations between the shape and size of ceria nanostructures and the mechanical performance of composites. The samples were character- ized by transmission electron microscopy, scanning electron microscopy, and X-ray diffraction. Compared with commercial ceria filled composites, the composites made with morphology-controlled ceria nanos- tructures show a higher impact strength. It is found that epoxy resins made with high-aspect-ratio ceria nanorods show the highest impact strength, up to 17.27 kJ/m2, which is about four times that of the neat epoxy resin.