Search Results (245)

The commercialization of V-based catalysts for the selective catalytic reduction of NOx by NH₃ (NH₃-SCR) is hindered by their narrow operating temperature window, insufficient low-temperature (LT) activity, and severe SO₂-to-SO₃ oxidation. To bridge this gap, we herein introduced Nb and hexagonal BN into a VW/TiO₂ system to simultaneously enhance its LT SCR activity, suppress undesired side reactions, and improve durability. Nb incorporation promoted V⁵⁺/V⁴⁺ redox cycling and enhanced lattice oxygen mobility, thus reducing the apparent activation energy and suppressing SO₂ oxidation at elevated temperatures. However, excessive Nb loading induced NH₃ oxidation and N₂O formation. This drawback was mitigated by introducing BN as a dispersion promoter, which helped secure high catalytic performance at a reduced Nb content. The VWNb/Ti-BN catalyst achieved superior NOx conversion and N₂ selectivity over a wide temperature range and benefited from notably suppressed NH₃ oxidation and SO₂-to-SO₃ oxidation. Kinetic analysis revealed that Nb primarily lowered the reaction energy barrier via redox property enhancement, whereas BN accelerated surface reaction turnover by stabilizing and dispersing active acidic sites, markedly increasing the turnover frequency without reducing the activation energy. In situ spectroscopic analysis confirmed the accelerated consumption of adsorbed NH₃ species and enhanced formation of reactive NOx intermediates, indicating SCR pathway enhancement. After aging in the presence of SO₂ and H₂O, the best-performing honeycomb-type monolithic catalyst retained and NOx conversion of >80%, demonstrating excellent long-term durability under practical conditions. A composition-aware machine learning model based on log-ratio-transformed variables quantitatively identified the synergistic balance among V, Nb, W, BN, and TiO₂ as the dominant factor governing LT SCR performance. Thus, this work provides valuable mechanistic insights and a strategy for designing wide-temperature-window SCR catalysts with improved activity, selectivity, and resistance to sulfur poisoning. Full article

Nitrogen oxides represent a major source of concern related to atmospheric pollution, causing substantial impacts on human health. One innovative approach to reducing these emissions, and a promising alternative to conventional methods using NH₃, is selective catalytic reduction with carbon (SCR-C). The aim of this study is the development of carbon-based catalysts that are active in the reduction of NO. For that, carbon nanotubes were subjected to treatments to modify their surface chemistry, including introducing oxygen and nitrogen groups, as well as potassium (K) and copper (Cu) incorporated as metal phases. In their original form, carbon nanotubes do not exhibit catalytic activity in reducing NO. However, catalytic performance is significantly improved by the addition of surface groups and Cu. Adding K to the support notably contributes to increasing the catalytic performance. N-doped carbon nanotubes impregnated with copper and potassium (CNT_M_BM@5Cu5K) achieved complete NO reduction at 360 °C. In this catalytic system, the formation of CO₂ and N₂ was observed and CO was not identified. Furthermore, although N₂O was detected during the reaction, its amount was very low compared to the N₂ and CO₂ products. The stability of this catalyst was investigated over 87 h continuous test, revealing deactivation after 41 h of reaction. Full article

A series of novel Ce-modified MnCoAl layered double oxides (Ce/MCA LDOs) were prepared using solvothermal and impregnation methods for NH₃-SCR denitration. Various characterizations, such as X-ray diffraction (XRD), scanning electron microscope (SEM), X-ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM), and H₂ temperature-programmed reduction (H₂-TPR) were used to investigate their structural properties and the mechanism of ammonia selective catalytic reduction (NH₃-SCR). The incorporation of Ce was found to effectively integrate into the LDO framework and enhance the catalytic activity over a wide temperature window. Moreover, the thermal stability and resistance of H₂O and SO₂ were evaluated. In situ DRIFTS studies revealed that the reaction follows both the “Langmuir–Hinshelwood” (L–H) and “Eley–Rideal” (E–R) mechanisms. This work provides systematic insights into the design of LDO-based catalysts, demonstrating their potential for practical application in denitration. Full article

Gas turbines operate at exhaust gas temperatures exceeding 500 °C. Vanadium-based catalysts encounter challenges in NH₃-SCR denitrification due to vanadium volatilization and titanium dioxide support phase transition at high temperatures. This restricts the effective denitrification temperature range to 300~400 °C, falling short of gas turbine denitrification requirements. Zeolite-supported catalysts, known for their high specific surface area, abundant acid sites, and stable framework structure, demonstrate superior catalytic activity and hydrothermal stability at high temperatures. This review synthesizes recent advancements in high-temperature catalysts utilizing ZSM-5, Beta, SSZ-13, and SAPO-34 zeolites as supports. It elucidates the interaction mechanisms between active components (e.g., transition metals Fe, Cu, W, rare earth elements) and zeolite supports. Furthermore, it examines variations in denitrification performance through the lens of the high-temperature NH₃-SCR reaction mechanism, offering valuable insights for high-temperature denitrification catalyst development. Full article

High denitration efficiency and strong adaptability to flue gas temperature fluctuations are the core properties of the NH₃-SCR catalyst. In this study, Fe₂O₃ modification is used as a means to explore the mechanism of adding Fe₂O₃ to broaden the temperature range of the 6CeO₂-40MnO₂/TiO₂ catalyst during the preparation process. The results show that the 6Fe₂O₃-6CeO₂-40MnO₂/TiO₂ catalyst exhibits excellent denitration performance, with a denitration efficiency higher than 90%. The temperature range is from 129 to 390 °C. N₂ selectivity and resistance to SO₂ and H₂O are good, and the denitration performance is significantly improved. When the Fe₂O₃ content is 6%, it promotes lattice shrinkage of TiO₂, improves its dispersion, refines the grain size, and increases the specific surface area of the catalyst. At the same time, Fe₂O₃ enhances the chemical adsorption of oxygen on the catalyst surface and increases the proportion of low-cost metal ions, thereby promoting electron transfer between active elements, generating more surface reactive oxygen species, increasing the oxygen vacancy content and adsorption sites for NO_x and NH₃, and significantly improving the redox performance of the catalyst. This effect is particularly conducive to the formation of strong acid sites on the catalyst surface. The NH₃-SCR reaction on the surface of the 6Fe₂O₃-6CeO₂-40MnO₂/TiO₂ catalyst follows both the L-H and E-R mechanisms, with the L-H mechanism being dominant. Full article

Nitrogen oxides (NO_x), one of the major air pollutants, not only are key substances in forming acid rain and photochemical smog, but can also enter the stratosphere and damage the ozone layer to some extent. The selective catalytic reduction (NH₃-SCR) technology has been widely utilized in industrial flue gas treatment for its efficient removal of NO_x. In recent years, nitrogen-doped carbon materials (NC) have emerged as a novel type of environmentally friendly catalyst, showing outstanding performance in the low-temperature NH₃-SCR reaction. This paper reviews the application advancements of nitrogen-doped carbon materials in the NH₃-SCR reaction, with a focus on the catalytic mechanisms, modification strategies, and stability issues. This paper analyzes multiple improvement ideas, such as regulating metal types and distributions to achieve synergy effects, optimizing carrier loading, and designing morphology structures, and discusses how these measures jointly act to enhance the overall performance of the catalyst. Finally, solutions to the deactivation problem of NC catalysts are proposed, and the future research directions are explored to meet the increasingly stringent environmental protection requirements and promote the development of related technologies. Full article

Copper and iron species were co-deposited onto a hydroxyapatite surface to produce bimetallic catalysts. Characterization techniques (XRD, XPS, DR-UV spectroscopy and TEM-EDX) helped in unveiling the speciation, nuclearity, and electronic properties of copper and iron in samples with variable total metal loading (1–10 wt.%) and relative Cu-to-Fe ratios. The speciation of Cu was revealed to be not affected by Fe and vice versa. Conversely, the metal loading turned out to be a key factor ruling the aggregation state of Cu and Fe species. The samples were tested as catalysts in the Selective Catalytic Reduction of NO by NH₃ (NH₃-SCR) in dry and wet environments under quasi-real conditions (50,000 ppm O₂; 50,000 ppm H₂O, if present; 120,000 h⁻¹ GHSV) in the 200−500 °C interval. Although the combination of Cu and Fe affords a modest improvement in water resistance compared to their monometallic counterparts, no substantial enhancement in activity was observed for the bimetallic hydroxyapatite-based SCR catalysts. Full article

Advancing catalysts for low-temperature NH₃-SCR enhances their viability as a terminal flue gas denitration solution across diverse operating regimes. A high-performance, hydrothermally stable catalyst for low-temperature SCR was synthesized by depositing MnO_x onto MgAlO_x composite oxide supports. These supports, featuring varied Mg/Al ratios, originated from layered double hydroxide (LDH) precursors. The obtained catalyst with the Mg/Al ratio of 2 (Mn/Mg₂AlO_x) possesses relatively high concentrations of active oxygen species (O_α) and Mn⁴⁺ and exhibits remarkable catalytic performance. The Mn/Mg₂AlO_x catalyst exhibits a wide operating temperature range (100–300 °C) for denitration, achieving over 80% NO_x conversion, along with robust water resistance. The temperature-programed surface reactions and NO oxidation reactions are performed to elucidate the promoting effect of water on N₂ selectivity, which is not only due to inhibition of catalyst oxidation capacity at high temperature but also is related to the competing adsorption of water and NH₃. In situ DRIFTS analysis confirmed that the NH₃-SCR mechanism over Mn/Mg₂AlO_x adheres to the Eley–Rideal (E–R) pathway. These findings highlight the significant promise of Mn/MgAlO_x catalysts for deployment as downstream denitration units within exhaust treatment systems. Full article

The pathways and mechanistic aspects of H₂-SCR over precious metal-based catalysts is still under debate. This study focusses on low loaded platinum-based catalysts (0.07–0.3%) in a large temperature range (50–500 °C), with special focus on (i) the role of NH₃ as a possible intermediate species, (ii) the origin of the undesired N₂O emission and (iii) the platinum sites involved in the H₂-SCR deNO_X reactions. Up to 60 °C, the N₂O selectivity was close to 100%, with no influence of the presence of oxygen in the 50–100 °C temperature range. Ammonia formation was observed at relatively low temperatures (from 60 °C), but its reactivity was then limited. All these low temperature reactions were associated with the same platinum sites, probably a mix of edge and face sites. The maximum outlet NH₃ was observed around 100 °C and the role of the NH₃-SCR in the whole H₂-SCR process appeared very limited. On the contrary, the ammonia oxidation by O₂, which started near 120 °C, significantly contributed to the H₂-SCR process and appeared responsible for the second N₂O emission peak (150–500 °C). This reaction did not imply the same platinum sites and appears mainly dependant on the platinum particle size. Full article

The rational design of high-performance Cu-SSZ-13 catalysts with enhanced low-temperature activity represents a critical challenge for meeting stringent Euro VII emission standards in diesel aftertreatment systems. Elevating Cu loading can theoretically improve catalytic performance; however, one-time ion exchange using common CuSO₄ solution makes it hard to accomplish high Cu-ion contents. Herein, we demonstrate that the conventional ion-exchange method, adopting Cu(CH₃COO)₂ as precursor in NH₄-SSZ-13 zeolite with a low Si/Al ratio (≈6–7), can achieve higher Cu content while maintaining superior dispersion of active sites. Comprehensive characterizations reveal a dual incorporation mechanism: canonical Cu²⁺ ion exchange and unique adsorption of the [Cu(CH₃COO)]⁺ complex. In the latter case, the surface-adsorbed [Cu(CH₃COO)]⁺ ions form high-dispersion CuO_x species, while the framework-confined ones convert to active Z[Cu²⁺(OH)]⁺ ions. The Cu(CH₃COO)₂-exchanged Cu-SSZ-13 catalyst exhibits superior low-temperature SCR activity and hydrothermal stability to its CuSO₄-exchanged counterpart, making it particularly suitable for close-coupled SCR applications. Our findings provide fundamental insights into Cu speciation control in zeolites and present a scalable, industrially viable approach for manufacturing next-generation SCR catalysts capable of meeting future emission regulations. Full article

The efficient simultaneous removal of NO_x and CO from sintering flue gas under low-temperature conditions (110–180 °C) in iron and steel enterprises remains a significant challenge in the field of environmental catalysis. In this study, we present an innovative strategy to enhance the performance of CuSmTi catalysts through silver modification, yielding a bifunctional system capable of oxygen structure regulation and demonstrating superior activity for the combined NH₃-SCR and CO oxidation reactions under low-temperature, oxygen-rich conditions. The modified AgCuSmTi catalyst achieves complete NO conversion at 150 °C, representing a 50 °C reduction compared to the unmodified CuSmTi catalyst (T_100% = 200 °C). Moreover, the catalyst exhibits over 90% N₂ selectivity across a broad temperature range of 150–300 °C, while achieving full CO oxidation at 175 °C. A series of characterization techniques, including XRD, Raman spectroscopy, N₂ adsorption, XPS, and O₂-TPD, were employed to elucidate the Ag-Cu interaction. These modifications effectively optimize the surface physical structure, modulate the distribution of acid sites, increase the proportion of Lewis acid sites, and enhance the activity of lattice oxygen species. As a result, they effectively promote the adsorption and activation of reactants, as well as electron transfer between active species, thereby significantly enhancing the low-temperature performance of the catalyst. Furthermore, in situ DRIFTS investigations reveal the reaction mechanisms involved in NH₃-SCR and CO oxidation over the Ag-modified CuSmTi catalyst. The NH₃-SCR process predominantly follows the L-H mechanism, with partial contribution from the E-R mechanism, whereas CO oxidation proceeds via the MvK mechanism. This work demonstrates that Ag modification is an effective approach for enhancing the low-temperature performance of CuSmTi-based catalysts, offering a promising technical solution for the simultaneous control of NO_x and CO emissions in industrial flue gases. Full article

The combustion of biomass fuels releases alkali metals, which induce severe catalyst deactivation due to alkali metal (K) poisoning in low-temperature ammonia selective catalytic reduction (NH₃-SCR) systems. To address this issue, this study developed a series of heteropoly acid (HPA)-modified Ce/AC catalysts prepared via incipient wetness impregnation. The low-temperature NH₃-SCR performance (80–200 °C) of these catalysts was systematically evaluated, with particular emphasis on their denitrification activity and K-poisoning resistance. The silicotungstic-acid (TSiA)-modified Ce/Ac (TSiA-Ce/AC) catalyst showed an improvement (>20%) in NO conversion activity under the K poisoning condition. The superior K-poisoning resistance of the TSiA-Ce/AC catalyst was attributed to the high density of Brønsted acidic sites and the strong K binding affinity of TSiA, which together protected active sites and preserved the standard SCR reaction pathway under K contaminations. This study proposes a novel strategy for enhancing catalyst K resistance in low-temperature NH₃-SCR systems. Full article

Nitrogen oxides (NO_x), harmful pollutants primarily from fossil fuel combustion, pose significant environmental and health risks. Among mitigation technologies, NH₃-SCR is widely adopted due to its high efficiency and industrial viability. MnO₂-based catalysts, particularly α-MnO₂, have gained attention for low-temperature NH₃-SCR owing to their redox properties, low-temperature activity, and environmental compatibility. In this study, α-MnO₂ catalysts with tunable oxygen vacancy concentrations were synthesized by varying calcination atmospheres. Compared to α-MnO₂-Air, the oxygen vacancy-rich α-MnO₂-N₂ exhibited stronger acidity, enhanced redox properties, and superior NH₃/NO adsorption and activation, achieving 98% NO conversion at 125–250 °C. Oxygen vacancies promoted NH₃ adsorption on Lewis/Brønsted acid sites, facilitating -NH₂ intermediate formation, while enhancing NO oxidation to reactive nitrates. In situ DRIFTS revealed a dual E-R and L-H reaction pathway, with oxygen vacancies crucial for NO activation, intermediate formation, and N₂ generation. These findings underscore the importance of oxygen vacancy engineering in optimizing Mn-based SCR catalysts. Full article

Platinum was supported on ZSM5 at loadings from 0.1 to 1 wt% and tested for the Selective Catalytic Reduction of NO with H₂ under excess O₂ in a fixed bed reactor to address the issue of NO_x emission abatement from H₂-fueled internal combustion engines avoiding the additional devices for urea storage and injection. To reduce the undesired NO oxidation to NO₂, which is activated by platinum at T > 200 °C, the 0.1%Pt/ZSM5 catalyst was further promoted with sodium. 5 wt% loading of Na strongly inhibited the NO oxidation while giving only a limited impact on the H₂-SCR activity. Unpromoted and Na-promoted catalysts were characterized by XRD, SEM/EDX, N₂ physisorption, and NH₃-TPD to investigate the morphological, structural, and acid properties; H₂ pulse chemisorption and DRIFTS of CO chemisorption were used to investigate the nature of Pt active species. Steady-state and transient operando DRIFTS experiments under NO+H₂+O₂ flow were employed to identify the adsorbed NO_x species interacting with H₂, and reaction intermediates as a function of the reaction conditions. The formation of ammonium intermediates via the reduction of surface nitrate species, playing a key role in H₂-SCR catalyzed by 0.1Pt/ZSM5, was preserved at low Na load whilst NO₂ formation was largely inhibited. Full article

To develop eco-friendly low-temperature NH₃-SCR catalysts for the non-electric industry, a series of CeMn-modified Ba₂Ti₅O₁₂ catalysts were synthesized using the sol-gel method to achieve denitrification. Activity tests revealed that Ce-Mn-modified Ba₂Ti₅O₁₂ catalysts exhibit excellent low-temperature denitrification performance with a broad operational temperature window. Characterization through XRD, XPS, BET, NH₃-TPD, and EPR indicated that Ce-Mn modification enhances surface oxygen chemisorption and increases acidity, significantly improving NO_x reduction. Notably, the optimal catalyst achieved NO_x conversion rates exceeding 90% within the temperature range of 90 to 240 °C under a gas hourly space velocity (GHSV) of 28,000 h⁻¹. In particular, the coexistence of Ce and Mn species promotes the oxidation of NO to NO₂, facilitating the “fast SCR” reaction. The abundance of valence states further enhances the catalyst’s ultra-low-temperature NH₃-SCR denitration performance. Full article