CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Lingqin Meng,Lu Wei,Duan Zhang,Jialong Wang,Yali Wang,Suping Cui
Tl poisons VTi catalysts by forming stable V-O-Tl bonds at V O active sites. • WO 3 provides steric shielding and acts as a sacrificial trap for Tl species. • WO 3 drives the electronic oxidation of highly toxic Tl + to less harmful Tl 3+ . • Optimized VWTi catalysts retain ~80% NO x conversion under cement kiln flue gas. Thallium (Tl), an extremely toxic and highly volatile heavy metal, has become the primary cause of rapid deactivation of V 2 O 5 /TiO 2 (VTi) SCR catalysts used in cement kilns. Industrial post-operation analyses consistently show exceptional Tl enrichment on catalyst surfaces—often 2–3 orders of magnitude higher than other heavy metals—resulting in a sharp decline in NO x removal efficiency and raising significant environmental and operational hazards. Motivated by real industrial observations that appropriate amounts of WO 3 substantially enhance the Tl tolerance of VTi catalysts, this study provides a mechanistic explanation for both the poisoning pathway and the mitigation effect. We demonstrate that Tl deactivation originates from its strong affinity for V O active sites, where it forms stable V-O-Tl bonds that collapse Lewis acidity, suppress oxygen-vacancy regeneration, and disrupt the V 5+ /V 4+ redox cycle essential for SCR activity. Through multi-scale characterization and DFT analysis, we reveal that WO₃ alleviates Tl toxicity through a dual synergistic mechanism: steric shielding that limits Tl access to vanadium centers, and oxidation of mobile Tl + to less reactive Tl 3+ , thereby weakening its ability to bind and deactivate V sites. This cooperative electronic-structural modulation preserves both acidity and redox functionality under realistic high-Tl exposure. The mechanistic insights presented here offer a rational foundation for developing durable, Tl-resistant SCR catalysts tailored for hazardous flue gas environments in cement and waste-incineration industries.
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DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2025
·
IF 11.3
Xinyu Han,Liangliang Jiang,Zeshu Zhang,Kaijie Liu,Mengyao Bian,Zhaoxu Yuan,Yannan Li,Cheng Rao,Xiangguang Yang,Yibo Zhang
Cerium-based catalysts for the selective catalytic reduction of NOx with ammonia (NH3-SCR) face significant challenges in practical applications, particularly their poor low-temperature activity and susceptibility to SO2 poisoning. In this study, photothermal catalysis was innovatively applied to the NH3-SCR reaction over MoWOx/CeO2 catalysts, achieving remarkable improvements in the low-temperature performance and SO2 resistance. Under photothermal conditions, the catalyst maintained NOx conversion above 90% at 200 °C, even in the presence of 250 ppm of SO2. Comprehensive characterization revealed that light irradiation significantly enhanced the formation of oxygen vacancies on the catalyst surface and weakened NO adsorption, indicating that the NH3-SCR reaction follows the Eley–Rideal mechanism, which contributes to its excellent low-temperature activity. Moreover, photothermal conditions reduced the chemical adsorption intensity of SO2, effectively inhibiting the formation of ammonium sulfate. Density functional theory calculations further demonstrated that the narrow band gap of MoWOx promotes electron transfer from the O 2p orbital to the Ce 4f orbital at the Ce–O–Mo(W) interface under light, leading to electron enrichment at active sites and suppression of SO2 oxidation. This work not only provides a novel strategy for enhancing the NH3-SCR performance but also represents a groundbreaking advancement in the design of highly efficient, SO2-resistant catalysts for low-temperature applications.
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Jingyan Zhang,Peng Ji,Li Ren,Yuhong Zhao,Shiqing Li,Hao Xu,Honggen Peng,Jin-Gang Jiang,Yejun Guan,Peng Wu
The small-pore CHA -type zeolites have received intensive attentions due to their outstanding performance in both of the methanol-to-olefin (MTO) process and ammonia selective catalytic reduction of nitrogen oxides (NH 3 -SCR of NO x ) reactions. However, the costly synthesis of CHA -type aluminosilicate is a great issue for the practical application. In this study, a novel and cheap organic structure-directing agent of N,N,N -trimethylisobutylammonium hydroxide was developed and used to synthesize CHA -type zeolites (name as ECNU-25) with boric acid as the supporting agent. The Si/Al ratio in the synthetic gel could be tailored in a wide range of 50 - ∞. [Al,B]-ECNU-25 zeolite thus synthesized served as an effective catalyst for the MTO reaction. After Cu 2+ -exchange, the Cu-[Al,B]-ECNU-25 was also highly active in the NH 3 -SCR of NO x .
研究领域:
化学工程
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环境科学
·
催化材料
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DOI
高影响因子
CATALYSIS COMMUNICATIONS
·
2023
·
IF 3.7
Jiuhu Zhao,Huiying Li,Yungang Wang,Rongshu Zhu,Senlin Sun,Jingwen Zhang,Chaolin Li,Mei Hong
Mesoporous In/Hβ-X series catalysts were prepared by desilication method with tetrapropylammonium hydroxide (TPAOH) and indium incorporation for selective catalytic reduction of NO with methane (CH 4 -SCR). The post desilication treatment conditions for preparing In/Hβ-X were optimized. Etching time is the most important desilication parameter influencing the resulting CH 4 -SCR performance of the catalyst. The In/Hβ-3 sample which was etched for 3 h presents the highest NO x conversion, 22% higher than In/H-Beta counterparts using commercial microporous beta. Obvious analysis reveals that besides generating mesopores, controlled desilication can modulate the proportion of InO + active sites and surface oxygen species, allowing more active sites to be exposed.
研究领域:
催化
·
环境科学
·
化学工程
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DOI
高影响因子
CATALYSIS COMMUNICATIONS
·
2023
·
IF 3.7
Li Guo,Jialing Chen,Shaokang He,Tingyu Liang,Lijun Lu,Shenke Zheng,Xinyue Hu,Lan Yi,Xiaoqin Wu
The [Fe, Al]-FER zeolites, which are prepared from the interzeolite conversion method (from MWW to FER topology) with high Al and Fe content (Si/Al of 8–18 and Si/Fe of 11–13), exhibit excellent catalytic performances and hydrothermal tolerance for NH 3 -SCR reaction. The interzeolite conversion process can be tuned by optimizing the zeolite synthesis conditions such as synthesis gel composition, crystallization time, crystallization temperature, and adding MWW seeds. The work can provide a new strategy to synthesize high Al and Fe content zeolite with high hydrothermal stability for NO x removal.
研究领域:
环境科学
·
催化化学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Jiafan Cheng,Weiman Li,Xiaoze Wang,Haidi Liu,Yunfa Chen
This work is dedicated to fabrication of catalytic fibers for the process of selective catalytic reduction of NO x by NH 3 (NH 3 -SCR). By employing vanadium-titanium as main catalytic components, we investigated the effect of different inorganic supports (glass fiber, aluminum silicate fiber and quartz fiber), preparation methods (a sol–gel method and a hydrothermal method) and loading weight of V 2 O 5 on the NH 3 -SCR performance of catalytic fibers. The catalytic aluminum silicate fiber with 5% vanadium/titanium ratio prepared by a sol–gel method (denoted as V5Ti/AF) showed the best SCR and mass transfer performance. Characterization results indicated that a relatively large surface area, strong acidity, well-dispersed catalyst particles, and good redox and desorption properties derived from the interaction between catalytic components and supports all contributed to the good performance of V5Ti/AF. The pressure drop of catalytic fibers were measured, and the total pressure drop of catalytic fibers and de-dust ceramic membranes was much lower than previously prepared catalytic ceramic membranes, indicating their potential use in the co-processing of dust and gaseous pollutants.
研究领域:
环境科学
·
材料科学
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DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Shibo Yu,Yiqing Zeng,Mengna Zhan,Shule Zhang,Zhaoxiang Zhong
The influence of phosphorus (P) on ammonia selective catalytic reduction (NH 3 -SCR) catalysts has been the subject of considerable scrutiny. Nevertheless, the precise mechanism of its influence remains a matter of contention. Furthermore, the impact of introducing P at varying stages during catalyst preparation process and its different sites within the catalyst structure on performance is frequently disregarded, significantly hindering practical guidance for designing effective modified catalysts. In this study, a series of P-modified CeO 2 /TiO 2 catalysts were synthesized by introducing P at different preparation stages, and various of characterization and comparison experiments were conducted to elucidate the effect of introducing P at different stages on NH 3 -SCR performance of NO x . Results show that introducing P before loading CeO 2 boosts catalyst activity, whereas delaying the introduction of P results in decreased activity and a progressive decline in catalyst performance as the sequence of P introduction is postponed. P introduced earlier tends to be distributed on the surface of the TiO 2 support, which contributes to the dispersion and anchoring of Ce species. In contrast, when the introduction of P was delayed, it tended to be distributed on the surface of the active species, which led to pore plugging and active sites being covered. Secondly, the variation in loading sites resulting from alterations in the stage of P introduction significantly affected on the chemical environment of Ce species, leading to notable differences in the redox capacity of the catalysts. This is the primary reason for the considerable discrepancy in the SCR performance of the catalysts. This study revealed the sensitivity of the stage of P introduction to CeO 2 /TiO 2 catalysts, providing new insights for designing modified CeO 2 /TiO 2 catalysts.
研究领域:
催化化学
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环境科学
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DOI
高影响因子
Journal of Physical Chemistry C
·
2021
·
IF 4.126
Shichao Han,Xiaomin Tang,Ye Ma,Qinming Wu,Jiaqi Shi,Jian Li,Xiangju Meng,Anmin Zheng,Feng-Shou Xiao
The selective catalytic reduction of nitrogen oxide with methane (CH4–SCR) has been considered as an alternative technology for the simultaneous removal of NOx and CH4, and one of the efficient catalysts for this reaction is Co-exchanged SSZ-13 (Co-SSZ-13) zeolite catalyst. However, the preparation of the Co-SSZ-13 zeolite catalyst is costly due to the use of an expensive organic template and Co exchange. We demonstrate here the design of a low-cost cobalt–amine complex (Co–DETA) as a novel structure-directing agent (SDA) for the one-pot synthesis of Co-SSZ-13 zeolite with the assistance of theoretical calculations. Physicochemical characterizations including X-ray diffraction, scanning electron microscopy, N2 sorption, and magic-angle spinning nuclear magnetic resonance show that the Co-SSZ-13 zeolite has good crystallinity, a cubic morphology, a high surface area, and four-coordinated aluminum species. Furthermore, thermogravimetry–differential thermal analysis, Fourier transform infrared spectroscopy, and diffuse reflectance ultraviolet–visible spectroscopy confirm that the Co–DETA complex acts as a SDA for the synthesis of Co-SSZ-13 zeolite. More importantly, the Co-SSZ-13 zeolite exhibits good catalytic performance in the CH4–SCR reaction with 10% H2O in the feed gas stream. The efficient and facile synthesis of Co-SSZ-13 zeolite plus its good catalytic performance might offer a good opportunity for its industrial applications in the future.
研究领域:
材料科学
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环境科学
·
催化化学
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DOI
高影响因子
Catalysis Science & Technology
·
2016
·Vol. 6
·期 14
·5543-5553
·
IF 5.287
Xin Zhao,Lei Huang,Supawadee Namuangruk,Hang Hu,Xiaonan Hu,Liyi Shi,Dengsong Zhang
A novel Zr–CeVO4/TiO2 catalyst was developed for the selective catalytic reduction (SCR) of NO with NH3. Both TiO2 nanosheets (TiO2-NS) and nanoparticles (TiO2-NP) with different crystal facets were used as supports for the catalyst. It was found that the TiO2-NS-supported catalyst showed much better activity, stability and H2O/SO2 durability than the TiO2-NP-supported catalyst. In particular, the catalyst loading amount was much lower than those of previously reported vanadate-based SCR catalysts. The crystal structures and morphologies were analysed by X-ray diffraction (XRD), Raman spectroscopy and (high-resolution) transmission electron microscopy ((HR)TEM). The redox properties, surface active species and acid sites of the catalysts were investigated through hydrogen temperature-programmed reduction (H2-TPR), X-ray photoelectron spectroscopy (XPS), ammonia and nitrogen oxide temperature-programmed desorption (NH3-TPD and NOx-TPD) and in situ diffuse reflectance infrared Fourier transform spectroscopy (in situ DRIFTs) experiments. The improved activity at lower temperature was due to the presence of more active oxygen species and Brønsted acid sites, as well as the formation of NO2 on the surface of the TiO2 nanosheets which have exposed (001) facets. The enhanced stability and H2O/SO2 durability of Zr–CeVO4/TiO2-NS was due to the limited formation of NH4NO3 and (NH4)2SO4/NH4HSO4. The excellent low operation temperature, low vanadium content and absence of WO3(MoO3) in this catalyst indicated that it has promising potential as a SCR catalyst for practical applications.
研究领域:
环境科学
·
催化化学
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DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2019
·
IF 4.63
Yuxing Wang,Qingji Ying,Yaoyu Zhang,Yue Liu,Zhongbiao Wu
In this paper, the reaction behaviors of CH 3 CN catalytic combustion over CuCeO x -HZSM-5 catalysts prepared by the physical mixing and wet impregnation methods were investigated. The experimental results had revealed that the composite catalysts exhibited excellent degradation efficiency and high N 2 selectivity: the Cu-Ce oxides ensured the high activity, and the introduction of HZSM-5 limited the formation of NO x . The involved reaction mechanism was then studied by an in situ DRIFT analysis. It could be deduced that different reaction pathways would occur over CuCeO x and HZSM-5. The catalytic reaction over CuCeO x mainly proceeded via an oxidation pathway. The CN group could be converted to isocyanate species [NCO(a)] which would be further oxidized to NO x . Over HZSM-5, CH 3 CN was mainly hydrolyzed into ammonia. For the CuCeO x -HZSM-5 composite catalysts, the over-oxidation of NCO(a) and NH 3 was inhibited, and an internal selective catalytic reduction (SCR) reaction could occur, thereby greatly improving the N 2 selectivity.
研究领域:
催化化学
·
环境科学
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DOI
高影响因子
FUEL
·
2023
·
IF 7.4
Fengyuan Liu,Junqi Li,Hong Yong Sohn,Chaoyi Chen,Jian Yang,Xudong Liu,Yuanpei Lan,Wei Zhang,Qin Wang,Li Liu
The objective of this work was to clearly elucidate the interactions on Mn-Ce interface and understand how they affect low temperature selective catalytic reduction (SCR) for NO x removal. In this work, three Mn-Ce catalysts in similar particle size and morphology with different Mn-Ce interface areas were prepared. MnO 2 @CeO 2 -F had the tightest and largest amount of Mn-Ce interfaces compared with MnO 2 @CeO 2 -P and MnO 2 -CeO 2 -M, and also exhibited the highest NO conversion degree at 100–150 °C as well as the strongest activity of Mn species and lowest generation of N 2 O. The TG-DTG, XPS and electrochemical impedance spectroscopy results proved the redox of Ce 4+ + Mn 3+ ↔ Ce 3+ + Mn 4+ on the Mn-Ce interface, and MnO 2 @CeO 2 -F had the highest Mn 4+ , Ce 3+ , O α concentrations. The results of the study on the redox reactions during the NH 3 -SCR process provided powerful evidence of the Mn 4+ /Mn 3+ and Ce 3+ /Ce 4+ recycles that are important for low temperature NH 3 -SCR process. Moreover, the Mn-Ce interface was directly proved to benefit the surface acid sites, redox ability, and activity of the adsorbed intermediates. Both the Eley-Rideal (E-R) and Langmuir-Hinshelwood (L-H) reaction mechanisms were observed in the SCR reaction with prepared Mn-Ce materials, where “fast SCR” can be observed with MnO 2 @CeO 2 -F. Moreover, the Mn-Ce interface also lowers the activation energy of the low-temperature SCR process, with MnO 2 @CeO 2 -F having the lowest activation energy. The results from this work offered powerful evidences for the interactions of Mn/Ce redox at the Mn-Ce interface and elucidated clear understanding of the effects of Mn-Ce redox on low-temperature SCR process, which is expected to promote the NO x removal process.
研究领域:
环境科学
·
催化化学
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DOI
高影响因子
VACUUM
·
2026
·
IF 4.3
Yuhao Wang,Jacob Senior Atta Owusu,Min Cui,Mingyu Su,Huqin Zheng,Sameer Shahid,Bingtao Zhao,Jarosław Zuwała,Yaxin Su
To advance hydrocarbon-selective catalytic reduction (HC-SCR) of NOx, ternary mixed metal oxide catalysts (Ni x Co y Ce z -LDO) were synthesized through calcination of layered double hydroxide (LDH) precursors prepared via urea-assisted homogeneous precipitation. The trimetallic catalysts demonstrated enhanced low-temperature activity, improved redox properties, and superior sulfur resistance, attributed to synergistic interactions among Ni, Co, and Ce. In particular, Ni 0.48 Co 0.24 Ce 0.28 -LDO exhibited optimal performance, attaining 96.6% NO conversion with 98.25% N 2 selectivity at 225 °C, while maintaining high stability under 5% O 2 and 0.02% SO 2 . Characterization (XRD, ICP, SEM and BET) confirmed the formation of highly dispersed nanocrystallites with uniformly distributed metals and identified CeO 2 as the dominant crystalline phase, which provided abundant Lewis acid sites for C 3 H 6 activation. XPS and H 2 -TPR results indicated that the incorporation of Ce increased the Ni 3+ /Ni 2+ and Co 3+ /Co 2+ ratios, promoted oxygen vacancy formation, and enhanced catalyst reducibility, while the presence of Ni facilitated the generation of mobile surface oxygen species (O β ). Py-FTIR analysis further revealed that the synergistic interaction between Ni and Co enhanced Lewis acidity by increasing the density of unsaturated cationic sites, explaining why the trimetallic Ni 0.48 Co 0.24 Ce 0.28 -LDO catalyst exhibited the highest Lewis acid content. In-situ DRIFTS demonstrated that both Lewis and Brønsted acid sites promoted the formation of reactive nitrate species, while C 3 H 6 oxidation to formate and acetate intermediates drove the NO X reduction pathway. Based on these results, a reaction mechanism was proposed. Overall, this study provides valuable insights for designing efficient and low-cost catalysts for HC-SCR applications.
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高影响因子
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