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FUEL · 2022 · IF 8.035

SO2 resistance of CeO2- and Co3O4-supported activated carbon during removal of mercury from flue gas: A comparative study

Shengji Wu,Yalun Ma,Wangsheng Yu,Hui Wang,Wei Yang,Lei Che,Zhongxi Han

How to enhance the SO 2 tolerance of transition metal oxide-supported activated carbon is one of the hottest issues in the field of mercury capture from flue gas. Addition of a foreign metal ion to prepare bimetallic adsorbent is a common method of improving the SO 2 tolerance of adsorbent. However, this approach suffers from high cost and a complex preparation process. In this study, CeO 2 - and Co 3 O 4 -supported activated carbon ( m %CeO 2 /AC and m %Co 3 O 4 /AC), with various loading values of active center, were prepared by an incipient wetness impregnation method, and their SO 2 tolerances were compared. The mercury removal performance and SO 2 tolerance of both CeO 2 /AC and Co 3 O 4 /AC could be remarkably improved through increasing the loading amount of the active center. Co 3 O 4 /AC exhibited high affinity with SO 2 , and the chemisorbed oxygen in Co 3 O 4 would be largely consumed, when SO 2 was present in the flue gas, resulting in a significant decrease of mercury removal efficiency. The mercury removal efficiencies of 20%CeO 2 /AC, 40%CeO 2 /AC and 60%CeO 2 /AC were 86.1%, 93.7% and 93.7%, respectively, during removal of mercury from flue gas at 150 °C in the presence of SO 2 . 20%CeO 2 /AC was the optimal adsorbent for mercury capture from flue gas, owing to its excellent mercury removal efficiency, strong SO 2 tolerance and relatively lower cost. The mercury species formed over spent 20%CeO 2 /AC were HgO and HgSO 4 . The HgO was generated through the reaction of mercury and chemisorbed oxygen, while the formation of HgSO 4 was due to the reaction between mercury, SO 2 and chemisorbed oxygen. The regeneration investigation indicated that the activity of spent 20%CeO 2 /AC could be almost fully recovered through a temperature-programmed decomposition and desorption process. The present study showed that the SO 2 tolerance of CeO 2 /AC could be easily improved through regulation of the loading amount of the active center.

研究领域: 环境科学 · 化学工程 · 材料科学
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH · 2016 ·Vol. 24 ·期 1 ·676-684 · IF 2.76

SO2-tolerant and H2O-promoting Pt/C catalysts for efficient NO removal via fixed-bed H2-SCR

Tu Baosheng,Shi Nian,Sun Wei,Cao Limei,Yang Ji

In this paper, Pt supports on carbon black powder (Vulcan XC-72) were synthesized via a hydrothermal method for selective catalytic reduction (SCR) of NO with H 2 in the presence of 2 vol% O 2 over a wide temperature of 20–300 °C. The results showed that the 3 and 5 wt% Pt/C catalysts resulted in high NO conversion (>90 %) over a temperature range of 120 to 300 °C, and the maximum NO conversion of 98.6 % was achieved over 5 wt% Pt/C at 120 °C. Meanwhile, the influence of SO 2 and H 2 O on the catalyst performance of 3 wt% Pt/C was investigated. The catalysts exhibited good SO 2 poisoning resistance when the SO 2 concentration was lower than 260 ppm. Moreover, a positive effect on NO conversion was detected with the addition of 3 and 5 vol% H 2 O in the feed gas stream. TEM image and good NO conversion performance of the Pt/C catalysts

CAS / MDL: 7440-06-4
研究领域: 催化化学 · 环境科学
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH · 2020 ·Vol. 27 ·期 22 ·27663-27673 · IF 3.056

Enhancement of the activity of Cu/TiO2 catalyst by Eu modification for selective catalytic reduction of NOx with NH3

Liu Yuan-zhen,Xu Qi-yan,Guo Rui-tang,Duan Chao-peng,Wu Gui-lin,Miao Yu-fang,Gu Jing-wen

The Cu/TiO 2 catalysts with the addition of Eu were developed by the sol-gel way for the selective catalytic reduction (SCR) of NO x by NH 3 . Activity tests revealed that CuEu/TiO 2 -0.15 catalyst showed the optimal de-NO x performance in a wide temperature range (150–300 °C), along with an admirable SO 2 tolerance. According to characterization analysis, the relationship between the NH 3 -SCR performance and physicochemical characters of samples was explored. The adjunction of Eu on Cu/TiO 2 catalyst can contribute to the formation of a large amount of Cu 2+ , adsorbed oxygen, and acid sites on the catalyst surface. Moreover, the Eu addition on Cu/TiO 2 is favorable to the generation of activated NO x and NH 3 substances adsorbed on the catalyst surface, which would conduce to the NH 3 -SCR process by Langmuir-Hinshelwood (L-H) mechanism effectively.

研究领域: 环境科学 · 催化化学
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Catalysts · 2022 ·Vol. 12 ·期 5 ·534 · IF 4.501

SO2 Tolerance of Rice Hull Ash Based Fe-Cu Catalysts for Low-Temperature CO-SCR of NO

Zhaohui Teng,Shan Huang,Na Li,Qulan Zhou

Rice husk ash (RHA) has potential as a supporter of catalysts. In this research, we studied the activity and SO2tolerance of RHA-based Fe-Cu oxide in the reduction of NO by CO. Characterization methods were employed to study the properties of the catalysts and their SO2tolerance. Activity and SO2resistance were also tested at different temperatures. We recommend two catalysts with SO2resistance ability: Fe0.67Cu0.33/RHA (the highest catalytic activity) and Fe0.8Cu0.2/RHA. The NO removal rate hardly changed with the addition of SO2and was kept at about 100%. However, the CO conversion rate decreased with increasing SO2at the lower reaction temperatures, which may be due to the formation of sulfites. Fortunately, the deactivation was reversible and can be reduced with an increase in the reaction temperature. The results of our research may help promote the application of CO-SCR.Keywords:rice husk ash;Fe-Cu catalysts;NO reduction;SO2resistance;CO-SCR

研究领域: 环境科学 · 催化化学
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Catalysis Science & Technology · 2021 ·Vol. 11 ·期 15 ·5125-5134 · IF 6.119

Application of ReOx/TiO2 catalysts with excellent SO2 tolerance for the selective catalytic reduction of NOx by NH3

Yanke Yu,Xianfang Yi,Jiali Zhang,Zhaojian Tong,Changwei Chen,Mudi Ma,Chi He,Jinxiu Wang,Jinsheng Chen,Bingbing Chen

Non-vanadium-based catalysts with high SO2 tolerance are still interesting in selective catalytic reduction of NO by NH3 (NH3-SCR) and SO2 adsorption is the foremost step for the deactivation of catalysts. In order to alleviate the adsorption of SO2, we fabricated a series of rhenium (Re; without stable sulfate) supported TiO2 catalysts and studied their SO2 tolerance for the first time. Owing to suitable surface acidity and reducibility, ReOx/TiO2 catalysts exhibited satisfactory activity in a wide temperature range of 250–350 °C. As expected, experimental results and DFT calculations indicated that SO2 adsorption on ReOx/TiO2 catalysts was rather weak, thus the catalysts performed excellent SO2 tolerance in the NH3-SCR reaction. Moreover, in situ DRIFTS indicated that the NH3-SCR reaction on ReOx/TiO2 catalysts followed the Eley–Rideal mechanism and SO2 had little effect on the reaction mechanism. Our findings should provide new insights into the development of SCR catalysts with high SO2 tolerance.

CAS / MDL: 13463-67-7
研究领域: 催化化学 · 环境科学
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CHEMOSPHERE · 2023 · IF 8.8

Improved activity and significant SO2 tolerance of Sb–Pd–V oxides on N-doped TiO2 for CB/NOx synergistic degradation

Guobo Li,Yaping Zhang,Peng Wu,Kai Shen,Shule Zhang,Shipeng Ding

The synergistic degradation of VOCs and NO x that were emitted from the incineration of municipal and medical wastes by a single catalyst is challenging, due to the poor activity at low temperatures, and the SO 2 poisoning on the active sites. Herein, N-doped TiO 2 (N–TiO 2 ) was used as the support for designing a highly efficient and stable catalyst system for CB/NO x synergistic degradation even in the presence of SO 2 . The prepared SbPdV/N–TiO 2 catalyst, which presented excellent activity and tolerance to SO 2 in the CBCO + SCR process, was investigated by a series of characterizations (such as XRD, TPD, XPS, H 2 -TPR and so on) as well as DFT calculations . The electronic structure of the catalyst was effectively modulated after N doping, resulting in effective charge flow between the catalyst surface and gas molecules. More importantly, the adsorption and deposition of sulfur species and reaction transient intermediates on active centers were restrained, while a new N adsorption center for NO x was provided. Abundant adsorption centers and superior redox properties ensured smooth CB/NO x synergistic degradation. The removal of CB mainly follows the L-H mechanism, while NO x elimination follows both E-R and L-H mechanisms. As a result, N doping provides a new approach to develop more advanced anti-SO 2 poisoning CB/NO x synergistic catalytic removal systems for extensive applications.

研究领域: 环境科学 · 催化化学
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NEW JOURNAL OF CHEMISTRY · 2024 ·Vol. 48 ·期 10 ·4335-4345 · IF 2.7

Reasonably designed CuSbTiOx series catalysts with high NH3-SCR activity and obviously improved SO2 tolerance

Jiali Zhang,Zhen Yan,Yanke Yu,Yanpeng Li

CuO/TiO2 catalysts with varying Sb doping ratios were synthesized and applied in the NH3-SCR process. The results of activity tests revealed that the addition of Sb effectively enhanced the performance of low-temperature SCR. Particularly, the CuSbTiOx-0.2 catalyst exhibited the highest activity, achieving over 91% conversion at 250 °C, along with the highest N2 selectivity and exceptional resistance to SO2. Comprehensive characterization analyses demonstrated that CuSbTiOx-0.2 possessed a significantly large specific surface area, the strongest surface acidity, and superior redox performance among the catalysts studied. In situ DRIFTS experiments provided further insights, indicating that Sb modification generated more active species, thereby enhancing the reactivity of ad-NH3 and ad-NOx species. The SCR reaction mechanism for CuSbTiOx-0.2 predominantly followed the Langmuir–Hinshelwood (L–H) and Eley–Rideal (E–R) mechanisms. These findings have the potential to advance the development of novel and effective non-vanadium SCR catalysts.

CAS / MDL: 6923-52-0 13463-67-7
研究领域: 环境科学 · 催化材料
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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

Rationally engineered ReOx-CuSO4/TiO2 catalyst with superior NH3-SCO efficiency and remarkably boosted SO2 tolerance: Synergy of acid sites and surface adsorbed oxygen

Yanke Yu,Desheng Wei,Zhaojian Tong,Jinxiu Wang,Jinsheng Chen,Chi He

Ammonia (NH 3 ) is a critical component causing environmental problems like haze and water pollution. Selective catalytic oxidation of ammonia (NH 3 -SCO) to N 2 and H 2 O is a promising method to abate NH 3 emission. However, inferior SO 2 tolerance is still a tremendous challenge to be conquered for present NH 3 -SCO catalysts regarding practical applications. Application of materials which was difficult to be sulfated by SO 2 should be an effective way to solve this problem. Here, a ReO x -CuSO 4 /TiO 2 catalyst which coupled the advantages of ReO x (Rhenium oxides, supplying highly active adsorbed surface oxygen enhancing NH 3 -SCO reaction) and CuSO 4 (providing Brønsted acid sites inhibiting the formation of N 2 O) was rationally fabricated. Results indicated that ReO x -CuSO 4 /TiO 2 catalyst exhibited excellent catalytic performance in NH 3 -SCO with almost 100% of NH 3 oxidized at 300 °C (N 2 selectivity as high as 96%). Crucially, the composite catalyst exhibited incredible activity and stability under harsh reaction conditions toward SO 2 (600 ppm) and H 2 O (4.0 vol%) owing to the superior inhibition capability for SO 2 adsorption. In situ DRIFTS, in situ Raman and in situ XPS demonstrated that the NH 3 -SCO reaction over ReO x -CuSO 4 /TiO 2 catalyst mainly obeyed a N 2 H 4 reaction mechanism and oxidation–reduction circle between Re 7+ and Re 6+ played a vital role. Moreover, SO 2 would not affect this reaction mechanism on ReO x -CuSO 4 /TiO 2 catalyst. The knowledge and understanding reported could provide critical insights for the design and optimization of efficient materials for industrial NH 3 oxidative elimination.

CAS / MDL: 13463-67-7 7758-99-8
研究领域: 催化化学 · 环境科学 · 材料科学
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ACS Catalysis · 2022 · IF 13.7

Negatively Charged Single-Atom Pt Catalyst Shows Superior SO2 Tolerance in NOx Reduction by CO

Yongjun Ji,Shaomian Liu,Shaojia Song,Wenqing Xu,Liang Li,Yu Zhang,Wenxing Chen,Huifang Li,Jingang Jiang,Tingyu Zhu,Zhenxing Li,Ziyi Zhong,Dingsheng Wang,Guangwen Xu,Fabing Su

Pt-based catalysts are promising for the selective catalytic reduction of NOx by CO (CO-SCR), but some technical issues hinder their practical application, including the high Pt loading needed, high reduction temperature, and the low tolerance toward SO2. Here, we report a novel Pt catalyst for CO-SCR, which has negatively charged single-atom Pt embedded on CuO squares, and the latter is supported on CoAlO nanosheets. This Pt–CuO/CoAlO catalyst with an ultra-low Pt loading (0.02 wt %) exhibited 91% NO conversion and 80% N2 selectivity in 3% O2 at 200 °C. More importantly, it showed almost no activity loss in 200 ppm SO2 over a 15 h test. The theoretical calculations reveal that the negatively charged Pt has a stronger NO adsorption ability than the positively charged Pt, and Cu serves as the CO adsorption site. The much-weakened SO2 adsorption on Pt–CuO/CoAlO relative to the NO and CO adsorption effectively avoids the catalyst poisoning by SO2.

CAS / MDL: 10026-22-9
研究领域: 催化化学 · 环境科学
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JOURNAL OF SOLID STATE CHEMISTRY · 2023 · IF 3.3

Metal-organic framework assisted preparation of α-Fe2O3 for selective catalytic reduction of NOX with NH3

Yuting Hu,Ting Cheng,Zhaozhong Jiang,Kai Qin,Han He,Chengzhu Zhu

Fe-MIL-101-NH 2 was prepared by solvothermal method with ferric nitrate and 2-Aminoterephthalic Acid (DBC-NH 2 ), and Fe-MIL-101-NH 2 as precursor was calcined to prepare α-Fe 2 O 3 catalyst. The optimum synthesis condition and the NO conversion efficiency of α-Fe 2 O 3 were systematically investigated, and its crystallinity, micro-morphology and surface acidity were characterized. The results showed that α-Fe 2 O 3 over calcination at 400 °C for 1 h had excellent catalytic activity, SO 2 tolerance, water resistance, and stability. When an initial NO concentration of 500 ppm, the gas hourly space velocity (GHSV) of 35000 h −1 , and a reaction temperature of 350 °C, the NO conversion efficiency of α-Fe 2 O 3 remained above 90 %. The crystal structure of the catalyst was α-Fe 2 O 3 which retained the original octahedral morphology of Fe-MIL-101-NH 2 and increased a lot of new pores, leading to more abundant Lewis acid sites for promoting NO conversion efficiency.

CAS / MDL: 68-12-2
研究领域: 材料科学 · 环境科学 · 化学工程
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FUEL · 2025 · IF 7.5

Highly efficient NOx reduction with superior H2O and SO2 resistance on Ce-Ti/γ-Fe2O3 dual single-atom Catalysts: Synergistic interactions and mechanistic insights

Jianping Ding,Xiaoyan Zhou,Zhengzheng Yang,Changgeng Liu,Mingchao Sun,Congling Yang,Lu Fan

In this study, a novel strategy was proposed for synthesizing dual single-atom Ce-Ti catalysts supported on γ-Fe 2 O 3 via ball milling and calcination. Compared to γ-Fe 2 O 3 and single-atom Ce/γ-Fe 2 O 3 and Ti/γ-Fe 2 O 3 catalysts, the Ce-Ti/γ-Fe 2 O 3 catalyst exhibits superior NO conversion rates and significantly enhanced tolerance to H 2 O and SO 2 at 200–240 °C. These advancements are attributed to the synergistic interactions between Ce and Ti, which enhance redox properties, increase Lewis acid site density, and facilitate the Langmuir-Hinshelwood reaction pathway. In-situ DRIFTS and density functional theory (DFT) analyses revealed the mechanistic role of surface-active oxygen species and intermediate formation in promoting the SCR reaction. The findings provide valuable mechanistic insights and establish a scalable approach for the development of high-performance, environmentally friendly catalysts for industrial NO x removal.

研究领域: 催化化学 · 环境科学 · 材料科学
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APPLIED SURFACE SCIENCE · 2018 · IF 4.439

The promoting effect of CeO2@Ce-O-P multi-core@shell structure on SO2 tolerance for selective catalytic reduction of NO with NH3 at low temperature

Weiyuan Yao,Yue Liu,Zhongbiao Wu

A series of CeO 2 @Ce-O-P “multi-core@shell” catalysts were synthesized in this paper for selective catalytic reduction (SCR) of NO with NH 3 . The experimental results had showed that CeO 2 @Ce-O-P-30:3 yielded best SO 2 tolerance of an over 70% deNO x efficiency at 250 °C in the presence of 100 ppm SO 2 for 20 h, which was much higher compared to pure Ce-O-P and CeO 2 samples. Further characterization results indicated that Ce-O-P coating layer could somewhat inhibit sulfur depositing on the catalysts during SCR reaction in the presence of SO 2 , thereby protecting the active sites from SO 2 poisoning. Especially, O 2 -TPD results illustrated that a great amount of active oxygen species were retained on used CeO 2 @Ce-O-P catalyst after a long term reaction. The synergetic effect of “multi-core@shell” structure could be attributed to such enhanced performances. The “core” CeO 2 devoted abundant active oxygen sites to fulfill the SCR reaction. And the “shell” Ce-O-P could not only provide acid sites, but also protect the active oxygen species by avoiding the over-adsorption of SO 2 on the catalyst. This work could provide a new way to increase the sulfur resistance for low temperature SCR catalysts.

研究领域: 催化化学 · 环境科学
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