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.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Catalysis
·
2025
·
IF 13.1
Zhiying Liu,Meiqing Shen,Shuhuan Wang,Chunjuan Zhang,Jun Wang,Wei Li,Feng Gao
To elucidate how CeO2 additives enhance the activity and stability of Cu-SSZ-13 SCR catalysts, we investigated two CeO2/Cu-SSZ-13 composite catalysts with Cu loadings of 1.0 and 2.5 wt %. These catalysts were characterized using an array of techniques, including XRD, SEM, TEM, NMR, H2-TPR, NH3-TPD, DRIFTS, DFT and SCR reactions under both steady-state and transient kinetic analysis conditions. Our findings demonstrate that CeO2 promotes low-temperature SCR by forming exchanged, isolated Ce-ions, which enhance Cu-ion coupling efficiency. External surface CeO2 particles can convert NO + O2 to surface nitrates, but these species primarily act as spectators below ∼250 °C, and do not contribute to the enhancement of low-temperature SCR activity. In contrast, these surface CeO2 particles can synergizes with Brønsted acid sites (BAS) to elevate high-temperature SCR activity. Furthermore, hydrothermal stability and sulfur resistance are improved by the presence of external surface CeO2 particles, a benefit that applies irrespective of Cu loading.
研究领域:
催化
·
环境化学
·
材料科学
·
物理化学
·
表面科学
✓ 已验证
DOI
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
·
环境科学
·
催化材料
✓ 已验证
产品关联
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
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2018
·
IF 4.439
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
✓ 已验证
产品关联
DOI
高影响因子
Advances in Materials Science and Engineering
·
2019
·
IF 1.399
Zhuo Yao,Dianli Qu,Yuxiang Guo,Yujing Yang,Hong Huang
Novel catalysts with high activity for the selective catalytic reduction of NO with NH3 (NH3-SCR) at low temperatures are highly demanded. In this study, mixed-node metal-organic frameworks (MOFs), e.g. Mn@CuBTC with controlled Mn composition in Cu3(BTC)2, were fabricated using postsynthetic exchange method and their structural characteristics and catalytic performances for NH3-SCR reaction were assessed. A series of analyses in terms of structure, surface morphology, texture, and chemical state determined that Mn ions were successfully incorporated into the Cu3(BTC)2 crystal lattice as well as adsorbed on the walls of nanopores in the framework. The pore sizes can be finely tuned in the presence of Mn ions in the cages, which significantly suppressed water adsorption. The NH3-SCR activity of Mn@CuBTC exhibited nearly 100% NOx conversion rate in the temperature range (230–260°C). The superior NH3-SCR performance is attributed to the proper pore sizes, reduced water content, and the synergistic effect between manganese and copper ions in the MOF structure, which enhanced NH3 bound to the active Lewis sites.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
CATALYSIS TODAY
·
2020
·
IF 5.825
Ye Ma,Shichao Han,Qinming Wu,Longfeng Zhu,Huimin Luan,Xiangju Meng,Feng-Shou Xiao
The metal-exchanged zeolites as catalysts have been widely applied in many catalytic reactions , but their syntheses are environmentally unfriendly due to the multiple steps such as ion-exchange for the formation of a large amount of wastes. Herein, we for the first time report a method for one-pot fabrication of metal-zeolite catalysts (M-SSZ-13, M-Beta, M-ZSM-5, and M-EU-1; M = Cu, Co, Ni) from a combination of solvent-free and sodium-free routes by mixing, grinding, and heating the raw materials of aluminosilicate gel, organic templates, and metal-amine complexes. As a typical example, Cu-SSZ-13 zeolite is successfully synthesized from heating the mixture of aluminosilicate gel, organic template, and Cu-amine complex. Catalytic tests in selective catalytic reduction of NO x with NH 3 (NH 3 -SCR) show that the synthesized Cu-SSZ-13 zeolite before and after hydrothermal aging at 750 °C for 16 h are completely comparable with the commercial Cu-SSZ-13 zeolite from the conventional hydrothermal synthesis. Very interestingly, the method in this work has obvious advantages such as high yield, reduced pollutants, and simple process, which should be potentially important for practical applications of the metal-zeolites in the future.
研究领域:
催化化学
·
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
Progress in Natural Science-Materials International
·
2012
·Vol. 22
·期 4
·265-272
·
IF 1.099
Lei Chen,Duan Weng,Zhichun Si,Xiaodong Wu
WO 3 –CeO 2 –TiO 2 catalysts for NO (nitrogen monoxide) reduction by ammonia were prepared by a sol–gel method. The catalysts were characterized by BET, XRD, Raman, NH 3 /NO adsorption and H 2 -TPR to investigate the relationships among the catalyst composition, structure, redox property, acidity and deNO x activity. WO 3 –CeO 2 –TiO 2 catalysts show a high activity in a broad temperature range of 200–480 °C. The low-temperature activity of catalysts is sensitive to the catalyst composition especially under low-O 2 -content atmospheres. It may be related to the synergistic effect between CeO x and WO x in the catalysts. On one hand, the interaction between ceria and tungsten oxide promotes the activation of gaseous oxygen to compensate the lattice oxygen consumed in NH 3 -SCR (selective catalytic reduction) reaction at low temperatures. Meanwhile, the Brønsted acid sites mainly arise from tungsten oxides, Lewis acid sites mainly arise from ceria. Both of the Brønsted and Lewis acid sites facilitate the adsorption of NH 3 on catalysts and improve the stability of the adsorbed ammonia species, which are beneficial to the NH 3 -SCR reaction.
✓ 已验证
DOI
高影响因子
JOURNAL OF THE ENERGY INSTITUTE
·
2018
·
IF 4.217
Shuai-wei Liu,Rui-tang Guo,Xiao Sun,Jian Liu,Wei-guo Pan,Zhi-ling Xin,Xu Shi,Zhong-yi Wang,Xing-yu Liu,Hao Qin
In present study, the poisoning mechanism of Cl on V/TiO 2 catalyst for SCR removal of NOx using NH 3 as the reductant was explored by in situ DRIFT technique. The experimental results revealed that the existence of Cl did not change the SCR reaction mechanism over V/TiO 2 catalyst, which was mainly under the control of both E-R and L-H mechanisms. The deactivation of V/TiO 2 catalyst by Cl was mainly resulted from the inhibited adsorption of NH 3 and NOx species, accompanied by the decrease of the reactivity of adsorbed NH 3 species.
研究领域:
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Xiangsen Xu,Jiangxiao Qiao,Shibo Yu,Jiahao Chen,Yiqing Zeng,Feng Zhang,Zhaoxiang Zhong,Weihong Xing
The rational design of catalysts and the establishment of uniform filter structure are key points in the development of high-performance catalytic filters. To resolve the issue of increased N 2 O concentration in catalysts with high vanadium content at high temperatures, a range of catalytic filters with low vanadium loading were fabricated by partially substituting vanadium in 6VWTi catalysts with transition metals (Mn, Cu, Co and Ce). The experimental results show that the introduction of Ce, which leads to rich surface-adsorbed reactive oxygen species, good redox properties and appropriate surface acidity, thus the 1V5CeWTi/SiC catalytic filter exhibits the highest denitration efficiency (NO conversion ＞90 % at the temperature of 300–500 °C without N 2 O production), presenting significant advantages in contrast to 1VWTi/SiC and 6VWTi/SiC. Furthermore, the preparation technology was optimized to obtain a more uniform structure, which enhanced NH 3 -SCR performance and reduced filter pressure drop. The optimized 1V5CeWTi/SiC also exhibited exceptional resistance to SO 2 + H 2 O and long-term stability for a duration of 200 h at 300 °C, as well as displays a noteworthy efficiency in filtering particulate matter (10 μm SiO 2 ). Therefore, the optimized 1V5CeWTi/SiC catalytic filter holds great potential in the realm of gas purification.
研究领域:
环境工程
·
催化
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2022
·
IF 8.035
Xiaodi Li,Shan Ren,Lian Liu,Xiangdong Xing,Lin Chen,Jiangling Li,Jian Yang,Qingcai Liu
The serious deactivation of denitration catalysts caused by heavy metals still a thorny issue in the practical application of selective catalytic reduction of NO x with NH 3 . Herein, we proposed a novel anti-poisoning strategy by designing SO 4 2− /ZrO 2 superacid supported CeO 2 /ZrO 2 catalyst, and the effect of SO 4 2− /ZrO 2 supported CeO 2 /ZrO 2 for PbO-resistance NO x catalytic reduction was investigated. It was worthy to note that the introduction of solid superacid SO 4 2− /ZrO 2 significantly enhanced catalytic performance over the entire temperature range, with an exceptionally high NO x removal efficiency over 98 % during 250–500 °C. When 2 wt% PbO was deposited on the fresh catalyst, the catalytic activity of CeO 2 /ZrO 2 catalyst decreased obviously, while CeO 2 /ZrO 2 -S catalyst can still maintain a higher NO x conversion over 90 % from 275 to 500 °C. The characterization results confirmed that the introduction of solid superacid SO 4 2− /ZrO 2 enhanced the surface acidity and promoted the transformation from Ce 4+ to Ce 3+ . The results of in situ DRIFTS implied that the Eley-Rideal (E-R) mechanism was obeyed over CeO 2 /ZrO 2 catalyst, and both Eley-Rideal (E-R) and Langmuir-Hinshelwood (L-H) mechanisms were followed over CeO 2 /ZrO 2 -S catalyst in the SCR process. With regard to poisoned catalysts, the NH 3 adsorption was inhibited to some extent, while the reaction mechanism wasn’t changed by PbO poisoning.
研究领域:
催化
·
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
Results in Surfaces and Interfaces
·
2025
·
IF 4.4
Xin Liu,Jinshan Zhang,Xin Wang,Xu Zheng,Yong Du,Meichen Pan,Chen Liu,Hisahiro Einaga,Hajime Hojo,Pengwei Huo
With the increasingly stringent requirements for the treatment of industrial nitrogen oxides (NO x ), ammonia selective catalytic reduction (NH 3 -SCR) has emerged as the most widely adopted denitrification technology in industrial settings. A series of CeNbO x nano-catalyst with varying Nb compositions were synthesized via the solvothermal method for NH 3 -SCR. All the CeNbO x samples presented considerable NO x conversion, exceeding 80% within a broad temperature window of 200-350°C. In addition, the optimal sample shown high stability and strong resistance to SO 2 /H 2 O at 225°C. The influence of Nb element on structural properties of the CeNbO x samples was investigated and elucidated using multiple characterization techniques. The NH 3 -SCR process was further studied by in situ infrared Fourier transform spectroscopy ( in situ FTIR ), temperature-programmed reduction with H 2 (H 2 -TPR) and X-ray photoelectron spectroscopy (XPS), which revealed that the improved NO x conversion can be attributed to the role of Nb in suppressing the crystal growth of CeO 2 , promoting the adsorption of oxygen species, increasing the distribution of Ce and improving the redox ability.
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）