Journal of Environmental Chemical Engineering
·
2021
·
IF 5.909
Zhifei Hao,Guoquan Liu,Nan Ma,He Zhang,Yi Li,Yuguo Xia,Dongpeng Zhang,Sihui Zhan
Acidity and redox properties of the catalyst are two crucial factors affecting the performance of NH 3 -SCR. Herein, we design a novel WO x /Cu-CeO 2 oxide catalyst in which the WO x species are highly dispersed on the {111}/{100}-terminated surface of Cu-doped CeO 2 nanospheres , which exhibits great deNO x activity advantage and wide operating temperature window (200–400 °C, over 85% NO x conversion with a gas hourly space velocity (GHSV) of 60,000 h −1 ), as well as good sulfur resistance and N 2 selectivity . The relationship among the composition, acidity and redox properties of the WO x /Cu-CeO 2 catalyst is established in the NH 3 -SCR reaction. The combined experimental studies and spectroscopic characterization reveal that the introduction of Cu into the lattice of CeO 2 not only increases the surface Ce 3+ and oxygen vacancy concentration but also provides more sites for capture and dispersion of WO x species, thus mediating and improving the Lewis and Brønsted acid sites and reducibility of catalyst. XPS and DFT calculations further demonstrate that electronic interaction between WO x and Cu-doped CeO 2 is enhanced duo to the existence of interactions of short-range Ce-O-Cu and Ce-O-W. Moreover, the NH 3 -SCR reaction over WO x /Cu-CeO 2 may follow both Langmuir-Hinshelwood and Eley-Rideal reaction pathway according to the in situ DRIFTS.
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
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Wenqi Liu,Jingyan Zhang,Mei Dong,Zhaoyi Ding,Qunfei Wang,Fanghao Ning,Qin He,Yanyan Chen,Zhen Zhao,Zhongfu Li,Conghua Liu
Low-silica chabazite (CHA) catalysts with varying configurations of Cu 2+ -2Z and [Cu(OH)] + -Z active centers are developed through the regulation of the opening of CHA-cages. The catalysts are subsequently applied to the selective catalytic reduction of NO x by NH 3 (NH 3 -SCR) reactions. A series of characterizations and performance evaluations indicate that the density of [Cu(OH)] + -Z in eight-member rings (8MRs) is positively correlated with low-temperature performance. Moreover, the presence of partial Cu 2+ -2Z in six-member rings (6MRs) enhances activity and tolerance at high temperatures. The residual K + ions in the CHA-cages after NH 4 + exchange are retained in the 6MRs. Density functional theory calculations demonstrate that the residual K + ions stabilize the 6MRs structure, ensuring the entry and stable presence of the active Cu 2+ -2Z centers. In situ analysis reveals the reaction intermediates involved in the NH 3 -SCR process on representative catalysts. These findings can further elucidate the active centers of CHA-type catalysts and guide the design of commercial 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
Journal of Environmental Chemical Engineering
·
2024
·
IF 7.4
Yanli Zhang,Jian Li,Jianyu Cai,Shuangye Li,Xing Fan,Liyun Song,Ruixue Guo,Jiasheng Liu
In this study, a series of γ-Fe 2 O 3 -modified V 2 O 5 -MoO 3 /TiO 2 (VMT) catalysts was prepared by wet impregnation method. The γ-Fe 2 O 3 -modified catalysts exhibited excellent catalytic performance, and 1.25 wt% γ-Fe 2 O 3 content improved the deNO x efficiency at 150 °C from 54% (unmodified VMT catalyst) to 84% (modified catalyst). BET, XRD, XPS, NH 3 -TPD, H 2 -TPR, and in situ DRIFTs were employed to characterize the physicochemical properties and reaction mechanisms of the catalysts. The introduction of γ-Fe 2 O 3 increased the V 5+ /V 4+ ratio, surface chemisorbed oxygen content, redox ability, and a number of acid sites in the prepared catalysts. XPS confirmed the addition of γ-Fe 2 O 3 introduced new charge transfer pathways (Fe 3+ /Fe 2+ ↔ V 5+ /V 4+ ). In situ DRIFTs suggested that the addition of γ-Fe 2 O 3 to the catalyst significantly increased the adsorption capacity of catalyst for NH 3 and NO x , while also exerting a strong activating effect on the adsorbed NH 3 . Furthermore, selective catalytic reduction over the VMT and 5PEG@1.25Fe-VMT catalysts followed the Eley-Rideal (E-R) mechanism. At temperatures above 200 °C, the 5PEG@1.25Fe-VMT catalyst also followed the Langmuir-Hinshelwood (L-H) mechanism.
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
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2018
·
IF 5.091
Yiqing Zeng,Yanan Wang,Shule Zhang,Qin Zhong,Weilong Rong,Xiaohai Li
In this work, novel (CeO 2 ) x -(CePO 4 ) 1−x (defined as Ce x P 1−x ) nanorod composites were prepared by a simple co-precipitation method, and the influence of CeO 2 on the catalytic performance of CePO 4 for selective catalytic reduction of NO by NH 3 (NH 3 -SCR of NO) was investigated. The catalytic performance evaluation revealed that the Ce x P 1−x catalysts, especially Ce 0.2 P 0.8 exhibited a much better catalytic activity and H 2 O + SO 2 resistance than CePO 4 . Structure characterizations via high-resolution transmission electron microscope (HRTEM) and Brunauer-Emmett-Teller (BET) revealed that the introduction of CeO 2 had a little effect on the shape of CePO 4 nanorods and it could promote the formation of new mesoporous then significantly enhance the surface area of catalyst. The analysis results of active sites suggested that phosphorus was the main adsorption site for NH 3 and the redox sites were controlled by CeO 2 on Ce x P 1−x catalysts. Finally, reaction process study demonstrated that the NH 3 -SCR over Ce x P 1−x was processed via Langmuir-Hinshelwood (L-H) mechanism. Combining the results of active sites and reaction mechanism analysis, it was drawn that the superior low temperature activity of Ce x P 1−x could be attributed to its excellent redox properties, which promoted the oxidation of NO then facilitated the process of NH 3 -SCR via “fast SCR”.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2014
·
IF 4.058
Jiancheng Wang,Zhaoliang Peng,Ying Chen,Weiren Bao,Liping Chang,Gang Feng
Cu-SSZ-13/cordierite monolithic catalyst was prepared by in situ hydrothermal synthesis method. The physicochemical properties of the as-prepared Cu-SSZ-13/cordierite were investigated by X-ray diffraction analysis, scanning electron microscopy, transmission electron microscopy, N 2 -adsorption, inductively coupled plasma, X-ray photoelectron spectroscopy, and solid-state NMR techniques. The removal of nitrogen oxides (NO x ) from simulated diesel vehicle exhaust gas was performed using fixed-bed reactor. The effects of crystallization time and addition of HF during hydrothermal synthesis, reaction space velocity, and aging treatment of catalyst on the catalytic performances of NO x reduction reactions were investigated. The results indicate that the optimum crystallization time was 72 h. Highly crystalline structure of zeolite Cu-SSZ-13 was formed, in a close combination with a carrier, via one step hydrothermal process. Cu-SSZ-13/cordierite showed excellent DeNO x performance for selective catalytic reduction (SCR) and anti-aging properties in a simulated diesel exhaust gas under a high space velocity. At a high space velocity of 72,000 h −1 , the highest conversion and N 2 selectivity of 94% and 90%, respectively, were achieved. After the aging for 50 h at 720 °C, NO x reduction rate was still >80% in the temperature range of 350–550 °C. The larger height to diameter ratio of the same catalysts enhanced the NH 3 -SCR catalytic activity and broadened the active temperature window. The addition of HF increased the catalytic activity and anti-aging performance of the sample.
研究领域:
催化材料
·
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Jiangxiao Qiao,Jinxin Gan,Fei Gao,Xiangsen Xu,Jiesong Tan,Yiqing Zeng,Feng Zhang,Feng Han,Zhaoxiang Zhong,Weihong Xing
Synergistic removal of nitrogen oxides (NOx) and particulate matter (PM) can be achieved using multifunctional catalytic membranes. In this work, CePO4 nanorods were loaded on the pore surfaces of SiC membranes to construct the CePO4/SiC-X catalytic membranes. The stacked nanorod structure of the CePO4 catalyst layer facilitates the diffusion of gases to the catalyst surface during reactions. Owing to the high specific surface area, rich surface acidity, and strong redox capacity, the CePO4/SiC-400 catalytic membrane exhibits the best ammonia-selective catalytic reduction (NH3–SCR) denitration activity, achieving >90% NO conversion at a temperature of 250–380 °C and negligible N2O byproduct. In addition, the CePO4/SiC-400 catalytic membrane demonstrates excellent H2O and SO2 resistance. The performance of dust filtration and simultaneous dust filtration and denitration at 250–350 °C proposed that the dust rejection efficiency reached more than 99% at various conditions, and the dust filtration process did not affect the NH3–SCR performance of the CePO4/SiC-400 catalytic membrane. From the above results, the CePO4/SiC-400 catalytic membrane presents a broad application prospect in the simultaneous dust removal and denitration of high-temperature flue gas.
研究领域:
环境科学
·
催化材料
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2020
·Vol. 27
·期 22
·27663-27673
·
IF 3.056
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
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Jiahao Chen,Bin Wang,Kai Yuan,Yutang Kang,Shasha Feng,Feng Han,Hongmiao Wu,Rongfei Zhou,Zhaoxiang Zhong,Yiqun Fan,Weihong Xing
The SiC catalytic membrane combining dust removal and denitration can realize the efficacious treatment of atmospheric pollutants. Unfortunately, a large amount of SiO 2 , formed by the partial oxidation of SiC at a high temperature, results in the decreased chemical resistance of SiC catalytic membrane. In addition, the complicated preparation processes and susceptible to loss of catalytic components under harsh conditions restrict the industrial application of SiC catalytic membranes. Here, the Cu-SAPO-34(D)/SiC catalytic membranes were directly prepared via a facile one-pot hydrothermal synthesis method, which ingeniously utilized the generated SiO 2 as a Si source to participate in the growth of Cu-SAPO-34 zeolites. Excellent binding strength and chemical resistance were simultaneously realized for the SiC catalytic membranes. As a comparison, a Cu-SAPO-34(I)/SiC catalytic membrane was fabricated via the conventional two-step ion-exchange method. The 0.2 Cu-SAPO-34(D)/SiC (Cu molar ratio of 0.2) achieved the best NH 3 -SCR performance among the prepared catalytic membranes for its highly active copper and oxygen species, abundant Lewis acid sites and remarkable redox capacity. When implementing the simultaneous removal of NO and PM, the 0.2 Cu-SAPO-34(D)/SiC catalytic membrane achieved a high NO degradation performance of 98% from 200 to 280 °C, coupled with an excellent PM 0.3 (model dust with average size of 300 nm) filtration performance of 99.99%. These results were better than those of the Cu-SAPO-34(I)/SiC catalytic membrane (92% for NO degradation and 99.98% for PM 0.3 filtration). The one-pot in situ synthesis of Cu-SAPO-34(D)/SiC catalytic membrane with enhanced binding strength and chemical resistance provides a novel strategy for preparation of high-performance SiC catalytic membrane with double benefits.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
Catalysis Science & Technology
·
2016
·Vol. 6
·期 24
·8516-8524
·
IF 5.287
Lei Huang,Kaiwen Zha,Supawadee Namuangruk,Anchalee Junkaew,Xin Zhao,Hongrui Li,Liyi Shi,Dengsong Zhang
Surface engineering of TiO2 is significant in the SCR reaction and worth studying. In a previous study, we found that TiO2 nanosheets (TiO2-NS) with the (001) plane exhibited a much better SCR performance than TiO2 nanoparticles (TiO2-NP) with the (101) plane. In this work, in situ DRIFTS and DFT calculations were applied to address the promotional effect of the (001) plane of TiO2-NS in the SCR reaction. The behavior of adsorption and desorption of NOx and NH3 on the two surfaces was studied. It was found that NH3 adsorbed on both TiO2-NS and TiO2-NP was in the form of NH3(g) on the Lewis acid sites. NOx on TiO2-NP were mainly trans-(NO)2 and N2O4 which were non-reactive. Differently, NO on TiO2-NS was mainly in the form of NO2 which was probably due to the high energy and abundant active oxygen species of the (001) facet. The formed NO2 could trigger the subsequent ‘fast SCR’ reaction thereafter promoting the activity. Therefore, TiO2-NS with more (001) facets had better SCR activity than TiO2-NP with the exposed (101) facet.
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
CHINESE JOURNAL OF CATALYSIS
·
2015
·
IF 1.964
Xin Zhao,Lei Huang,Hongrui Li,Hang Hu,Jin Han,Liyi Shi,Dengsong Zhang
Different transition metals were used to modify V 2 O 5 -based catalysts (M-V, M = Cu, Fe, Mn, Co) on TiO 2 via impregnation, for the selective reduction of NO with NH 3 . The introduced metals induced high dispersion in the vanadium species and the formation of vanadates on the TiO 2 support, and increased the amount of surface acid sites and the strength of these acids. The strong acid sites might be responsible for the high N 2 selectivity at higher temperatures. Among these catalysts, Cu-V/TiO 2 showed the highest activity and N 2 selectivity at 225–375 °C. The results of X-ray photoelectron spectroscopy, NH 3 -temperature-programmed desorption, and in-situ diffuse reflectance infrared Fourier transform spectroscopy suggested that the improved performance was probably due to more active surface oxygen species and increased strong surface acid sites. The outstanding activity, stability, and SO 2 /H 2 O durability of Cu-V/TiO 2 make it a candidate to be a NO x removal catalyst for stationary flue gas.
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
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Jingang Wang,Jianbo Zhang,Cheng Xing,Taosheng Jin,Jinpeng Liu,Meiting Ju,Xuejiao Tang
Phosphorus (P) poisoning of NH 3 -SCR catalysts is inevitable in application of NO x abatement of diesel exhaust. The distinct effects on Cu-SSZ-13 of P from different precursors (H 3 PO 4 and (NH 4 ) 2 HPO 4 ) were figured out and the mechanism was further investigated. P-poisoned Cu-SSZ-13 (Si/Al = 6) catalysts were prepared and characterized using N 2 adsorption, X-ray powder diffraction (XRD), scanning electron microscope with energy-dispersive X-ray spectroscopy mapping (SEM-EDX), ammonia temperature-programmed desorption (NH 3 -TPD), X-ray photoelectron spectroscopy (XPS), hydrogen temperature programmed reduction (H 2 -TPR), electron paramagnetic resonance (EPR) and 27 Al solid-state magic angle spinning nuclear magnetic resonance spectroscopies ( 27 Al NMR). Significant enhancement of high-temperature activities (400–600 °C) were observed for the catalysts with P loading of 0.3–0.9 wt%, since the appropriate incorporation enabled to bind P atoms to CuO x in remained framework. However, the high P content of 1.5 wt% resulted in a detrimental effect on framework to induce the accumulation of Cu species. Interestingly, the dominant P from H 3 PO 4 was inclined to directly attack the framework Al leading to more severe dealumination, while the P from (NH 4 ) 2 HPO 4 interacted with Cu 2+ to form copper phosphate with more Cu 2+ migrating to the surface of the catalyst which promoted the NO x conversation at each active site resulting in the low-temperature catalytic activity unchanged. So, control of the P/Cu and form of P is capable of preventing P poisoning and unlocks the potential of Cu-SSZ-13 in exhaust treatment.
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
·
2026
·
IF 9
Bo Song,Zhenxing Shen,Zitong Wang,Qin Peng,Jia Liu
Traditional Mn-based NH 3 -SCR catalysts have a narrow temperature window, limiting low-temperature use. In this work, Mn@N-7 was prepared by a simple hydrothermal method using potassium permanganate and urea. The hydrothermal conditions are much milder than those used for most Mn-based catalysts. Graphite felt (GF) serves as a green support, providing a 3D carbon fiber network for uniform growth of manganese oxide nanowebs. Its high surface area (83.10 m 2 g −1 ) and open channels promote active species dispersion and fast mass transfer. The strong carbon framework prevents sintering at high temperatures. Mn@N-7 shows nearly 100% NO conversion at 100–200 °C and maintains good activity for 30 h. Its estimated cost is 1.2–1.8 USD kg −1 , lower than 3.0–4.5 USD kg −1 for V 2 O 5 -WO 3 /TiO 2 catalysts. The mild hydrothermal process avoids high-temperature calcination. This work demonstrates GF is a sustainable support and offers guidance for carbon-based catalysts in clean air applications.
✓ 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）