Journal of the Taiwan Institute of Chemical Engineers
·
2016
·
IF 2.848
Huan Liu,Zhen Ma
LaPO 4 has been used as a support to make supported catalysts in some investigations, but the effect of different LaPO 4 supports on the catalytic performance of supported catalysts has been rarely reported. In this work, conventional hexagonal LaPO 4 (LaPO 4 H) was prepared by precipitation, and hexagonal LaPO 4 nanowires (LaPO 4 HNW) was prepared by hydrothermal synthesis at 150 °C. Monoclinic LaPO 4 nanowires (LaPO 4 -MNW-220 and LaPO 4 -MNW-900) were prepared by hydrothermal synthesis at 220 °C or calcining LaPO 4 HNW at 900 °C. These samples were used to support Rh 2 O 3 via impregnation using Rh(NO 3 ) 3 as a precursor. The activities of these supported catalysts in N 2 O decomposition and CO oxidation follow the same sequence of Rh 2 O 3 / LaPO 4 HNW > Rh 2 O 3 / LaPO 4 H > Rh 2 O 3 / LaPO 4 -MNW-220 > Rh 2 O 3 / LaPO 4 -MNW-900, i.e. , two hexagonal LaPO 4 supports are better than two monoclinic LaPO 4 supports in making active catalysts, and hexagonal LaPO 4 nanowires are better than hexagonal LaPO 4 composed of nanoparticles and short nanorods. The most active catalyst has highly dispersed Rh 2 O 3 species interacting strongly with the support, more oxygen-adsorption capacity, and more basic sites.
研究领域:
催化化学
·
材料科学
✓ 已验证
DOI
高影响因子
Frontiers of Chemical Science and Engineering
·
2017
·Vol. 11
·期 4
·586-593
·
IF 1.712
Liu Huan,Ma Zhen
Hexagonal CePO 4 nanorods were prepared by a precipitation method and hexagonal CePO 4 nanowires were prepared by hydrothermal synthesis at 150 °C. Rh (NO 3 ) 3 was then used as a precursor for the impregnation of Rh 2 O 3 onto these CePO 4 materials. The Rh 2 O 3 supported on the CePO 4 nanowires was much more active for the catalytic decomposition of N 2 O than the Rh 2 O 3 supported on CePO 4 nanorods. The stability of both catalysts as a function of time on stream was studied and the influence of the co-feed (CO 2 , O 2 , H 2 O or O 2 /H 2 O) on the N 2 O decomposition was also investigated. The samples were characterized by N 2 adsorption-desorption, inductively coupled plasma optical emission spectroscopy, X-ray diffraction, transmission electron microscopy, X-ray photoelectron microscopy, hydrogen temperature-programmed reduction, oxygen temperature-programmed desorption, and CO 2 temperature-programmed desorption in order to correlate the physicochemical and catalytic properties.
研究领域:
催化化学
·
材料科学
✓ 已验证
DOI
高影响因子
ChemCatChem
·
2024
·
IF 3.8
Yuxin Sun,Yunshuo Wu,Zhuoyi Zhang,Xuanhao Wu,Haiqiang Wang,Zhongbiao Wu
Graphical Ce-Pr co-doped Co 3 O 4 achieved 100% N 2 O conversion at 400 °C over Pr 0.02 Ce 0.2 Co 1 . The introduction of Ce facilitated the formation of oxygen vacancies, which were essential for N 2 O activation. But these Ce species strictly inhibited Co 3 O 4 crystallization and surface exposure, which were unfavorable to N 2 O decomposition. By the codoping of Pr, these negative effects were eliminated, leading to remarkable catalytic performance. Nitrous oxide (N 2 O) has gained increasing attention as a non-carbon dioxide greenhouse gas, and catalytic decomposition is an effective method for mitigating its emissions. In this study, Ce-Pr Co-doped Co 3 O 4 was synthesized via a coprecipitation method and used for the catalytic decomposition of N 2 O. The experimental results revealed that the N 2 O decomposition achieved 100% conversion at 400 °C on the catalyst with a Pr/Ce/Co molar ratio of 0.02:0.2:1, exhibiting an 80 °C decrease of T 100 compared with that of Co 3 O 4 . The introduction of Ce reduced the size and crystallization of Co 3 O 4 particles, increased the activity of the lattice oxygen of Co 3 O 4 , and facilitated the formation of oxygen vacancies, thereby enhancing the activation of N 2 O. However, the introduction of Ce inhibited the crystallization of Co 3 O 4 and the surface coverage of CeO 2 decreased the exposure degree of N 2 O molecules to the Co 3 O 4 surface. Co-doping strategy of Ce-Pr was performed to alleviate the negative effects of ceria. Consequently, the incorporation of Ce and Pr species enhanced the redox properties of Co 3 O 4 , leading to remarkable catalytic performance of N 2 O decomposition. This study elucidated the interaction between Ce and Pr dopants and Co 3 O 4 , and encouraged more attention on designing novel catalysts for N 2 O mitigation.
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
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2021
·
IF 9.028
Ying Xiong,Yumei Zhao,Xingkun Qi,Jiayi Qi,Yuanyuan Cui,Haibiao Yu,Ying Cao
In this paper, Gd-promoted Co3O4 catalysts were prepared via a facile coprecipitation method for low-temperature catalytic N2O decomposition. Due to the addition of Gd, the crystallite size of Co3O4 in the Gd0.06Co catalyst surprisingly decreased to 4.9 nm, which is much smaller than most additive-modified Co3O4 catalysts. This huge change in the catalyst’s textural structure endows the Gd0.06Co catalyst with a large specific surface area, plentiful active sites, and a weak Co–O bond. Hence, Gd0.06Co exhibited superior activity for catalyzing 2000 ppmv N2O decomposition, and the temperature for the complete catalytic elimination of N2O was as low as 350 °C. Meanwhile, compared with pure Co3O4, Ea decreased from 77.4 to 46.8 kJ·mol–1 and TOF of the reaction increased from 1.16 × 10–3 s–1 to 5.13 × 10–3 s–1 at 300 °C. Moreover, Gd0.06Co displayed a quite stable catalytic performance in the presence of 100 ppmv NO, 5 vol % O2, and 2 vol % H2O.
研究领域:
催化化学
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2022
·
IF 5.723
Feilin Zhao,Chizhong Wang,Dongdong Wang,Yimeng Yin,Jie Yu,Jinchi Han,Jie Zeng,Huazhen Chang
A series of Cd-doped NiO catalysts were prepared and tested in the N 2 O catalytic decomposition reaction. In comparison with NiO, it was found that the Cd 0.04 Ni catalyst showed higher N 2 O decomposition activity in the temperature range of 300–450 °C with or without O 2 , and lower activation energy (77.8 kJ mol −1 ). The incorporation of Cd into the NiO lattice was verified by X-ray diffraction (XRD) patterns and Raman spectra. This led to the distortion of the original NiO structure and weakened the Ni-O bond. X-ray photoelectron spectroscopy (XPS) results showed that compared with NiO and CdO, Cd 0.04 Ni possessed higher Ni 2+ and Cd (n+1)+ contents, which might have been induced by the electron transfer behavior between CdO and NiO. A possible mechanism for active site regeneration and O 2 desorption over Cd 0.04 Ni was proposed. The Cd 0.04 Ni catalyst also exhibited good resistance to NO and O 2 .
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
ACS ES&T Engineering
·
2024
·
IF 7.4
Zhuoyi Zhang,Yunshuo Wu,Yuxin Sun,Haiqiang Wang,Zhongbiao Wu,Xuanhao Wu
Nitrous oxide (N2O) is a potent greenhouse gas with a high global warming potential. The N2O direct decomposition (deN2O) is currently the most widely used technique due to its operational simplicity and lack of secondary pollution. The presence of impurity gases in industrial exhaust increases the challenge of eliminating N2O, urging the development of highly active and stable catalysts for its degradation. In this study, a series of praseodymium (Pr)-doped nickel oxide (NiO) catalysts were synthesized for N2O degradation. These catalysts showed higher N2O decomposition activity (T100 = 400–440 °C) than pure NiO (T100 = 480 °C) and also demonstrated high resistance to impurity gases in simulated industrial nitric acid tail gas. In the catalyst with a Pr to Ni ratio of 0.002, the highly dispersed Pr on the NiO surface regulated its particle size and increased specific surface area and pore volume. DFT calculations revealed that Pr significantly enhanced the electron-donating ability of Ni2+, facilitating the dissociative adsorption of N2O on the catalyst surface, where O existed in the form of Ni3+-O*. Additionally, Pr reduced the desorption energy of O2, the rate-determining step. During the reaction, Pr3+ transferred electrons to Ni3+ via f-d electron hopping, stabilizing the active Ni2+ sites and enabling an efficient catalytic reaction. These findings demonstrate the practical potential of this catalyst and provide new insights into the degradation of N2O in industrial exhaust gases, offering a promising avenue for application.
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 CATALYSIS
·
2017
·
IF 6.844
Chuande Huang,Yanyan Zhu,Xiaodong Wang,Xin Liu,Junhu Wang,Tao Zhang
A series of BaFe 1− x Sn x O 3− δ catalysts were prepared by sol-gel method and tested for N 2 O decomposition to shed light on the effect of B-site substitution on the catalytic behavior of perovskite catalysts. 119 Sn and 57 Fe Mössbauer results confirmed that the 5-fold coordinated Fe 3+ cations with one adjacent oxygen vacancy (Fe 3+ O 5 ) were the main active centers for N 2 O decomposition. Doping of Sn cations can significantly improve the percentage of Fe 3+ O 5 from 30% ( x = 0) to 68% ( x = 0.8). More importantly, the valence state of Fe could be gradually reduced due to weakening of Fe O bond with increasing the Sn content, which was attributed to the stronger force of Sn than Fe in Fe O Sn structure to draw the oxygen anion and expansion of unit cell volume. Such change of Fe chemical state favored the oxygen mobility of the catalyst, leading to reduction in activation energy for N 2 O decomposition from ca. 241 ( x = 0) to 178 kJ mol −1 ( x = 0.8). BaFe 0.2 Sn 0.8 O 3− δ catalyst exhibited the highest intrinsic rate of 1.49 s −1 (550 °C), nearly 4 times larger than that of BaFeO 3− δ (0.43 s −1 ).
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Shuang Cao,Zhuoyi Zhang,Yunshuo Wu,Yuxin Sun,Zhe Li,Yanxia Gao,Haiqiang Wang,Xuanhao Wu,Zhongbiao Wu
Nitrous oxide (N 2 O) is a potent greenhouse gas with high global warming potential. It is urgent to develop active and stabile catalysts for N 2 O direct catalytic decomposition (deN 2 O) in industrial exhaust gas. In this study, a series of Eu-doped NiO catalysts were synthesized by co-precipitation method. The catalyst with an Eu to Ni molar ratio of 0.04 showed the highest deN 2 O ability, reaching 100 % conversion at 400 °C without generating NO x by-products. The catalyst also displayed resilience against O 2 and NO impurity gases, maintaining structural stability and achieving complete transformation of N 2 O at 440 °C. Eu was uniformly dispersed in NiO in the form of Eu 2 O 3 , which not only regulated the particle size and specific surface area of NiO, but also changed the surface chemistry of NiO by inducing more Ni 2+ active sites and more mobile O β species. Eu-doping altered the decomposition mechanism of N 2 O from L-H to E-R mechanism, reducing the energy barrier of O 2 desorption, which was the rate-determining step. During the reaction, Eu 0.04 Ni showed an activation behavior after cyclic use and long-term reaction and reduced T 100 to 320 °C after 14-hr experiment. These findings demonstrate the potential of the catalyst for practical application and provide new routes for the direct decomposition of N 2 O in industrial exhaust gas.
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
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2024
·
IF 10.8
Yunshuo Wu,Xuanhao Wu,Jie Fan,Haiqiang Wang,Zhongbiao Wu
Iron zeolites are promising candidates for mitigating nitrous oxide (N2O), a potent greenhouse gas and contributor to stratospheric ozone destruction. However, the atomic-level mechanisms by which different iron species, including isolated sites, clusters, and particles, participate in N2O decomposition in the presence of CO still remain poorly understood, which hinders the application of the reaction in practical technology. Herein, through experiments and density functional theory (DFT) calculations, we identified that isolated iron sites were active for N2O activation to generate adsorbed O* species, which readily reacted with CO following the Eley–Rideal (E-R) mechanism. In contrast, Fe2O3 particles exhibited a different reaction pathway, directly reacting with CO to generate oxygen vacancies (Ov), which could efficiently dissociate N2O following the Mars-van Krevelen (MvK) mechanism. Moreover, the transformation of iron oxide clusters into undercoordinated FeOx species by CO was also revealed through various techniques, such as CO-temperature-programmed reduction (TPR), and ab initio molecular dynamics (AIMD) simulations. Our study provides deeper insights into the roles of different iron species in N2O-SCR by CO, and is anticipated to facilitate the understanding of multicomponent catalysis and the design of efficient iron-containing catalysts for practical applications.
研究领域:
催化化学
·
环境科学
·
材料科学
✓ 已验证
DOI
PubMed
高影响因子
ENERGY & FUELS
·
2021
·
IF 3.605
Hairong Tang,Yong He,Peixi Liu,Jiaming Shao,Fawei Lin,Zhihua Wang
Zeolitic-imidazolate framework precursors (ZIF-67) were synthesized in an inorganic solution with triethylamine as a deprotonating agent for N2O decomposition, and the catalytic activities of the pyrolysis products under different conditions were investigated. Among them, the Co/CoOx@carbon catalyst pyrolyzed at 650 °C in a N2 atmosphere (Co-650N) exhibited excellent low-temperature catalytic activity and stability, achieving 50% decomposition efficiency at 305 °C and ∼100% at 400 °C, which benefitted from its large specific surface area, great reduction performance, abundant cobalt active sites, and surface oxygen species. Further, utilizing temperature-programmed desorption (TPD) and in situ diffused reflectance infrared Fourier transform spectroscopy (DRIFTS) results, it was found that N2O molecules preferentially combined with oxygen species bound to cobalt sites. The absorbed N2O was decomposed into N2 and oxygen species, and the latter was subsequently transferred to carbon frameworks. Interestingly, the amorphous graphitic carbon frameworks played an important role in transferring/storing active oxygen and regenerating cobalt sites. Moreover, Co-650N exhibited better resistance to SO2, and the efficiency could be recovered via heating and finally stabilized at 100%. Finally, the mechanisms of N2O decomposition and sulfur poisoning-reactivation on Co/CoOx@carbon catalysts were proposed for the first time.
研究领域:
催化化学
·
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
CHEMOSPHERE
·
2022
·
IF 8.943
Ying Xiong,Yumei Zhao,Weijun Shan,Xiaogeng Feng,Junshuo Cui,Zhenning Lou,Guoxiang Shao,Min Dong,Haibiao Yu
In order to enhance the catalytic performance of the Gd-modified Co 3 O 4 catalyst (Gd 0.06 Co) for the N 2 O decomposition, alkali metal K was introduced as the promoter by impregnating the Gd 0.06 Co powder with an aqueous solution of KNO 3 (with K/Co ratios 0.01–0.05). With the doping of K, the catalytic activity over Gd 0.06 Co was significantly improved and the temperature of N 2 O complete decomposition was decreased from 350 °C to 300 °C. Combining the results of XPS and O 2 -TPD, the superior catalytic performance of the optimum catalyst K 0.025 Gd 0.06 Co was mainly owing to the synergistic effect of Gd and K, which weakened the Co–O bond and endowed the catalyst surface with much more amount of oxygen vacancies. Even under the coexist of the impurity gases, such as 5 vol% O 2 , 100 ppmv NO and 2 vol% H 2 O, the K 0.025 Gd 0.06 Co catalyst exhibited prominently better catalytic activity than Gd 0.06 Co and K 0.025 Co catalysts.
研究领域:
催化化学
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Jiayi Qi,Xingkun Qi,Yan Pan,Junshuo Cui,Ying Xiong,Weijun Shan,Haibiao Yu
Sm 0.06 Ni with excellent H 2 O resistance for eliminating N 2 O was prepared by co-precipitation method. Research indicated that the introduction of Sm into Sm 0.06 Ni has the following effects: (1) Sm species (Sm 2 O 3 ) highly dispersed on the surface of Sm 0.06 Ni catalyst, which not only decreased the crystallite size of NiO, but also produced a certain number of edge dislocations and defects. (2) Sm 2 O 3 weakened the Ni-O band and increased the number of active sites. (3) The redox cycle of Ni 2+ + Sm 3+ ↔ Ni 3+ + Sm 2+ was formed on the surface of Sm 0.06 Ni during the reaction. Based on the above changes, Sm 0.06 Ni exhibited superior catalytic performance and much lower E a for the reaction compared with pure NiO. Over Sm 0.06 Ni, the TOF at 350 ℃ was 4.1 × 10 −3 s −1 , 37 times of that over pure NiO. More importantly, Sm 0.06 Ni exhibited excellent H 2 O resistance performance under submitted real reaction conditions, about 76 % N 2 O conversion can be obtained at 400 ℃.
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
危险品化学品经营许可证（带存储）