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
JOURNAL OF SOLID STATE CHEMISTRY
·
2022
·
IF 3.656
Lei Ma,Feifei Zhang,Kunjie Li,Yingying Zhang,Zhiqiang Song,Li Wang,Jiangfeng Yang,Jinping Li
The capture of N 2 O from CO 2 by an adsorption-based mechanism remains a significant challenge due to their similar molecular sizes and physical properties. Although substituent engineering has been widely employed for the selectivity regulation and improvement of gas mixtures in metal-organic frameworks, its effect on N 2 O/CO 2 separation has yet not been explored. Herein, four isoreticular MTN-type metal-organic frameworks (MOFs) with different substituents (-H, –NH 2 , -Br or –NO 2 ) are reported for the capture of N 2 O from a N 2 O/CO 2 mixture. As revealed by isothermal measurements, thermodynamic studies and ideal adsorbed solution theory computations, the N 2 O/CO 2 separation potential can be effectively improved by an electron-donating group (-NH 2 ), whereas electron-withdrawing groups (-NO 2 or -Br) exhibit the opposite effect. Notably, MIL-101(Cr)–NH 2 exhibits, by far, the highest ideal adsorbed solution theory equilibrium adsorption selectivity of 1.91 for 50/50 N 2 O/CO 2 . The N 2 O/N 2 separation ability of the modified materials is also studied and functionalization with a -Br group yields an improved separation potential compared to the parent MIL-101(Cr) material. The strategy of using substituents to enhance the N 2 O/CO 2 separation efficiency of MOFs could also be extended to other porous materials for chemical separation processes.
研究领域:
材料科学
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化学工程
✓ 已验证
DOI
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
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
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
International Journal of Environmental Research and Public Health
·
2023
·Vol. 20
·期 6
·4902
·
IF 4.614
Ruiqi Wu,Ning Liu,Chengna Dai,Ruinian Xu,Ning Wang,Gangqiang Yu,Biaohua Chen
N2O is a greenhouse gas and a candidate oxidant. Volatile organic pollutants (VOCs) have caused great harm to the atmospheric ecological environment. Developing the technique utilizing N2O as the oxidant to oxidize VOCs to realize the collaborative purification has significant importance and practical value for N2O emission control and VOC abatement. Therefore, the study of N2O catalytic oxidation of tert-butanol based on zeolite catalysts was carried out. A series of molecular sieves, including FER, MOR, ZSM-5, Y, and BEA, were selected as the catalyst objects, and the 1.5% wt Fe and Co were, respectively, loaded on the zeolite catalysts via the impregnation method. It was found that the catalytic performance of BEA was the best among the molecular sieves. Comparing the catalytic performance of Fe-BEA under different load gradients (0.25~2%), it was found that 1.5% Fe-BEA possessed the best catalytic activity. A series of characterization methods showed that Fe3+content in 1.5% Fe-BEA was the highest, and more active sites formed to promote the catalytic reaction. The α-O in the reaction eventually oxidized tert-butanol to CO2over the active site. The Co mainly existed in the form of Co2+cations over Co-BEA samples; the 2% Co-BEA possessing higher amounts of Co2+exhibited the highest activity among the prepared Co-BEA samples.
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
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Li Wang,Zhangmiao Ye,Caihong Lin,Yugao Wang,Jinping Li,Jiangfeng Yang
N2O/CO2 separation in the tail gas of adipic acid presents a significant challenge due to the closely resembling physical characteristics exhibited by CO2 and N2O. Herein, adsorption and separation performances of CO2 and N2O on FAU-type zeolite Y with different cations (Na+ and Ag+) were studied comprehensively. After Ag+ exchange, zeolite Y changes from a CO2-selective adsorbent to a N2O-selective adsorbent. AgY shows high N2O uptake (95.7 cm3/g) but relatively low adsorption heat (23.1 kJ/mol), making it suitable for N2O/CO2 separation. In situ Fourier transform infrared spectrometry indicates that N2O is successfully adsorbed on AgY. The breakthrough experiment reveals that AgY exhibits superior performance in the separation of N2O/CO2 at a flow rate of 20 mL/min while also exhibiting a favorable retention time and ratio of retention time with CO2 breakthrough time, which can reach up to 4.1 min and 0.24, respectively, which makes it an optimum N2O/CO2 separation material reported so far.
研究领域:
化学工程
·
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
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
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2018
·
IF 3.141
Yongheng Xiong,Qin Zhong,Man Ou,Wei Cai,Shipeng Wan,Yang Yu,Shule Zhang
The discovery of effective methods toward nitric oxide (NO) removal by solution is valuable for the cost-effective flue gas control. In this study, it is first reported that nitrous oxide (N2O) is obviously suppressed by using copper oxide (CuO) combined with (NH4)2SO3 (NS) solution. CuO has been characterized, and the effects of reactants concentration, additives, temperature, pH and powder size on NO absorption process have been evaluated. The selectivity of N2O can drop from 91.30% to 11.25% under the optimum experimental conditions. Furthermore, based on the method of single-factor analysis, the inhibition of N2O is identified as the coeffect of NS/CuO. In addition, the pathways of NO removal are divided into two parts—N2O formation and NO absorption—and its ratio is calculated in the range of 0.29–0.53. Because of the continuous supply of NS from ammonia desulfurization, this study opens the feasibility of simultaneous desulfurization and denitrification.
研究领域:
环境科学
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化学工程
·
大气污染控制
✓ 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
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环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Agronomy-Basel
·
2024
·Vol. 14
·期 6
·1113
·
IF 3.3
Jing Wang,Linfang Guo,Fengmin Yang,Jian Xiang,Lizhi Long,Kang Ni
The excessive application of nitrogen in tea plantations leads to severe soil acidification and N2O emission boosting. To promote sustainable agriculture, nanoparticles (NPs) have emerged as alternative fertilizers, but their effects on soil nitrification and greenhouse gas emissions in tea plantations remain unclear. In this study, the effects of NP type (ZnO-NPs and Fe2O3-NPs) and dose (0, 1, 10, and 100 mg·kg−1) on soil N2O emissions were investigated via a lab incubation trial. Soil pH, ammonium, and nitrate changes were also monitored during the incubation period. The abundance of functional genes related to nitrification and denitrification processes was analyzed as well. The results showed that ZnO-NPs led to a decrease in N2O emissions. The reduction effect was stronger with increasing dose and resulted in a 33% reduction at an addition rate of 100 mg·kg−1. The cumulative N2O emissions had significantly positive correlations with NH4+-N and NO3−-N. ZnO-NP addition showed a significantly negative effect on Ammonia-Oxidizing Archaea (AOA) but a positive effect on Ammonia-Oxidizing Bacteria (AOB) gene abundance. In contrast, Fe2O3-NPs showed an insignificant impact on N2O emissions and soil N content, as well as nitrification–denitrification gene abundance, regardless of different doses. These results imply that the application of ZnO-NPs may inhibit nitrification through the retarding of AOA activity. This study provided us with a potential practice to reduce N2O emissions in tea plantations by applying ZnO-NPs, but the efficiency of this reduction needs further examination under ambient conditions before field application.
研究领域:
农业生态学
·
微生物学
·
环境科学
✓ 已验证
产品关联
DOI
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
危险品化学品经营许可证（带存储）