Reaction behaviors of CH3CN catalytic combustion over CuCeO -HZSM-5 composite catalysts: The mechanism of enhanced N2 selectivity

Wang, Yuxing; Ying, Qingji; Zhang, Yaoyu; Liu, Yue; Wu, Zhongbiao

doi:10.1016/j.apcata.2019.117373

Cited by 36 publications

(18 citation statements)

References 57 publications

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“…Such results affirmed that the Cu-BETA catalyst maintained excellent catalytic activity and N 2 selectivity. Results from the present study could surpass other works reported in the literature [7,8,39], where the N 2 selectivity decreases as the reaction proceeds [40]. Cu-BETA also showed exceptionally high turnover frequencies (TOF = 5.3-11.7 × 10 -4 s -1 ) at a temperature range of 300-600 °C compared to CuO (TOF = 0.5-2.3 × 10 -4 s -1 ) and La 2 CuO 4 (TOF = 0-7.8 × 10 -4 s -1 ) catalysts.…”

Section: Resultscontrasting

confidence: 60%

“…Treatment of acetonitrile by traditional thermal combustion technique is controlled by chain-terminating reaction sequences at elevated temperatures (above 1000 °C) and often leads to the formation of undesirably large amounts of nitrogen oxides and HCN [4]. According to earlier studies [3,[5][6][7], the selective catalytic combustion (SCC) of acetonitrile toward N 2 and CO 2 is the most efficient and environmentally benign route, owing to its high purification efficiency, low operation cost at lower temperatures, and fewer secondary pollutants.…”

Section: Introductionmentioning

confidence: 99%

“…The literature reports some studies discussing the performance of catalysts prepared via impregnation for the acrylonitrile-SCC [3,13,14] and rare works related to acetonitrile-SCC [7,8]. In terms of the zeolite topology, BETA was the most effective material among various commercial zeolites (MFI, FER, MOR, FAU) with similar Si/Al ratios for the decomposition of N 2 O [15] and exhibited superior activity in comparison with ZSM-5 [16].…”

Section: Introductionmentioning

confidence: 99%

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Acetonitrile Combustion over Copper-Based Nanocatalysts: A Structure-Performance Relationship Study

Ponciano¹,

Batista²

2021

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In this paper, the relationship between activity and structure of Cu2+ in different chemical environments of Cu-BETA, La2CuO4, and CuO nanocatalysts was systematically investigated for acetonitrile combustion. The study revealed that exchanged and octahedral species of Cu2+ coexist in Cu-BETA, while octahedral species are dominant in CuO and La2CuO4. All nanocatalysts achieved high conversion rates of acetonitrile, which rapidly increased with temperature. CuO and La2CuO4 led to the formation of undesired products such as N2O and NO. On the other hand, Cu-BETA showed high acetonitrile conversion along with a high N2 yield. The excellent performance of Cu-BETA can be attributed to the easy reducibility of the highly dispersed Cu-species and the small crystallite size. Cu-BETA also exhibited exceptional stability. Therefore, the high conversion rate and the high N2 yield make Cu-BETA a promising catalyst for acetonitrile combustion.

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Section: Resultscontrasting

confidence: 60%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Acetonitrile Combustion over Copper-Based Nanocatalysts: A Structure-Performance Relationship Study

Ponciano¹,

Batista²

2021

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“…The observed peaks are characteristic of Cu 1+ and Cu 2+ , excluding the formation of Cu 0 (919 eV) in the surface of the as-prepared catalysts. − In this work, a peak at around 937.5 eV is observed, displaying a remarkably higher binding energy than that in literature. Such a shift explains the strong interaction between CuO and the Ce–Al support (to form Cu 2+ -O 2– -Ce 4+ species) due to the charge transfer from the metal ion toward the support matrix. , This peak has been reported and ascribed to Cu 2+ bonded with oxygen species from the support (Cu–O–Ce) previously in literature. − Indeed, the formed electronic Cu–Ce interaction can introduce more oxygen vacancies, which has been claimed to have positive effect on CO 2 adsorption and activation, opening an effective reaction pathway for the CO 2 hydrogenation. , Therefore, proportions of Cu 2p 3/2 species are quantitively given in Table . It implies that the bimetallic Fe–Cu samples, especially the 0.25Fe0.75Cu, have a relatively high amount of Cu-doped ceria (represented by Cu 2+ -O 2– -Ce 4+ in Table ) than Bare Cu, showing more potential to interact and activate CO 2 .…”

Section: Resultsmentioning

confidence: 76%

Highly Active and Selective Multicomponent Fe–Cu/CeO₂–Al₂O₃ Catalysts for CO₂ Upgrading via RWGS: Impact of Fe/Cu Ratio

Yang

Pastor‐Pérez

Villora-Picó

et al. 2021

ACS Sustainable Chem. Eng.

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The reverse water–gas shift reaction (RWGS) reaction represents a direct route for CO2 conversion whose selectivity significantly depends on the selected catalyst. In this work, a new family of bimetallic iron–copper oxide catalysts supported on ceria-alumina with various Fe/Cu oxides ratios were investigated for the RWGS reaction. Additionally, bare Fe-based and Bare Cu-based catalysts were synthesized for comparison. Our results demonstrate that the developed bimetallic Fe–Cu catalysts present a remarkable enhancement of catalytic performance when compared to monometallic systems, especially at the so-called “low-temperature range” for RWGS. Characterization results evidence that Cu species undergo different states on the catalytic surface during the reaction, wherein the formed metallic Cu is linked to the catalytic activity via the strength of the interaction with the multioxide phases, such as Fe3O4/CeO2, while the copper-dopped ceria could contribute to the promotion of CO selectivity. Besides, we identify that the Fe/Cu oxides mass ratio of 0.25/0.75 is an optimal formulation rendering highly commendable CO2 conversion levels at 450 °C with excellent selectivity and stability for long-term runs. Very importantly, without preactivation, our multicomponent materials still display an optimum performance which have a potential realistic application from cost perspective than other Cu-based catalysts. Overall, this work showcases a strategy to design highly effective multicomponent Fe–Cu catalysts for CO2 conversion via RWGS.

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“…Metal–organic frameworks (MOFs) exhibit a high adsorption capacity of H 2 S due to their chemical composition, ligand functionality, cavity dimensions, and a rigid framework structure. − However, the irreversible chemisorbed sulfur species limits the regeneration performance of MOFs . In recent years, HZSM-5 has drawn substantial attention because of its high thermal stability, high porosity, high mechanical strength, relatively low-cost reactivation, and excellent ion-exchange performance. , Therefore, HZSM-5 is considered an ideal sorbent matrix. Metal oxides supported on HZSM-5 may have substantial potential for the removal of H 2 S and PH 3 from industrial tail gas.…”

Section: Introductionmentioning

confidence: 99%

Cu/HZSM-5 Sorbent Treated by NH₃ Plasma for Low-Temperature Simultaneous Adsorption–Oxidation of H₂S and PH₃

Feng

Wang

et al. 2021

ACS Appl. Mater. Interfaces

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In this study, an NH3 plasma-treated Cu/HZSM-5 sorbent was introduced to simultaneously remove H2S and PH3 in low-temperature and low-oxygen environments. The effects of the Cu loading amounts, modification methods, and plasma-treatment conditions on the adsorption–oxidation performance of the sorbents were investigated. From the performance test results, the sorbent treated by NH3 plasma with the specific energy input (SEI, electrical input energy to the unit volume of gas) value of 1 J·mL–1 (Cu/HZSM-5-[S1]) was identified as having the highest breakthrough capacities of 108.9 mg S·g–1 and 150.9 mg P·g–1 among all of the materials tested. After three times of regeneration, the sorbent can still maintain the ideal performance. The results of Fourier transform infrared (FT-IR) spectroscopy and CO2 temperature-programmed desorption (CO2-TPD) indicated that the NH3 plasma treatment can introduce amino groups (functional groups) onto the sorbent surface, which greatly increases the number and strength of the basic sites on the sorbent surface. Results of N2 adsorption/desorption isotherms and scanning electron microscopy–energy dispersive spectroscopy (SEM–EDS) showed that the morphology of the sorbent changed after the plasma treatment, which exposed more active sites (copper species). In situ IR spectra showed that the amino groups are continuously consumed during the reaction process, indicating that these amino groups can help sorbents to capture gas molecules. Moreover, X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS) analyses indicated that CuO is the main active species and the consumption of CuO and accumulation of the reaction products on the surface and inner pores of the sorbent are the primary reasons for the deactivation of the sorbent.

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Reaction behaviors of CH3CN catalytic combustion over CuCeO -HZSM-5 composite catalysts: The mechanism of enhanced N2 selectivity

Cited by 36 publications

References 57 publications

Acetonitrile Combustion over Copper-Based Nanocatalysts: A Structure-Performance Relationship Study

Acetonitrile Combustion over Copper-Based Nanocatalysts: A Structure-Performance Relationship Study

Highly Active and Selective Multicomponent Fe–Cu/CeO₂–Al₂O₃ Catalysts for CO₂ Upgrading via RWGS: Impact of Fe/Cu Ratio

Cu/HZSM-5 Sorbent Treated by NH₃ Plasma for Low-Temperature Simultaneous Adsorption–Oxidation of H₂S and PH₃

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Reaction behaviors of CH3CN catalytic combustion over CuCeO -HZSM-5 composite catalysts: The mechanism of enhanced N2 selectivity

Cited by 36 publications

References 57 publications

Acetonitrile Combustion over Copper-Based Nanocatalysts: A Structure-Performance Relationship Study

Acetonitrile Combustion over Copper-Based Nanocatalysts: A Structure-Performance Relationship Study

Highly Active and Selective Multicomponent Fe–Cu/CeO2–Al2O3 Catalysts for CO2 Upgrading via RWGS: Impact of Fe/Cu Ratio

Cu/HZSM-5 Sorbent Treated by NH3 Plasma for Low-Temperature Simultaneous Adsorption–Oxidation of H2S and PH3

Contact Info

Product

Resources

About

Highly Active and Selective Multicomponent Fe–Cu/CeO₂–Al₂O₃ Catalysts for CO₂ Upgrading via RWGS: Impact of Fe/Cu Ratio

Cu/HZSM-5 Sorbent Treated by NH₃ Plasma for Low-Temperature Simultaneous Adsorption–Oxidation of H₂S and PH₃