One-step control of Brønsted acid sites and oxygen vacancies in Mn-based perovskite for boosting catalytic oxidation of chlorobenzene

Wu, Haixia; Zhang, Wenjing; Liu, Yuwei; Zhou, Bing; Liu, Jingyin; Liu, Lizhong

doi:10.1016/j.jece.2023.110210

Cited by 5 publications

(2 citation statements)

References 54 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…Furthermore, O 2 -TPD results (Supporting Information Figure S30) also suggested the presence of the highest number of oxygen defects/vacancies in the MIL88B-800PMA catalyst, which can enhance the amount of reactive oxygen species on the catalyst surface and can improve the oxidation capability of the MIL88B-800PMA catalyst. 98 These sites are advantageous for catalytic activity. 99 Previously, Liu et.…”

Section: In Situ Atr-irmentioning

confidence: 99%

Unraveling High Chemoselectivity in Oxidative Dehydration of Glycerol into Acrylic Acid over a Bifunctional Metal–Organic Framework–Polyoxometalate Composite Catalyst

Koley,

Chandra Shit,

Yoshida

et al. 2024

ACS Catal.

View full text Add to dashboard Cite

The selective conversion of glycerol into acrylic acid (AA) using polyoxometalate catalysts poses a challenge due to low conversion and selectivity, as the acrolein intermediate is not effectively stabilized on the catalyst surface. In this study, we introduce a novel approach to develop a bifunctional active catalyst that incorporates dehydration and oxidation active sites while also confining these sites within a porous material to enhance product selectivity. A unique synthetic method was devised to create such a bifunctional catalyst (MIL88B-800PMA) comprising a metal− organic framework (MIL88B) and polyoxometalate (PMA). These catalysts demonstrated 100% conversion with 96.4% selectivity toward AA under mild reaction conditions. The complete encapsulation of PMA can account for the high catalytic activity within the pores of the MOF, facilitating the chemical bond formation and structural modulation between PMA and the MOF, as confirmed by detailed X-ray absorption spectroscopy (XAS) analysis. The presence of oxidative species such as Mo 6+ and Fe 2+ , along with oxygen vacancies, promotes the highest catalytic conversion and selectivity. A comprehensive kinetic study, including in situ ATR-IR analysis, illustrates the formation and stabilization of the specific intermediate acrolein, guiding the selective formation of AA. This finding is corroborated by theoretical quantum chemistry calculations, offering a quantitative understanding of the surface interaction between glycerol and the Brønsted acid sites present on the MIL88B and PMA composite catalysts. Additionally, the activation energy of the synthesized catalysts is evaluated, aiding in the comprehension of the underlying reasons for their high catalytic activity.

show abstract

Section: In Situ Atr-irmentioning

confidence: 99%

Unraveling High Chemoselectivity in Oxidative Dehydration of Glycerol into Acrylic Acid over a Bifunctional Metal–Organic Framework–Polyoxometalate Composite Catalyst

Koley,

Chandra Shit,

Yoshida

et al. 2024

ACS Catal.

View full text Add to dashboard Cite

show abstract

“…CB S are easily released into the environment and cause serious air pollution, water pollution and soil pollution, particularly through the formation of dioxins, photochemical smog, ozone layer deterioration and haze [15]. In addition, CB S are toxic to humans and accumulate in the human body, which damages the liver, kidney, immune system and nervous system and can lead to cancer, deformity and mutation [16]. Thus, CB S were listed as the priority control as typical persistent VOCs in many countries and regions, and their treatment has emerged as a critical issue worldwide.…”

Section: Introductionmentioning

confidence: 99%

Treatment of Monochlorobenzene from Polymers Process through Electrochemical Oxidation

Wang,

Yue,

Wang

et al. 2024

Polymers

View full text Add to dashboard Cite

With the rapid development of the economy and the demands of people’s lives, the usage amount of polymer materials is significantly increasing globally. Chlorobenzenes (CBS) are widely used in the industrial, agriculture and chemical industries, particularly as important chemical raw materials during polymers processes. CBS are difficult to remove due to their properties, such as being hydrophobic, volatile and persistent and biotoxic, and they have caused great harm to the ecological environment and human health. Electrochemical oxidation technology for the treatment of refractory pollutants has been widely used due to its high efficiency and easiness of operation. Thus, the electrochemical oxidation system was established for the efficient treatment of monochlorobenzene (MCB) waste gas. The effect of a single factor, such as anode materials, cathode materials, the electrolyte concentration, current density and electrode distance on the removal efficiency (RE) of MCB gas were first studied. The response-surface methodology (RSM) was used to investigate the relationships between different factors’ conditions (current density, electrolyte concentration, electrode distance), and a prediction model was established using the Design-Expert 10.0.1 software to optimize the reaction conditions. The results of the one-factor experiments showed that when treating 2.90 g/m3 MCB gas with a 0.40 L/min flow rate, Ti/Ti4O7 as an anode, stainless steel wire mesh as a cathode, 0.15 mol/L NaCl electrolyte, 10.0 mA/cm2 current density and 4.0 cm electrode distance, the average removal efficiency (RE), efficiency capacity (EC) and energy consumption (Esp) were 57.99%, 20.18 g/(m3·h) and 190.2 (kW·h)/kg, respectively. The results of the RSM showed that the effects of the process parameters on the RE of MBC were as follows: current density > electrode distance > electrolyte concentration; the interactions effects on the RE of MBC were in the order of electrolyte concentration and current density > current density and electrode distance > electrolyte concentration and electrode distance; the optimal experimental conditions were as follows: the concentration of electrolyte was 0.149 mol/L, current density was 18.11 mA, electrode distance was 3.804 cm. Under these conditions, the RE achieved 66.43%. The response-surface variance analysis showed that the regression model reached a significant level, and the validation results were in agreement with the predicted results, which proved the feasibility of the model. The model can be applied to treat the CBS waste gas of polymer processes through electrochemical oxidation.

show abstract

Progress of catalytic oxidation of VOCs by manganese-based catalysts

Zhou,

Su,

Xing

et al. 2024

Fuel

View full text Add to dashboard Cite

One-step control of Brønsted acid sites and oxygen vacancies in Mn-based perovskite for boosting catalytic oxidation of chlorobenzene

Cited by 5 publications

References 54 publications

Unraveling High Chemoselectivity in Oxidative Dehydration of Glycerol into Acrylic Acid over a Bifunctional Metal–Organic Framework–Polyoxometalate Composite Catalyst

Unraveling High Chemoselectivity in Oxidative Dehydration of Glycerol into Acrylic Acid over a Bifunctional Metal–Organic Framework–Polyoxometalate Composite Catalyst

Treatment of Monochlorobenzene from Polymers Process through Electrochemical Oxidation

Progress of catalytic oxidation of VOCs by manganese-based catalysts

Contact Info

Product

Resources

About