INORGANIC CHEMISTRY
·
2024
·
IF 4.3
Zhiqiang Wang,Xiaomei Zhou,Gehui Wang,Qing Tong,Haiqin Wan,Lin Dong
The elimination of toluene is an obligatory target with increasing VOC emission in recent years. This study successfully prepared a single-atom Ir catalyst (Ir1/CeO2) by a simple incipient wetness impregnation method, confirmed by in situ CO DRIFTS and AC-HAADF-STEM. Compared to the cluster Ir catalyst (Ir/CeO2-C), Ir1/CeO2 exhibited excellent catalytic performance, stability, and water resistance for the oxidation of toluene. By Raman, H2-TPR, O2-TPD, and XPS experiments, abundant oxygen defects and a unique Ir3+–Ov–Ce3+ structure were formed for the Ir1/CeO2 sample because it had a lower oxygen vacancy formation energy. Furthermore, the DFT results revealed that the Ir1/CeO2 sample had a lower ring-opening energy barrier and adsorption energy of the ring-opening products, which was the rate-determining step for the oxidation of toluene. This work provides instructive insights into the construction of Ir/CeO2 catalysts for the highly efficient removal of VOCs.
研究领域:
催化化学
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环境科学
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材料科学
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产品关联
DOI
PubMed
高影响因子
Molecular Catalysis
·
2020
·
IF 3.687
Jiajun Dai,Yunlong Guo,Luhang Xu,Guilin Zhuang,Yi Zheng,Daohua Sun,Jiale Huang,Qingbiao Li
Bovine serum albumin (BSA)-templated CeO 2 was prepared by citrate sol-gel method and used as a support to synthesize Au catalyst for benzene oxidation. It was found that the Au/BSA-CeO 2 with 3.2 nm Au nanoparticles (NPs) gave rise to superior catalytic performance for benzene oxidation in which the temperature for 90 % benzene conversion was only 210 °C. In addition, the catalytic activity of Au/BSA-CeO 2 remained stable for 140 h of on-stream reaction. Besides, density functional theory calculation demonstrated how the porous structure of CeO 2 influenced the oxygen vacancy generation, and the synergetic effects of Au NPs and CeO 2 support facilitated the activation of benzene which was adsorbed on Au NPs prior to benzene oxidation. The catalysis of benzene oxidation over Au/CeO 2 catalyst follows the dual-site mechanism. BAS-templated CeO 2 support possessed hierarchical structure, abundant adsorbed oxygen species and synergic interaction with Au that determined the performance of Au/BSA-CeO 2 .
研究领域:
催化化学
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材料科学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
Solar RRL
·
2022
·Vol. 6
·期 8
·2200279
·
IF 9.173
Jie Deng,Wanying Lei,Junwei Fu,Huile Jin,Quanlong Xu,Shun Wang
Herein, photocatalytic selective oxidation of hydrocarbons through O 2 represents a promising way for fine chemical industry on account of its mild reaction condition. In this work, Co 3 O 4 -modified BiOBr/AgBr S-scheme heterojunction can effectively oxidize sp 3 C H bonds at benzylic position to its corresponding aldehydes, with a toluene to benzaldehyde selectivity of 94%, which is much higher than that of pure BiOBr (21.7%) and AgBr (58.9%). A unique S-scheme charge-transfer mode is confirmed for the ternary composites by the X-ray photoelectron spectroscopy and reactive species quenching measurement. The remaining photogenerated electrons in AgBr with powerful reduction ability can react with O 2 to generate •O 2 − species, which can further oxidize the benzyl radical formed on the Co 3 O 4 surface to peroxyl radicals and then thermodynamically decompose to benzaldehyde. Herein, this work has important guiding significance for the structure regulation of photocatalysts and application in selective oxidation of sp 3 C H bond of hydrocarbons.
研究领域:
材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Jiaqi Wu,Jian Tian,Weijian Zhou,Siyu Liu,Daohua Sun
In the catalytic combustion of volatile organic compounds (VOCs) using noble metal catalysts, resistance to SO 2 poisoning poses a significant challenge. To tackle this problem, Pt nanoparticle catalysts encapsulated in hollow carbon spheres (Pt@HCS catalysts) are synthesized. The Pt@HCS catalyst exhibits excellent benzene conversion, achieving 100 % conversion at 165 °C under an air velocity of 20,000 mL/(g h). Compared to the conventional supported Pt/HCS catalyst, the Pt@HCS catalyst demonstrates a significantly improved resistance to SO 2 poisoning. In the presence of 25 ppm SO 2 , the Pt@HCS catalyst is capable of maintaining a 100 % benzene conversion rate within 24 h, whereas the conversion rate of Pt/HCS drops substantially to approximately 52 %. It is confirmed that the hollow porous structure provided a larger specific surface area and more adsorption sites, thereby facilitating benzene oxidation. More importantly, in situ DRIFTS reveals that the adsorption and desorption processes of SO 2 , along with the generation of substances like SO 3 2− , are strictly limited to the surface of the carbon shell, thereby preserving the integrity of the internal reaction environment. Multiple characterizations combined with density functional theory (DFT) have demonstrated a unique separation effect over Pt@HCS, whereby the hydroxyl groups on the carbon shell preferentially capture SO 2 while allowing benzene molecules to enter the cavities of the catalyst. In this way, any internal ingress of SO 2 and competition with benzene for Pt adsorption is effectively avoided. This study offers a potential solution to enhance the performance of noble metal catalysts in the presence of sulfur compounds.
研究领域:
环境科学
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材料科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2024
·
IF 4.8
Jie Fan,Lutao Mao,Mingli Fu,Peng Liu,Zuliang Wu,Daiqi Ye
The high efficiency and stability of catalysts are crucial for their practical application in toluene oxidation . Herein, a novel octahedral Pt/Mn 3 O 4 -110 catalyst with excellent structural stability was synthesized and 100 % toluene conversion can be achieved at low-temperature 160 °C. XRD and Raman results indicated that the structure of Pt/Mn 3 O 4 -110 can be well maintained after 120 h on-stream reaction, the resistance to H 2 O (3 or 5 vol%) and high concentration toluene (3000 ppm)/CO 2 (5 vol%) tests. In situ DRIFTS comparative studies between Pt/Mn 3 O 4 -110 and Pt/Mn 3 O 4 -100 (30 % toluene conversion at 160 °C) samples demonstrated that the rate-control steps of toluene oxidation on Pt/Mn 3 O 4 -110 and Pt/Mn 3 O 4 -100 were both the further oxidation of benzoate species in the presence of gas-phase oxygen, while the transformation of benzaldehyde to benzoate species was the rate-control step on Pt/Mn 3 O 4 -100 in the absence of gas-phase oxygen. The weaker Mn-O bonds, richer oxygen vacancies and higher mobility of oxygen species on Pt/Mn 3 O 4 -110 sample than that of Pt/Mn 3 O 4 -100 are beneficial for the easier release of lattice oxygen from the surface of catalyst and then participated in toluene oxidation via Mars-van Krevelen mechanism, contributing to easier oxidation of benzaldehyde to benzoate species and formation of formic acid and bicarbonate species.
研究领域:
催化化学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Sciences
·
2024
·
IF 5.9
Xuan Liang,Jin Zhang,Juntai Tian,Zenghua Xie,Yue Liu,Peng Liu,Daiqi Ye
Herein, three supported catalysts, CuO/Al 2 O 3 , CeO 2 /Al 2 O 3 , and CuO-CeO 2 /Al 2 O 3 , were synthesized by the convenient impregnation method to reveal the effect of CeO 2 addition on catalytic performance and reaction mechanism for toluene oxidation. Compared with CuO/Al 2 O 3 , the T 50 and T 90 (the temperatures at 50% and 90% toluene conversion, respectively) of CuO-CeO 2 /Al 2 O 3 were reduced by 33 and 39 °C, respectively. N 2 adsorption-desorption experiment, XRD, SEM, EDS mapping, Raman, EPR, H 2 -TPR, O 2 -TPD, XPS, NH 3 -TPD, Toluene-TPD, and in-situ DRIFTS were conducted to characterize these catalysts. The excellent catalytic performance of CuO-CeO 2 /Al 2 O 3 could be attributed to its strong copper-cerium interaction and high oxygen vacancies concentration. Moreover, in-situ DRIFTS proved that CuO-CeO 2 /Al 2 O 3 promoted the conversion of toluene to benzoate and accelerated the deep degradation path of toluene. This work provided valuable insights into the development of efficient and economical catalysts for volatile organic compounds.
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
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL
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2015
·
IF 3.615
Qiming Zhao,Kexian Chen,Wensong Zhang,Jia Yao,Haoran Li
A metal- and initiator-free catalytic system comprising N -hydroxyquinolinimide (NHQI) and 4-carboxyl- N -hydroxyphthalimide (Car-NHPI) was developed for the oxidation of ethylbenzene using molecular oxygen as the terminal oxidant. The catalytic activity of Car-NHPI/NHQI catalytic system was higher than that of Car-NHPI or NHQI alone. The high catalytic performance of Car-NHPI/NHQI catalytic system could be attributed to the dual interactions of radical exchange and acid-base neutralization, which resulted in the increment of the conversion of ethylbenzene up to 70% and the selectivity of acetophenone up to 66% at 120 °C under 1 atm O 2 for 15 h.
研究领域:
化学工程
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2021
·
IF 3.764
Jian Tian,Lu Wang,Lixue Qi,Qun Li,Daohua Sun,Qingbiao Li
As an abundant and renewable biological resource, straw has been attracting wide attention due to its distinctive tubular structure and property. Herein, soybean straw was pretreated by KOH and was used as a support for Pt nanoparticles (NPs) to realize efficient benzene combustion. The scanning electron microscopy (SEM) and transmission electron microscopy (TEM) images of straw-derived samples illustrated the channel wall with open macropores and uniform distribution of Pt NPs in the straw skeleton. As a result, the temperature for 90% benzene conversion (T90%) by Pt/KAC-3 (Pt/KAC-n, where n represents the mass ratio of straw to KOH that was varied between 1:1, 1:2, and 1:3) was determined to be 179 °C under a space velocity (SV) of 120 000 mL/(g·h). Additionally, thermal stability was enhanced to nearly 96 h. This performance is predominantly attributed to its inherent channel structure, which has open and accessible pores, resulting in a uniform distribution of Pt NPs. Such structure enables the rapid transfer of benzene molecules between channels and ensures the accessibility of Pt NPs. Furthermore, the diffusion properties were confirmed by Fick’s second law. This study demonstrated a design of more efficient catalysts while using a renewable and abundant biomaterial.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2022
·
IF 8.047
Xiaodong Zhang,Fukun Bi,Zhenyuan Zhao,Yang Yang,Yintao Li,Liang Song,Ning Liu,Jingcheng Xu,Lifeng Cui
Supported single-atoms and sub-nanometre clusters have exhibited superb catalytic performance toward many reactions. However, inactivation of single-atom or cluster catalysts in complex reactive conditions poses major challenge for their practical application. Herein, we demonstrate that the prepared Pd-UiO-66 with ultra-low Pd loading (0.05 wt%) contains three robust active Pd species, (isolated Pd atom (Pd 1 ), sub-nanometre Pd clusters (Pd c ) and Pd nanoparticles (Pd n )) and presents superb activity for toluene oxidation and water resistance (10.0 vol%). Experiments and theoretical calculations firstly confirm that consecutive H 2 -O 2 and reaction gas treatment (1000 ppm toluene in 20 vol.%O 2 /Ar) induce residual N species from solvent N, N-dimethylformamide to enter UiO-66 skeleton forming Pd 1 -N 1 structures. DFT calculations reveal that the synergistic effect of Pd species (namely, the enhanced activation of O 2 and H 2 O by Pd 1 and the improved adsorption of toluene by Pd c and Pd n ) is the main factor for the excellent activity of Pd-U-H-O-reused catalyst.
研究领域:
催化化学
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环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
CATALYSIS LETTERS
·
2023
·
IF 2.8
Zhong Zhihao,Liu Yalan,Liu Shantang
To develop and design highly efficient composite oxide nanoparticles for the combustion of chlorinated volatile organic compounds (CVOCs), a series of Co 3 O 4 /In 2 O 3 catalysts were synthesized and tested for the catalytic oxidation of chlorobenzene (CB) as a typical example for CVOCs. The catalytic performance of as-prepared samples manifested that In x Co 1 O y nanorods catalysts with an appropriate proportion of In/Co exhibited superior catalytic activity better than that of pure Co 3 O 4 nanorods, indicating that the strong interactions between cobalt oxide and indium oxide assisted the degradation of CB. To understand the synergistic mechanism, a series of experimental characterization have been employed to explore the physicochemical properties of the catalysts. The result indicates that the introduction of In 2 O 3 increases the Co 3+ contents and the mobility of surface oxygen species, which synergistically contribute to the degradation process of chlorobenzene. Furthermore, the intermediates that appeared in the process of CB degradation on the In 3 Co 1 O y catalyst have been monitored by in situ DRIFTS. The detailed reaction mechanism is established by the analysis of the intermediates. Graphical Abstract
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
INORGANIC CHEMISTRY
·
2023
·
IF 4.6
Qun Li,Wenyu Zhou,Chunyan Deng,Chenyang Lu,Peng Huang,Dong Xia,Luxi Tan,Cailong Zhou,Yong-Wei Zhang,Lichun Dong
In catalytic oxidation reactions, the presence of environmental water poses challenges to the performance of Pt catalysts. This study aims to overcome this challenge by introducing hydroxyl groups onto the surface of Pt catalysts using the pyrolysis reduction method. Two silica supports were employed to investigate the impact of hydroxyl groups: SiO2–OH with hydroxyl groups and SiO2–C without hydroxyl groups. Structural characterization confirmed the presence of Pt–Ox, Pt–OHx, and Pt0 species in the Pt/SiO2–OH catalysts, while only Pt–Ox and Pt0 species were observed in the Pt/SiO2–C catalysts. Catalytic performance tests demonstrated the remarkable capacity of the 0.5 wt % Pt/SiO2–OH catalyst, achieving complete conversion of benzene at 160 °C under a high space velocity of 60,000 h–1. Notably, the catalytic oxidation capacity of the Pt/SiO2–OH catalyst remained largely unaffected even in the presence of 10 vol % water vapor. Moreover, the catalyst exhibited exceptional recyclability and stability, maintaining its performance over 16 repeated cycles and a continuous operation time of 70 h. Theoretical calculations revealed that the construction of Pt–OHx sites on the catalyst surface was beneficial for modulating the d-band structure, which in turn enhanced the adsorption and activation of reactants. This finding highlights the efficacy of decorating the Pt surface with hydroxyl groups as an effective strategy for improving the water resistance, catalytic activity, and long-term stability of Pt catalysts.
研究领域:
化学
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催化科学
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环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Reaction Kinetics Mechanisms and Catalysis
·
2018
·Vol. 125
·期 2
·707-731
·
IF 1.515
Li Wang,Zhang Qingjun,Zeng Aiwu
A systematic study on the synthesis of the Cu x Mn 3.66−x Mo 3 O 12 using citrate sol–gel technique is presented. The influence of the copper substitution, citric acid concentration and pH of the precursor solution on the exclusive formation of Cu–Mn–Mo polymetallic oxide are studied. The physicochemical properties of as-prepared oxides are characterized by XRD, ICP-MS, SEM, TEM, XPS, FT-IR, BET, and H 2 -TPR, and their dependence on the conditions of synthesis is explored. It is found that these three synthesis factors remarkably alter the crystal phases and surface structures. The catalytic behaviors of synthesized catalysts for liquid-phase toluene oxidation are evaluated with toluene-catalyst mixture under uniformly distributed conditions. The evaluation reveals that the ratios of Mn 3+ /Mn 2+ as well as O ads /O lat on catalysts play a crucial role in the activity and selectivity. Factors effecting reaction parameters, such as reaction temperature, residence time, catalyst weight, promoter weight, airflow rate and the volume ratio of substrate to solvent, are investigated in detail. The reusability of the catalyst is examined through conducting repeat runs with the same catalyst, exhibiting no significant decline in its activity even after 8 runs. A toluene conversion of 60% with 57.4% selectivity toward benzaldehyde is observed after 4 h over the high-crystalline Cu x Mn 3.66−x Mo 3 O 12 nanoparticles.
研究领域:
材料科学
·
催化化学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）