Nature Catalysis
·
2022
·Vol. 5
·期 1
·45-54
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IF 40.706
Qi Guodong,Davies Thomas E.,Nasrallah Ali,Sainna Mala A.,Howe Alexander G. R.,Lewis Richard J.,Quesne Matthew,Catlow C. Richard A.,Willock David J.,He Qian,Bethell Donald,Howard Mark J.,Murrer Barry A.,Harrison Brian,Kiely Christopher J.,Zhao Xingling,Deng Feng,Xu Jun,Hutchings Graham J.
The oxidation of methane, the main component of natural gas, to selectively form oxygenated chemical feedstocks using molecular oxygen has been a long-standing grand challenge in catalysis. Here, using gold nanoparticles supported on the zeolite ZSM-5, we introduce a method to oxidize methane to methanol and acetic acid in water at temperatures between 120 and 240 °C using molecular oxygen in the absence of any added coreductant. Electron microscopy reveals that the catalyst does not contain gold atoms or clusters, but rather gold nanoparticles are the active component, while a mechanism involving surface adsorbed species is proposed in which methanol and acetic acid are formed via parallel pathways.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Zepeng Rao,Guanhong Lu,Lu Chen,Asad Mahmood,Gansheng Shi,Zixia Tang,Xiaofeng Xie,Jing Sun
To identify the distinctive role of reactive oxygen species (ROS) and trace the intermediates not only help to decompose the pollutants in high efficiency but also for avoiding more harmful intermediates formed. Here, we developed a new method to generate different ROSs by controlling the atmosphere to distinguish their role in the degradation of flowing gas-phase VOCs, including o -xylene, styrene, and acetaldehyde. This method is in good agreement with the traditional sacrificial agent capture experiment. The results show that • OH radicals play a dominant role in the degradation of o -xylene and styrene, while • O 2 − radicals primarily take part in the acetaldehyde degradation. Additionally, we distinguish the role of holes, • OH and • O 2 − played during the VOCs photo-oxidation through the radical trapping, in situ DRIFTS, and GC-MS analysis. Under the attack of • O 2 − radicals, aromatic VOCs were photo-oxidized to intermediates containing benzene rings and ketones (i.e., toluene and butanone), while carbon chain compounds (i.e., 3-methylfuran and ethanol) tend to form under the action of • OH and holes. This can be associated with the different reaction paths initiated by ROS. For acetaldehyde removal, •O 2 − species facilitate the formation of acids (i.e., acetic acid) while the •OH species and holes lead to the production of ketones (i.e., acetone). This work provides deep understanding on the role of various ROS in the photocatalytic oxidation of VOCs, which can guide the design of efficient photocatalysts, selective formation of intermediates to be easily decomposed or as raw materials for further application.
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JOURNAL OF THE EUROPEAN CERAMIC SOCIETY
·
2021
·
IF 5.302
Guangjin Chen,Cuiwei Li,Hao Li,Lu Wang,Kepi Chen,Linan An
Single-phase (Ce 0.2 Zr 0.2 Ti 0.2 Sn 0.2 Ca 0.2 )O 2-δ porous high-entropy ceramics have been in-situ fabricated by foam-gelcasting-freeze drying method at different temperatures. The microstructure, phase composition, and properties of the obtained ceramics were investigated. The results indicate that compared with other porous ceramics reported in the literatures, this type of ceramics exhibits excellent performance. The sample prepared at 1350 °C shows high porosity (88.6 %), low thermal conductivity (0.023 W m -1 K -1 ), and high compressive strength (1.48 MPa). The current study suggests that porous (Ce 0.2 Zr 0.2 Ti 0.2 Sn 0.2 Ca 0.2 )O 2-δ high entropy ceramics are promising candidates for thermal insulation applications.
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NEW JOURNAL OF CHEMISTRY
·
2024
·Vol. 48
·期 37
·16230-16242
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IF 2.7
Liang Wei,Sihong Li,Haibo Wang,Zimei Mo,Junji Chen,Meng Li,Hongxi Zhang,Jing Yang,Xiande Yang
Aflatoxin B1 (AFB1), a mycotoxin commonly found in foodstuffs, poses significant health risks when ingested through contaminated food sources. Therefore, it is imperative to devise a safe and efficient method for AFB1 degradation. Graphitic carbon nitride (g-C3N4) stands out as an exceptionally stable, non-toxic, and economical photocatalyst, which is widely used in photocatalysis. In this study, we explored the photocatalytic performance of four g-C3N4 catalysts derived from different precursors (dicyandiamide (D-CN), melamine (M-CN), thiourea (T-CN), and urea (U-CN)) in AFB1 degradation under visible light. Notably, the U-CN catalyst displayed an impressive degradation rate of 93.5% for AFB1 within 30 min, outperforming M-CN (82.5%), T-CN (78.5%), and D-CN (46.2%). This superior performance is attributed to its inherent porous structure, enlarged specific surface area, and reduced electron–hole pairs’ recombination rate. Additionally, our investigation identified ˙O2− as the primary active species in AFB1 degradation. Furthermore, we explored the degradation pathway of AFB1 and its associated inactivation mechanism mediated by the U-CN catalyst. This work provides a theoretical foundation for developing highly efficient photocatalysts in AFB1 degradation.
研究领域:
环境科学
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化学
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材料科学
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毒理学
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2019
·
IF 3.375
Qun Li,Tareque Odoom-Wubah,Yaping Zhou,Rafal Mulka,Yanmei Zheng,Jiale Huang,Daohua Sun,Qingbiao Li
The search for efficient and durable catalysts for volatile organic compounds oxidation is essential for environmental remediation. Herein, porous coral-like cobalt–manganese oxide (CoMnOx) catalyst was synthesized through annealing Co–Mn–1,3-propanediol precursors at 300 °C in air and applied for the catalytic oxidation of benzene. The as-prepared CoMnOx exhibited uniform porous coral-like structure, with an improved benzene catalytic abatement performance as compared to those of Mn3O4 and Co3O4 samples prepared by the same method, respectively. According to BET, H2-TPR, O2-TPD, and XPS analysis, the as-obtained CoMnOx catalyst showed the highest BET surface area, better low-reducibility temperature, and high content of absorbed oxygen groups when compared to Mn3O4 and Co3O4, which makes significant contribution to its catalytic benzene oxidation activity. Moreover, a plausible surface reaction mechanism for benzene oxidation over CoMnOx catalyst was also proposed through the in situ DRIFTS study.
研究领域:
环境科学
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催化
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材料科学
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NEW JOURNAL OF CHEMISTRY
·
2024
·Vol. 48
·期 6
·2558-2568
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IF 2.7
Shiman Zhou,Qianqian Zhu,Denan Li,Lifeng Zhang,Yanshuo Li,Zhenxin Zhang
Tetrabromobisphenol A (TBBPA), a prevalent brominated flame retardant, poses significant environmental and health risks, necessitating its removal. In this study, WO3 with different structures was synthesized for TBBPA photodegradation under visible light using H2O2 and O2 as oxidants. The catalyst exhibited robust stability and reusability, rendering it suitable for practical applications. The crystalline structure and surface structure of WO3 controlled its catalytic activity towards TBBPA photodegradation. Monoclinic WO3 with the (022) plane was found to be the most active for ˙O2− active species generation from H2O2 and thus active for TBBPA degradation. Degradation product analysis showed that the catalyst was active not only for the removal of TBBPA, but also for the debromination of TBBPA. Nearly 100% debromination was achieved.
研究领域:
环境科学
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材料科学
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化学工程
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
·
IF 8.1
Jiaming Wang,Feifei Kang,Yifei Chen,Xiujuan Zhang,Xiaobin Jiang,Gaohong He,Xuehua Ruan
Artificial lung membranes are the heart for extracorporeal oxygenation. Hereinto, the nonporous PDMS-based membranes have excellent biocompatibility, and also isolation ability to both blood and harmful matters. Nevertheless, their CO 2 /O 2 selectivity, in the conventional cases using pure-oxygen sweeping stream, is not enough to accomplish sufficient CO 2 removal in balance with O 2 addition. In this work, the oxygenation mode using oxygen-enriched stream, faithfully based on the permeation mechanism, is established to overcome this bottleneck. To neutralize the negative impacts caused by lowering oxygen content and its partial pressure, PDMS-based composite membranes with ultra-thin selective layer to enhance mass transfer have been fabricated successfully. The experiments manifest that the selective layer, on the basic condition that the composite structure is stable enough to make surface modification and realistic utilization, is decreased to 376 nm on the porous substrates. O 2 and CO 2 permeation rates through the ultimate membrane samples have been enhanced to 502 GPU and 4117 GPU, respectively. In this instance, the essential oxygenation could be sustained with O 2 partial pressure less than 446 mmHg in the sweeping stream. The minimum membrane area for a common treatment case is 0.05 square meters. Once the membrane area is increased to 0.18 square meters, the sterile air after purification could be directly used for oxygenation. In comparison to the oxygenation devices being used currently, membrane area can be saved by about 90 %, which is highly significant to reduce the injuring influence on blood cells. All in all, the artificial lung membranes with ultra-thin PDMS coating layer have promising future in realistic utilization.
研究领域:
生物医学工程
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材料科学
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
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2024
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IF 11.2
Shuang Zhou,Da Wen,Wei Zhong,Jianjun Zhang,Yaorong Su,Aiyun Meng
The effective adsorption of oxygen (O 2 ) molecules over photocatalysts is a critical step in promoting the performance of photocatalytic H 2 O 2 production. However, g-C 3 N 4 usually features a Yeager-type (side-on) adsorption configuration of O 2 molecules, which causes the breaking of O–O bonds and severely hinders the H 2 O 2 production activity. Herein, we synthesized an oxygen-vacancy-rich TiO 2– x /g-C 3 N 4 step-scheme (S-scheme) heterojunction to regulate the oxygen adsorption configuration and improve the 2e – ORR selectivity of H 2 O 2 production. In-situ X-ray photoelectron spectroscopy (in-situ XPS) and density functional theory (DFT) calculations reveal that the S-scheme heterojunction is formed between TiO 2– x and g-C 3 N 4 . The difference between their Fermi levels leads to the electron flow from g-C 3 N 4 to TiO 2– x , which increases the electron-deficient sites in g-C 3 N 4 . As a result, the cleavage of O–O bonds on the surface of g-C 3 N 4 is avoided and the oxygen adsorption configuration is tuned from Yeager-type to Pauling-type (end-on). Consequently, the photocatalytic H 2 O 2 production rate is dramatically improved to 1780.3 μmol h –1 , which is about 5 times higher than that of pristine g-C 3 N 4 . This work paves a new way to tailor the oxygen adsorption configuration by rationally designing S-scheme heterojunction photocatalysts.
研究领域:
材料科学
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催化化学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Changshun Deng,Xiaorong Zhu,Jun Yao,Yibo Wang,Chenyang Shen,Bingqing Ge,Chaoxiang Li,Nianhua Xue,Luming Peng,Xuefeng Guo,Yan Zhu,Yafei Li,Weiping Ding
The direct oxidation of toluene by O 2 to benzaldehyde with high efficiency is a bright route for the green production of benzaldehyde but still a significant challenge. In this study, we develop a ligand modification strategy by bonding organophosphonic acid (OPA) to VTiO x /γ-Al 2 O 3 to restructure its interface microenvironment for enhancement of toluene oxidation to benzaldehyde. The as-prepared catalyst exhibits excellent selectivity over 99 % under mild conditions. Results of comprehensive characterizations and calculations reveal that the OPA bonding in bidentate with the V 6-coordinated species causes noticeable phase reconstruction between VO x and TiO 2 , thereby generating nearby new reactive oxygen species, which is responsible for the conversion of toluene to benzaldehyde at temperatures as low as ∼50 °C, much lower than that over VO x /TiO 2 (>130°C). The interface microdomain around the bonding site of OPA helps to significantly weaken the methyl C H bond of toluene molecule in reaction manifested as the significant decrease in apparent activation energy. Hence, the current work reveals a novel mechanism of the typical catalyst VO x /TiO 2 under OPA bonding, which is useful to solve the classic difficult reaction of toluene to benzaldehyde by O 2 oxidation.
研究领域:
催化化学
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绿色化学
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PubMed
高影响因子
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
·
2017
·Vol. 164
·期 6
·A1321
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IF 3.259
Chaolumen Wu,Taoran Li,Chenbo Liao,Qingkai Xu,Yuancheng Cao,Lei Li,Jun Yang
Triethylene glycol dimethyl ether (G3) is evaluated as an electrolyte solvent for non-aqueous lithium-oxygen (Li-O2) batteries. A liquid electrolyte of 1 M LiTFSI in G3 shows lower viscosity, higher oxygen solubility and diffusion, higher ionic conductivity and lithium ionic transference number compared to the conventional liquid electrolyte of 1 M LiTFSI in tetraethylene glycol dimethyl ether (G4). Then the Li-O2 battery using the G3-based electrolyte shows better cycling stability and higher rate capability compared to the battery using the G4-based electrolyte. At a higher current density of 2.5 A gcarbon−1, the discharge capacity of the battery using the G3-based electrolyte is about 1472 mAh gcarbon−1, which is about four times higher than that of the battery using the G4-based electrolyte. At current density of 1 A gcarbon−1 with a fixed capacity of 1000 mAh gcarbon−1, the battery using the G3-based electrolyte can be operated stably for 80 cycles, while only 20 cycles are achieved by using the G4-based electrolyte. Therefore, we think the G3-based electrolyte could be a proper alternative electrolyte to the conventional G4-based electrolyte for the development of Li-O2 batteries.
研究领域:
材料科学
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电化学
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2018
·
IF 11.698
Meichao Gao,Jinxiang Yang,Tao Sun,Zizhong Zhang,Dafeng Zhang,Huijuan Huang,Huaxiang Lin,Yi Fang,Xuxu Wang
The photocatalytic overall conversion of CO 2 with H 2 O to chemical fuel and oxygen mimicking natural photosynthesis is a huge challenge in photocatalysis. This work shows the achievement of the solar-driven photocatalytic overall CO 2 reduction with H 2 O to CO and O 2 over a Persian buttercup-like BiOBr x Cl 1-x solid solution. A CO generation rate of 15.86 μmol g −1 h −1 with the approximate stoichiometric O 2 evolution is yielded on BiOBr 0.6 Cl 0.4 solid solution under simulated solar light irradiation, which was about 7.5 and 10.2 times higher than that of pure BiOCl (2.11 μmol g −1 h −1 ) and BiOBr (1.55 μmol g −1 h −1 ), respectively. The enhanced photoactivity is contributed to the mediate band gap and energy level tuned by the formation of BiOBr x Cl 1-x solid solution to facilitate the separation of photogenerated charges. Besides the unique electron structure, the photoinduced oxygen vacancy (O V ) formed on BiOBr x Cl 1-x solid solution also plays an important role in the CO 2 reduction.
研究领域:
化学
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材料科学
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环境科学
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CHINESE JOURNAL OF CHEMICAL ENGINEERING
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2020
·
IF 2.627
Yingfei Hou,Lin Jiang,Yaoyao Zhang,Zhiwen Qin,Chi Jiang,Ming Wang
Lithium-air (also known as lithium-oxygen) batteries have attracted considerable global attention in recent years due to their extremely high energy density (11,140 W·h·kg −1 ). The electrolyte is a key element in lithium-air batteries and the traditional organic electrolyte has great safety risk due to leakage. On the contrary, the polymer electrolyte has the advantages of high safety, high stability and easy processing comparing with the organic liquid electrolytes. In this paper, a new idea was proposed to coat the Nafion membrane on a layer of polymer for blocking the oxidation reduction electric (RM) and Li based on the selective permeability on lithium ion of the Nafion membrane. Self-made thickness-controllable Nafion membrane, polyvinylidene fluoride-hexafluoropropylene copolymer (PVDF-HFP) and 2,2,6,6-tetramethylpiperidinooxy (TEMPO) were used to prepare a quasi solid polymer electrolyte (NSPE). Electrochemical workstation and LAND battery testing system were used to perform a galvanostatic charge/discharge test on Li-O 2 . The ionic conductivity of NSPE was 4.3 × 10 −4 S·cm −1 at room temperature and the discharge platform was 2.6 V and the charging voltage was 3.7 V after 50 cycles with the cut-off capacity of 500 mA·h·g −1 .
研究领域:
材料科学
·
电化学
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