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CHEMOSPHERE · 2021 · IF 7.086

Well-dispersed iron and nitrogen co-doped hollow carbon microsphere anchoring by g-C3N4 for efficient peroxymonosulfate activation

Likun Chen,Kewen Xing,Qikai Shentu,Yifei Huang,Weiyang Lv,Yuyuan Yao

Developing single-atom Fenton-like catalysts with the maximum utilization of active sites present an attractive potential in environmental remediation. Herein, the single-atom Fe and N co-doped hollow carbon microsphere loaded g-C 3 N 4 catalyst (HFeNC-g-C 3 N 4 ) was prepared by an innovative cascade anchoring strategy using polystyrene as the hard template, iron phthalocyanine, polydopamine and urea as the Fe, N and C precursor, in which the in-situ generated g-C 3 N 4 could not only effectively anchor Fe atom to create the well-dispersed Fe-N x active sites, but also accelerate the electron transfer in peroxymonosulfate (PMS) activation. Taking advantages of such sequential protecting strategy, the as-synthesized HFeNC-g-C 3 N 4 catalyst with single-atom Fe-N x active sites, verified by XRD , XPS and HAADF-STEM, could work as an efficient Fenton-like catalyst for PMS activation, which achieved almost 100% removal of 4-chlorophenol (4-CP) in 5 min with the turnover frequency calculated to be 34.6 times higher than that of the homogeneous Fe 2+ catalyst. The mechanism of O 2 •- dominated radical combined with nonradical 1 O 2 pathway was confirmed by quenching experiments and ESR analysis, which might be interrelated to the improvement of pH adaptability and interference immunity of HFeNC-g-C 3 N 4 /PMS system. Overall, the present findings provided an innovation strategy for the synthesis of excellent single-atom Fe based catalyst in wastewater purification.

研究领域: 环境科学 · 催化 · 材料科学
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POLYMER DEGRADATION AND STABILITY · 2021 · IF 5.03

A pseudo-homogeneous system for PET glycolysis using a colloidal catalyst of graphite carbon nitride in ethylene glycol

Zishuai Wang,Yaoqiang Wang,Shengnan Xu,Yu Jin,Zequn Tang,Gang Xiao,Haijia Su

Glycolysis of poly (ethylene terephthalate) (PET) is a promising way to recycle waste PET and produce bis-(2-hydroxyl ethyl) terephthalate (BHET), the monomer of PET. However, traditional catalysts will cause environment pollution and economic burden. In this work, based on the green and low-cost graphitic carbon nitride colloid, we developed a pseudo-homogeneous system for PET glycolysis, and poly (bisphenol A carbonate) (BPA-PC) and polylactic acid (PLA) methanolysis. Using this system, 100% conversion of PET and 80.30% yield of BHET were achieved, and the reaction time was 2-8 times shorter than that of other metal-based catalysis systems. Catalyst and ethylene glycol were reused five times directly preserving their activity. Furthermore, the degradation of real commercial plastics has also been achieved. According to FT-IR, XPS, and 1 H NMR characterization results, the nucleophilic attack ability of ethylene glycol and electrophilicity of the PET carbonyl's carbon are enhanced by the formation of hydrogen bond between ethylene glycol, PET and catalyst.

CAS / MDL: 959-26-2
研究领域: 材料科学 · 化学工程 · 环境科学 · 催化 · 高分子化学 · 回收技术
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2021 · IF 19.503

Ingenious control of adsorbed oxygen species to construct dual reaction centers ZnO@FePc photo-Fenton catalyst with high-speed electron transmission channel for PPCPs degradation

Hengli Qian,Guanjie Yu,Qidong Hou,Yifan Nie,Chuanyunlong Bai,Xinyu Bai,Haozhi Wang,Meiting Ju

To achieve efficient degradation of pharmaceutical and personal care products (PPCPs), dual reaction centers [email protected] photo-Fenton catalysts with high-speed electron transmission channel were designed through surface hydroxyl-induced assembly. In [email protected] catalytic system, the photocatalysis center of ZnO and Fenton catalytic center of FePc were formed simultaneously. Concept and process for the control of hydroxyl groups to construct a dual reaction center [email protected] photo-Fenton catalyst were verified ingeniously based on the density functional theory (DFT) analysis and experimental results. A series of catalysts, including ZIF-8 (400 ℃-N 2 ), FePc (400 ℃-N 2 ), ZIF-8 (400 ℃)-FePc (400 ℃) and [email protected] were prepared and characterized by XRD, FTIR, TEM, BET, XPS, PL and DRS, respectively. The [email protected] catalyst showed superior performance for the photo-Fenton degradation of ibuprofen, affording degradation rate larger than 90 % within just 10 min under simulateed sunlight. The excellent performance of [email protected] catalyst is mainly attributed to the synergistic effect between dual reaction centers of [email protected] This work provides a novel method to construct dual reaction centers [email protected] catalyst with efficient photo-generated electrons transmission link and to strengthen the synergistic effect of dual reaction centers.

CAS / MDL: 7761-88-8
研究领域: 环境化学 · 催化 · 材料科学 · 光化学
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS · 2020 ·Vol. 31 ·期 15 ·12467-12475 · IF 2.22

One-step self-triggered microwave-assisted fabrication of NiCo/graphene for microwave attenuation

Xie Xinxin,Wang Hui,Zhou Yanping,Huang Kama

Microwave-assisted reduction of graphene oxide (GO) has been reported to be very effective in producing high-quality reduced graphene oxide (rGO) and its composites. However, either pretreatment (e.g., heating) or an external trigger (e.g., copper wire) is required to initiate the process due to the poor microwave absorption ability of GO. In this work, we report a one-step self-triggered microwave-arcing approach for synthesizing rGO composites (NiCo/rGO) for the first time. Evidenced by permittivity value, the synergic microwave absorption between GO and the metal nitrate salts is found to play an important role in initiating the process. From XRD, Raman, XPS and TEM results, it is proposed that mildly reduced rGO is firstly formed after 10 s, which further enables stronger microwave absorption to facilitate the complete reduction of GO as well as formation of well-crystallized NiCo nanoparticles about 10 nm after 90 s. The as-synthesized product shows a minimum refection loss value of − 44.48 dB with an absorption bandwidth of 3.66 GHz at 4.5 mm.

CAS / MDL: 10026-22-9 13478-00-7
研究领域: 材料科学 · 纳米技术 · 电磁材料 · 复合材料
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2019 · IF 3.375

Selective Oxidation of Amino Alcohols to Amino Acids over Au Supported on Monoclinic ZrO2: Dominant Active Sites and Kinetic Study

Xiangzhan Meng,Yongqiang Zhang,Zengxi Li,Hui Wang,Suojiang Zhang

Au supported on monoclinic ZrO2 (Au/m-ZrO2) prepared by deposition–precipitation method showed excellent catalytic performance in the aerobic oxidation of amino alcohols to amino acids, i.e., glycine, alanine, serine, β-alanine, and 2-aminobutyric acid. The Au particle size and valence distribution of the gold species were adjusted by calcination temperature, as demonstrated by XRD, TEM, UV–vis DRS, XPS, and H2-TPR, which significantly influenced the catalytic activity but not the selectivity of amino acids. Metallic gold atoms on the surface were shown to be the active sites by the correlation between reaction rate per mole of metallic Au and Au particle size. The kinetics of oxidation of monoethanolamine (MEA) was studied in detail, and the results indicated that MEA oxidation is a first-order reaction with an activation energy of 52.8 kJ·mol–1.

研究领域: 催化 · 化学工程 · 材料科学 · 物理化学
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH · 2022 ·Vol. 29 ·期 24 ·36337-36350 · IF 5.19

Preparation of non-polluting Tb-doped mesoporous carbon nitride photocatalyst and study on the efficacy and mechanism of degradation of antibiotics in water

Wang Bing,Cao Qingtong,Li Guomin,Zhang Jian

Given that the biological treatment of antibiotic wastewater can easily induce resistant bacteria, the photocatalytic degradation of antibiotics is considered as a better method for treating antibiotic wastewater. Therefore, the ability to remove Tylosin (TYL) and Tetracycline (TC) in aqueous solution using rare earth element Tb-doped g-C 3 N 4 under simulated natural solar radiation was investigated. A series of rare earth Tb 3+ doped mesoporous g-C 3 N 4 were successfully prepared by nitric acid treatment and Tb(NO 3 ) 3 ·5H 2 O samples showed significantly higher degradation efficiency for TYL and TC than pure g-C 3 N 4 . Leaching toxicity experiments were carried out on the catalyst using chard seeds and demonstrated negligible toxicity of the leachate from the catalyst. The structure, elemental state, optical properties, morphology, and photogenerated carrier separation of the prepared xTCN catalysts were characterized by XRD, XPS, UV–Vis DRS, TEM, and PL. The results show that Tb doping enhanced the photocatalytic activity of the g-C 3 N 4 catalyst by narrowing the band gap while improving the light-trapping ability; The separation and transport rate of photogenerated carriers were significantly increased after Tb doping. Finally, a simple, efficient, and non-polluting Tb-doped carbon nitride photocatalyst is successfully developed in this paper.

研究领域: 环境科学 · 材料科学 · 化学 · 光催化
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Journal of Environmental Chemical Engineering · 2022 · IF 7.968

Preparation of a transition metal-supported TiO2 catalyst and the catalytic oxidative degradation of toluene

Zhengfeng Gu,Daiwei Liu,Mengnan Yu,Teng Bao,Xiaowei Liu,Ling Zhang,Haitao Ding,Zhimin Yu,Chengxun Deng

The synthesis of supported transition metal oxides with satisfactory low-temperature catalytic performance and application potential is still a challenge for the complete degradation of VOCs. Ni-Cu-loaded TiO 2 catalysts were prepared by an impregnation method. The lattice defect and oxygen vacancy concentrations of the prepared materials could be tuned by controlling the Ni/Cu molar ratio and the mass proportion of the TiO 2 support. 5Ni-Cu/TiO 2 exhibited the best catalytic activity and showed superior catalytic stability during complete toluene oxidation . The obtained catalysts were fully characterized by XRD, FT-IR, TEM, N 2 adsorption analysis, XPS, H 2 -TPR, O 2 -TPD, TPD analysis, and XPS. The 5Ni-Cu/TiO 2 catalyst had improved pore sizes and specific surface area, had more oxygen vacancies on its surface, had increased concentrations of adsorbed and lattice oxygen species, and had good redox properties; these characteristics were favorable for low-temperature catalytic performance and catalytic stability. Cyclic transformations of metal valence states between Cu + and Cu and between Ni and Ni 2+ were observed in the catalytic system. A potential catalytic reaction process based on the M-vK mechanism was proposed. This work serves as a reference for the application of supported transition metal catalysts for the degradation of VOCs.

CAS / MDL: 13463-67-7
研究领域: 催化 · 环境科学 · 材料科学
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APPLIED SURFACE SCIENCE · 2022 · IF 7.392

Enhanced visible-light-driven photocatalytic activity of bi-phase titanium dioxide @ covalent organic framework Z-scheme system for photocatalytic removal of Cr (Ⅵ)

Yi Wen,Zheng Huang,Min Zhao,Longshan Zhao

The discharge of industrial heavy metal wastewater not only leads to environmental pollution, but also harms human health, so it is imperative to control heavy metal pollution. In the current work, a sequence of anatase/brookite TiO 2 @COF with different mass ratios, bi-phase TiO 2 and bare COF were successfully synthesized by simple hydrothermal synthesis. The photocatalytic activity of the prepared catalysts was assessed by reducing Cr(Ⅵ) in model pollutant (K 2 Cr 2 O 7 ). Under the condition of pH = 3, the Cr(Ⅵ) reduction rate of TiO 2 @COF-4 was as high as 99.19% in 30 min. The photocatalytic activity of TiO 2 @COF-4 remained stable in four consecutive cycles, suggesting that it has a potential application prospect for the removal of Cr(Ⅵ) in the actual environment. The morphology and structure of photocatalysts were observed by different techniques (SEM/EDS, HRTEM, BET analysis, XRD, FTIR and XPS). The specific reasons for the enhancement of photocatalytic performance of materials were explored by different methods (PL, UV–vis DRS, Mott-Schottky plots, I-T curves and EIS). Finally, we concluded that the photocatalytic system of TiO 2 @COF-4 may follow the typical direct Z- scheme mechanism. This work provides an effective solution for the water treatment of heavy metal pollution.

研究领域: 环境科学 · 材料科学 · 化学工程 · 纳米技术
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JOURNAL OF POROUS MATERIALS · 2021 ·Vol. 28 ·期 6 ·1737-1747 · IF 2.496

Highly-dispersed Pd nanoparticles on UiO-66 in assistance of supercritical fluid and its catalytic performance of CO2 methanation

Jiang Haoxi,Zhao Yingying,Lin Jing,Chen Yifei,Wang Sheng

Highly dispersed palladium nanoparticles (NPs) supported on UiO-66 as catalyst for CO 2 methanation were prepared by supercritical fluid deposition (SFD). As a result, the most suitable Pd precursor salt and co-solvent are Na 2 PdCl 4 and ethanol/DMF, respectively. The best SFD process condition to deposit the Pd precursor on UiO-66 is 40 °C, 10 MPa and 2 h. Under the above condition, 4% Pd/UiO-66 exhibits the highest activity with 53% of CO 2 conversion and 95% of CH 4 selectivity while the turnover frequency (TOF) value is 3669.4 h −1 . The catalysts were characterized by XRD, BET, TEM, XPS, TGA, CO-DRIFTS and ICP-OES to investigate the structure–activity relationship. The 4% Pd/UiO-66 with the average size of 2.2 nm of Pd prepared in assistance of supercritical fluid behaved the similar activity as the 6%Pd/UiO-66 with average size of 9.7 nm of Pd prepared by sol–gel method. It is showed prospect of technique for reducing noble metal loading resulting from high dispersion effect.

研究领域: 催化 · 材料科学 · 化学工程 · 环境科学
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Sustainable Chemistry and Pharmacy · 2021 · IF 4.508

Study on corrosion inhibition behavior and adsorption mechanism of novel synthetic surfactants for carbon steel in 1 M HCl solution

Jingbao Wang,Jing Jing,Li Feng,Hailin Zhu,Zhiyong Hu,Xuemei Ma

The corrosion inhibition behavior and adsorption mechanism of three novel synthetic surfactants in 1 M HCl solution on carbon steel were investigated. The PP results confirmed that all the synthetic surfactants behave as mixed-type inhibitors, while the EIS results validated the existence of a protective layer by the adsorption of inhibitor molecules on the carbon surface. T 3 was observed to offer the highest inhibition efficiency ( η w , 96.28%) at 1 mM by the static weight loss measurements due to two different hydrophobic chains which form a more compact film with the crosswise arrangement. SEM/EDS and XPS results revealed the formation of the surfactants film on the carbon steel surface. Molecular dynamics simulation (MD) was further executed to determine the adsorption mechanism in molecular level insights. In addition, a linear correlation between surface activity ( γ ) and corrosion inhibition efficiency ( η w ) was verified. The adsorption of the prepared surfactants followed the Freundlich isotherm at different concentration ranges. Moreover, the bilayer/multilayer adsorption mechanism was also proposed and confirmed by experimental, adsorption isotherm studies and MD. Hence, both MD simulations and experimental results revealed the analogous inhibition with the order follows: T 3  > T 2  > T 1 .

研究领域: 材料科学 · 腐蚀工程 · 表面化学
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MACROMOLECULES · 2013 · IF 5.521

Synthesis of Highly Monodisperse Surface-Functional Microspheres by Photoinitiated RAFT Dispersion Polymerization Using Macro-RAFT Agents

Jianbo Tan,Xin Rao,Jianwen Yang,Zhaohua Zeng

Highly monodisperse PMMA microspheres have been synthesized by photoinitiated RAFT dispersion polymerization in the presence of a Macro-RAFT agent and a small molecular RAFT agent. A particle yield of over 90% was achieved within 3 h under UV irradiation at room temperature. The Macro-RAFT agent acts as a stabilizer and stabilizes the particles via formation of block copolymers in situ, and XPS analysis shows that about 29.9% of the particle surface was covered by the stabilizer. Various surface functional microspheres were prepared by using four kinds of Macro-RAFT agents, including poly(methoxy poly(ethylene glycol) acrylate)-based trithiocarbonate (P(mPEGA)-TTC), poly(methoxy poly(ethylene glycol) acrylate-co-acrylic acid)-based trithiocarbonate (P(mPEGA-co-AA)-TTC), poly(acrylic acid)-based trithiocarbonate (PAA-TTC), and poly(methoxy poly(ethylene glycol) acrylate-co-4-vinylpyridine)-based trithiocarbonate (P(mPEGA-co-4VP)-TTC). Ag/PMMA nanocomposite spheres were prepared using the P(mPEGA-co-AA)-TTC stabilized microspheres. The PAA-TTC stabilized microspheres showed pH sensitivity. The colloidal stability of the particles prepared by this photoinitiated RAFT dispersion polymerization was also investigated.

CAS / MDL: 2638-94-0
研究领域: 高分子化学 · 材料科学 · 纳米技术 · 胶体与界面科学
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RSC Advances · 2016 ·Vol. 6 ·期 86 ·82707-82715 · IF 3.289

The enhanced performance of a CeSiOx support on a Mn/CeSiOx catalyst for selective catalytic reduction of NOx with NH3

Wei Li,Rui-tang Guo,Shu-xian Wang,Wei-guo Pan,Qi-lin Chen,Ming-yuan Li,Peng Sun,Shu-ming Liu

A series of Mn/CeSiOx catalysts were prepared by the wet impregnation method and used for selective catalytic reduction of NO with NH3. As can be seen from the experimental results, the Mn/CeSiOx catalyst with a Ce/Si molar ratio of 2/1 showed excellent low-temperature SCR activity, high N2 selectivity and excellent SO2 and H2O tolerance. The relationship between the CeSiOx support and the SCR performance of Mn/CeSiOx (2 : 1) catalyst was investigated based on the characterization results of N2 adsorption, XRD, XPS, H2-TPR, NH3-TPD and in situ DRIFT. The strong interaction between Ce and Si resulted in the good dispersion of Mn species on the support; correspondingly, the redox ability and NH3 adsorption capacity were greatly enhanced. The results of in situ DRIFT study revealed that the NH3-SCR reactions over Mn/CeO2 and Mn/CeSiOx (2 : 1) mainly obeyed both the E–R mechanism and the L–H mechanism. Furthermore, the formation of more Mn4+ and chemisorbed oxygen greatly facilitates the oxidation of NO to NO2, as a result, promoting the low-temperature SCR performance of Mn/CeSiOx (2 : 1).

研究领域: 催化 · 环境科学 · 化工
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