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EES Catalysis · 2024 · IF 0

Photothermal catalytic oxidation of toluene over Pt-Mn2O3/CN nanocomposite catalyst

Xiao Yu,Chuang Zhao,Lixia Yang,Jian Zhang,Chunlin Chen

The Pt-Mn2O3/CN catalyst formed through the synthesis via the solvent-thermal method involves a synergistic combination of polymer CN and Pt nanoparticles loaded on Mn2O3 to catalyze the degradation of toluene. The composition incorporates Mn2O3 as the central element for photothermal conversion, CN as a uniformly dispersed matrix for Pt nanoparticles, and Pt as the catalytically active center, demonstrating significant efficacy. Particularly noteworthy is the discernible enhancement in the photothermal catalytic degradation capability of the Pt-Mn2O3/CN composite catalyst, specifically in the context of toluene. When subjected to light intensity of 300 mW cm-2 and a toluene concentration of 400 ppm, Pt-Mn2O3/CN achieves toluene conversion and CO2 mineralization rates of 99% and 80.9%, respectively. This improvement primarily stems from the Pt nanoparticles inducing a substantial presence of oxygen vacancies within the catalyst structure, thereby increasing oxygen adsorption capacity and surface mobility. This, in turn, activates adsorbed oxygen species at the catalyst’s interface. The adept utilization and conversion of solar irradiance for volatile organic compound (VOC) abatement underscore its potential as an environmentally friendly and renewable energy source.

研究领域: 环境科学 · 材料化学 · 催化化学
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JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL · 2016 · IF 3.958

Roles of the active species involved in the photocatalytic oxidation of benzyl alcohol into benzaldehyde on TiO2 under UV light: Experimental and DFT studies

Lei Zhao,Baoyue Zhang,Xin Xiao,Feng Long Gu,Rui-Qin Zhang

Active species such as holes, electrons, hydroxyl radicals ( OH), and superoxide radical anions ( O 2 − ) involved in the photocatalytic oxidation of benzyl alcohol (BA) into benzaldehyde (BAD) on TiO 2 under ultraviolet (UV) light were investigated by adding corresponding scavengers. The experimental results show that the oxidation of BA into BAD is driven mainly by the holes and OH radical. The role of dissolved O 2 was studied by bubbling N 2 through the reaction. The results show that the dissolved O 2 is, to some extent, the source of OH. Additional density functional theory (DFT) calculations identified two H-abstraction pathways ( R abs OH and R abs α). The structure of the R abs OH product is less stable and tends to transfer resulting in the R abs α product. The holes are the main driving force for the abstracting of H from BA. The OH radical combines with the H-abstract product to form a precursor of product BAD, detected by LC–MS technique ( m / z 123), which then undergoes an intramolecular dehydration reaction to form BAD. The results will help to select the optimal active species for the photocatalytic oxidation of BA into BAD on TiO 2 under UV light.

研究领域: 物理化学 · 光催化 · 环境化学 · 材料化学 · 理论计算化学
✓ 已验证 DOI 高影响因子
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS · 2018 ·Vol. 29 ·期 16 ·13925-13930 · IF 2.324

Structure, morphology and electrical conductivity of Sm and Bi co-doped CeO2 electrolytes synthesized by co-precipitation method

Li Tianjing,Shi Qingle

In this paper, explain a new relationships between Bi 3+ content, the phase crystal, microstructure and conductivity for Sm and Bi co-doped Ce 0.8− x Sm 0.2 Bi x O 1.9−1/2 x ( x  = 0, 0.05, 0.1, 0.15, 0.2) electrolytes prepared by co-precipitation method. The XRD patterns showed that this compounds exhibit a fluorite-type cubic structure after the samples calcined at 700 °C for 4 h and the cell volumes of increased when the Bi content increased. In addition, for the samples sintered at 1400 °C for 4 h, the Bi doping improves the relative density, the grain size and the average thermal expansion coefficient (TEC). More in details, the relative density and TEC increase with the Bi content. Form the AC impedance spectroscopy measurements, the conductivity of the sintered samples is found to improve with the increasing of Bi content (for x  ≤ 0.15), which is ascribed to the increasing of the number of oxygen ion vacancies and the increase in the unit cell volume. However, the conductivity decreases when the Bi content is further increased (0.15 <  x  ≤ 0.2), which is ascribed the reduction of the number of free oxygen vacancies. The highest conductivity at 800 °C is 5.6 × 10 −2  S/cm and the activation energy is 0.83 eV for Ce 0.65 Sm 0.2 Bi 0.15 O 1.825 , indicating that this would be a promising electrolyte for the intermediate temperature-solid oxide fuel cell applications.

研究领域: 材料科学 · 无机非金属材料 · 固态离子学 · 能源材料 · 燃料电池
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JOURNAL OF SUPERCRITICAL FLUIDS · 2022 · IF 4.514

Erosion-corrosion behavior of Nickel based alloys in supercritical water oxidation environment

Jianqiao Yang,Shuzhong Wang,Jiahuan Wang,Jinlong Wang,Baoquan Zhang,Lu Liu,Wei Liu,Yanhui Li,Donghai Xu

In this study, the erosion-corrosion experiment of Ni based alloys in high-temperature and high-pressure supercritical water environment was performed. SiO 2 and Al 2 O 3 particles with the average diameter of 30 µm and 50 µm were used as erodent. The special designed specimens were fixed on a blade impeller , and the erosion tests were performed in a high pressure autoclave with a magnetic stirrer system. Results show that the basic corrosion mechanism is not changed by the erosion process. A Cr-rich inner oxide layer and a Fe/Ni rich outer oxide layer were formed on the alloy surface. However, the oxidation rates of the alloys were affected by the erosion process. Parts of the outer Fe and Ni oxides were removed by the erodent particles during the tests. The inner Cr oxide layer still exists owing to the self-healing ability of the Cr 2 O 3 layer, acting as a barrier to resist further corrosion of the alloys. The factors that affect the degree of erosion and the erosion-corrosion mechanism in SCW environment is analyzed.

研究领域: 材料科学 · 腐蚀科学 · 高温高压环境材料行为 · 表面工程 · 能源材料
✓ 已验证 DOI 高影响因子
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2015 · IF 2.587

Zinc Oxide Supported trans-CoD(p-Cl)PPCl-Type Metalloporphyrins Catalyst for Cyclohexane Oxidation to Cyclohexanol and Cyclohexanone with High Yield

Yujia Xie,Fengyong Zhang,Pingle Liu,Fang Hao,Hean Luo

Direct functionalization of saturated C–H bonds by metalloporphyrin catalysts is among the topical and challenging areas within the chemical industry and synthetic chemistry. In this work, supported CoD(p-Cl)PPCl metalloporphyrin catalysts were prepared and characterized. It has been found that the CoD(p-Cl)PPCl/ZnO catalyst shows better catalytic activity than the supported catalyst (ZrO2, MCM-41, kaolin, Zr(OH)2, and boehmite (BM)) in cyclohexane oxidation with dioxygen. The effects of the reaction pressure, reaction temperature, and reaction time on the catalytic activity were considered by the supported CoD(p-Cl)PPCl/ZnO catalyst. The CoD(p-Cl)PPCl/ZnO catalyst can be facilely recovered and was recycled up to seven times without a significant decrease in catalytic performance. The average cyclohexane conversion and selectivity to KA oil are 10.98% and 84.34%, respectively, and the turnover number is 2.10 × 107.

研究领域: 催化化学 · 有机合成 · 工业化学 · 材料化学 · 绿色化学
✓ 已验证 DOI 高影响因子
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APPLIED SURFACE SCIENCE · 2013 · IF 2.112

Synthesis of novel nanocomposite Fe3O4/ZrO2/chitosan and its application for removal of nitrate and phosphate

Hualin Jiang,Pinghua Chen,Shenglian Luo,Xinman Tu,Qun Cao,Meng Shu

A novel nanocomposite with a BET surface area of 212.9   m 2 /g was synthesized from chitosan and Fe 3 O 4 /ZrO 2 using an inexpensive protocol at mild condition. The Fe 3 O 4 /ZrO 2 /chitosan composite has the ability to adsorb both nitrate and phosphate. The maximum adsorption amount of nitrate and phosphate is 89.3   mg/g and 26.5   mg   P/g, respectively. The adsorption process fits well to the pseudo-first-order kinetic rate model, and the mechanism involves simultaneous adsorption and intra-particle diffusion. The experimental results suggest that the composite is a promising adsorbent for treating water that is contaminated with nutrients.

研究领域: 环境科学 · 材料科学 · 水处理 · 纳米技术 · 环境污染控制
✓ 已验证 DOI 高影响因子
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JOURNAL OF RARE EARTHS · 2020 · IF 3.104

A novel study of sulfur-absorption via samarium-doped cerium sorbent at high temperature

Xuechao Hu,Junhui Dong

Sulfides existing in many gas mixtures of high temperature cases have a negative effect on various industrial applications. In this study, we present samarium-doped cerium (SDC) sorbent to remove H 2 S at high temperature. Compared with pure CeO 2 , the SDC sorbent shows excellent ability in sulfur removal because of the positive effect of the doping of Sm. The H 2 has a negative influence on sulfidation of the SDC sorbent and significantly shortens the breakthrough time, hence breakthrough sulfur capacity (BSC). The carbon monoxide present in the feed gas has no obvious effect on the sulfur-removal performance. A suitable samarium loading in SDC leads to an optimum interaction between metal oxide species and the surface oxygen vacancies , which results in an optimal adsorbed activity of reduced gas (H 2 , H 2 S) and hence desulphurization performance. In addition, the SDC sorbents have a good regenerated ability by a simple calcination process.

研究领域: 材料科学 · 环境化学 · 能源工程 · 无机化学 · 催化化学
✓ 已验证 DOI 高影响因子
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ELECTROCHIMICA ACTA · 2014 · IF 4.086

Electrolysis of solid copper oxide to copper in Choline chloride-EG eutectic melt

Qibo Zhang,Rui Wang,Konghao Chen,Yixin Hua

Electrochemical deoxygenation of porous CuO pellet to prepare copper was investigated in the 33.3-66.7 mol% Choline chloride (ChCl)-EG eutectic melt at 353   K. Cyclic voltammetry of the Pt-powder cavity microelectrode loaded with CuO powder exhibited that the solid CuO can be electrochemically reduced in solid state in the eutectic melt. Constant-voltage (2.0 to 2.4   V) electrolysis, with an assembled cathode of a sintered porous CuO pellet and a graphite anode, that performed in the eutectic melt demonstrated the conversion process of oxide-to metal as confirmed by scanning electron microscopy, energy-dispersive X-ray, and X-ray diffraction spectra. A mechanism for this reduction process has been proposed on the basis of the in situ formation of numerous gas at the cathode, emphasizing that the oxidation of cathodically generated O 2− ions occurred nearby along with the copper electroreduction , in which the new formed metal was served as a temporary anode, oxygen was generated at the interface of the reduced copper and electrolyte inside the cathode.

研究领域: 电化学 · 材料科学 · 冶金工程 · 无机化学 · 能源材料
✓ 已验证 DOI 高影响因子
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WATER AIR AND SOIL POLLUTION · 2019 ·Vol. 230 ·期 2 ·41 · IF 1.774

Formation of Multiple Nitrosamines from the Ozonation of Corresponding Precursor Secondary Amines: Influencing Factors and Transformation Mechanisms

Wang Wanfeng,Liang Fang,Guo Yanling,Wu Ruijie,Pan Feng,Jin Caixia,Wang Jun

Since nitrosamine disinfection by products is highly carcinogenic, they have attracted considerable attention due to their increased presence in ambient waterways and potable water supplies. For the present study, the potential formation of nitrosamines from corresponding precursor secondary amines during ozonation was investigated. The results revealed that five nitrosamines were observed during the ozonation of their corresponding secondary amines. The molar yields initially increased and then decreased with longer contact times and higher ozone doses. These phenomena indicated that ozone not only promoted nitrosamine formation but also degraded the formed nitrosamines. High pH had a positive influence on nitrosamine formation at room temperature. Further, coexisting substances including nitrate, nitrite, humic acid, and tert-butanol inhibited the generation of nitrosamines due to hydroxyl radical (·OH) competition and scavengers, whereas in the presence of hydroxylamine, nitrosamine formation increased considerably without ozone due to its capacity for independent formation between secondary amines and hydroxylamine. Further, the generation of nitrosamines from secondary amines was primarily attributed to O 3 and ·OH oxidation, which was produced through the decomposition of ozone. The transformation pathways were mainly comprised of the indirect routes between the O 3 /·OH intermediates. The findings of this study were helpful toward expanding the knowledge of nitrosamine formation during the corresponding precursor secondary amine ozonation process.

研究领域: 环境科学 · 水处理化学 · 污染物转化 · 消毒副产物 · 氧化过程
✓ 已验证 DOI 高影响因子
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Desalination and Water Treatment · 2024 · IF 1

Enhanced adsorption of tetracycline antibiotics from pharmaceutical wastewater on expanded graphite composites modified by metal oxide

Zhi Song,Yu-Long Ma,Cong-Er Li

Tetracycline (TC), a major pollutant in water, has an adverse effect on ecosystem and human health. Thus, it is urgent to remove but still remains a challenging. In this work, a new adsorbent of MnO 2 decorated on sodium hypochlorite treated expanded graphite (MnO 2 /TEG) was developed by an in situ hydrothermal method, which exhibited a highly removal rate of 99.2% to pharmaceutical wastewater treated by flocculation. The structure and morphology of the adsorbent was studied by detailed physical characterization. Meanwhile, the main influencing factors on the adsorption behavior such as pH value, concentration, temperature of the solution, adsorption time, metal oxide species and MnO 2 loading amount were also investigated in detail. It was found that the electrostatic adsorption between Mn 4+ in MnO 2 /TEG and dimethylamino groups in TC molecules played an important role during the adsorption process. These excellent properties proved that the novel composite could be applied to remove TC residues in pharmaceutical wastewater.

研究领域: 环境科学 · 水处理技术 · 材料科学 · 环境污染与控制 · 药物残留去除
✓ 已验证 DOI 高影响因子
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY · 2023 · IF 7.2

RuOx modified PrBaFe1.8Hf0.2O5+δ surface for boosting the performance of symmetrical solid oxide fuel cells

Xingxing Li,Yan Zhu,Nan Zhang,Yansheng Gong,Rui Wang,Huanwen Wang,Jun Jin,Ling Zhao,Beibei He

The development of symmetrical solid oxide fuel cells (SSOFCs) faces a significant challenge in designing electrode materials that exhibit both high activity and stability. In this work, a novel layered perovskite oxide symmetric electrode material PrBaFe 1.8 Hf 0.2 O 5+δ (PBFH) for SSOFCs is proposed and synthesized. Doping Hf at the B-site of PrBaFe 2 O 5+δ (PBF) improves the stability in reducing atmosphere and increases the concentration of oxygen vacancies . Furthermore, a small amount of RuO x is deposited by atomic layer deposition (ALD) onto PrBaFe 1.8 Hf 0.2 O 5+δ scaffold as symmetric electrodes. The surface modification of ALD-RuO x significantly boosts the catalytic activity for both fuel oxidation and oxygen reduction, simultaneously. Compared to PBF electrodes, the interfacial polarization resistances of RuO x -PBFH decrease to 0.77 Ω cm 2 under H 2 /Ar and 0.021 Ω cm 2 under air atmosphere at 800 °C, respectively. At 800 °C, SSOFCs equipped with RuO x -PBFH symmetric electrodes exhibit a high peak power density of 0.85 W cm −2 and 0.41 W cm −2 using humidified hydrogen and propane as fuels, respectively. Moreover, the RuO x -PBFH electrode demonstrates long-lasting performance, displaying high resistance against coking. These findings reveal a facile ALD approach for tailoring symmetric perovskite electrodes, offering robust and efficient electrocatalysis with efficient noble metal utilization.

研究领域: 材料科学 · 电化学 · 能源材料 · 固体离子学 · 催化化学 · 功能陶瓷
✓ 已验证 DOI 高影响因子
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Science Advances · 2022 ·Vol. 8 ·期 40 · IF 14.957

An enzyme-mimic single Fe-N3 atom catalyst for the oxidative synthesis of nitriles via C─C bond cleavage strategy

Jingzhong Qin,Bo Han,Xixi Liu,Wen Dai,Yanxin Wang,Huihui Luo,Xiaomei Lu,Jiabao Nie,Chensheng Xian,Zehui Zhang

The cleavage and functionalization of recalcitrant carbon─carbon bonds is highly challenging but represents a very powerful tool for value-added transformation of feedstock chemicals. Here, an enzyme-mimic iron single-atom catalyst (SAC) bearing iron (III) nitride (FeN 3 ) motifs was prepared and found to be robust for cleavage and cyanation of carbon–carbon bonds in secondary alcohols and ketones. High nitrile yields are obtained with a wide variety of functional groups. The prepared FeN 3 -SAC exhibits high enzyme-like activity and is capable of generating a dioxygen-to-superoxide radical at room temperature, while the commonly reported FeN 4 -SAC bearing FeN 4 motifs was inactive. Density functional theory (DFT) calculation reveals that the activation energy of dioxygen activation and the activation energy of the rate-determining step of nitrile formation are lower over FeN 3 -SAC than FeN 4 -SAC. In addition, DFT calculation also explains the catalyst’s high selectivity for nitriles.

研究领域: 催化化学 · 有机化学 · 材料科学 · 理论化学 · 可持续化学
✓ 已验证 DOI 高影响因子
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