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Efficient dechlorination of 2,4-dichlorophenol in an aqueous media with a mild pH using a Pd/TiO

Jiangkun DU,Jianguo BAO,Wei HU

《环境科学与工程前沿（英文）》 2015年 第9卷 第5期   页码 919-928 doi: 10.1007/s11783-015-0794-x

摘要： In this study, palladium-loaded titania nanotubes was fabricated on a titanium plate (Pd/TiO NTs/Ti) for efficient electrodechlorination of 2,4-chlorophenol with a mild pH condition. The nature of Pd/TiO NTs/Ti electrodes was characterized by field-emission scanning electron microscope (FESEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and cyclic voltammetry (CV) techniques. The characterization results indicated the generation of Pd nanoparticles which were evenly dispersed on titania nanotubes arrays on the Pd/TiO NTs/Ti surface. An effective degradation efficiency of up to 91% was achieved within 60 min at cathode potential of −0.7 V ( SCE) and initial pH of 5.5. The effects of the applied cathode potential and initial pH on the degradation efficiency were studied. A near neutral condition was more favorable since very low and very high pHs were not conducive to the dechlorination process. Furthermore, the intermediates analysis showed that the Pd/TiO NTs/Ti electrode could completely remove chlorine from 2, 4-dichlorophenol since only phenol was detected as the byproduct and the concentration of released chlorine ions indicated near-complete dechlorination. This work presents a good alternative technique for eliminating persistent chlorophenols in polluted wastewater without maintaining strong acidic environment.

关键词： Pd/TiO2NTs/Ti cathode     chlorophenols     electrocatalytic dechlorination     wastewater treatment    

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Effective regeneration of thermally deactivated commercial V-W-Ti catalysts

Xuesong SHANG, Jianrong LI, Xiaowei YU, Jinsheng CHEN, Chi HE

《化学科学与工程前沿（英文）》 2012年 第6卷 第1期   页码 38-46 doi: 10.1007/s11705-011-1167-z

摘要： An effective method for the regeneration of thermally deactivated commercial monolith SCR catalysts was investigated. Two types of regenerated solutions, namely NH Cl (1 mol/L) and dilute H SO (0.5 mol/L), were employed to treat the used catalyst. The effects of temperature and the regeneration process on the structural and textural properties of the catalysts were determined by X-ray diffraction, scanning electron microscopy, N adsorption/desorption, elemental analysis and Fourier transform infrared spectroscopy. The results suggest that the anatase phase of the used catalyst is maintained after exposure to high temperatures. Some of the catalytic activity was restored after regeneration. The catalyst regenerated by aqueous NH Cl had a higher activity than that of the catalyst treated by dilute H SO . The main reason is that the NH generated from the decomposition of NH Cl at high temperatures can be adsorbed onto the catalyst which promotes the reaction. The aggregated V O were partially re-dispersed during the regeneration process, and the intrinsic oxidation of ammonia with high concentrations of O is a factor that suppresses the catalytic activity.

关键词： V2O5-WO3/TiO2 catalysts     thermal deactivation     regeneration     NH4Cl     dilute H2SO4 solution    

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An electrochemical process that uses an Fe

Chaojie Jiang, Lifen Liu, John C. Crittenden

《环境科学与工程前沿（英文）》 2016年 第10卷 第4期 doi: 10.1007/s11783-016-0860-z

摘要： A bio-electrochemical fuel cell reactor with cathodic Fe /TiO generates electricity. It destroys recalcitrant pollutants in cathode chamber without photocatalysis. Fe /TiO generates reactive oxygenated species in the dark or under photocatalysis. Cathodic produced ROS (hydroxy radical/superoxide radical) can degrade tetracycline or dyes. Electricity generation is enhanced by semiconductor catalyzed cathodic degradation of pollutants. In this study, a new water treatment system that couples (photo-) electrochemical catalysis (PEC or EC) in a microbial fuel cell (MFC) was configured using a stainless-steel (SS) cathode coated with Fe /TiO . We examined the destruction of methylene blue (MB) and tetracycline. Fe /TiO was prepared using a chemical reduction-deposition method and coated onto an SS wire mesh (500 mesh) using a sol technique. The anode generates electricity using microbes (bio-anode). Connected via wire and ohmic resistance, the system requires a short reaction time and operates at a low cost by effectively removing 94% MB (initial concentration 20 mg·L ) and 83% TOC/TOC under visible light illumination (50 W; 1.99 mW·cm for 120 min, MFC-PEC). The removal was similar even without light irradiation (MFC-EC). The of the MFC-PEC system was approximately 0.675 kWh·m ·order , whereas that of the MFC-EC system was zero. The system was able to remove 70% COD in tetracycline solution (initial tetracycline concentration 100 mg·L ) after 120 min of visible light illumination; without light, the removal was 15% lower. The destruction of MB and tetracycline in both traditional photocatalysis and photoelectrocatalysis systems was notably low. The electron spin-resonance spectroscopy (ESR) study demonstrated that ·OH was formed under visible light, and ·O was formed without light. The bio-electricity-activated O and ROS (reactive oxidizing species) generation by Fe /TiO effectively degraded the pollutants. This cathodic degradation improved the electricity generation by accepting and consuming more electrons from the bio-anode.

关键词： Bio-anode     Photocatalytic cathode     Fe0/TiO2     ESR     Dye and antibiotics     Advanced oxidation    

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Facile synthesis and enhanced visible-light photocatalytic activity of Ti

Xiaojie Zhang,Lei Wang,Shuqing Chen,Yi Huang,Zhuonan Song,Miao Yu

《化学科学与工程前沿（英文）》 2015年 第9卷 第3期   页码 349-358 doi: 10.1007/s11705-015-1523-5

摘要： Ti -doped TiO nanosheets with tunable phase composition (doped TiO (A/R)) were synthesized via a hydrothermal method with high surface area anatase TiO nanosheets TiO (A) as a substrate, structure directing agent, and inhibitor; the activity was evaluated using a probe reaction-photocatalytic CO conversion to methane under visible light irradiation with H as an electron donor and hydrogen source. High-resolution transmission electron microscope (HRTEM), field emission scanning electron microscope, UV-Vis diffuse reflectance spectra, and X-ray diffraction (XRD) etc., were used to characterize the photocatalysts. XRD and HRTEM measurements confirmed the existence of anatase-rutile phase junction, while Ti and single-electron-trapped oxygen vacancy in the doped TiO (A/R) photocatalyst were revealed byelectron paramagnetic resonance (EPR) measurements. Effects of hydrothermal synthesis temperature and the amount of added anatase TiO on the photocatalytic activity were elucidated. Significantly enhanced photocatalytic activity of doped TiO (A/R) was observed; under the optimized synthesis conditions, CH generation rate of doped TiO (A/R) was 2.3 times that of Ti -doped rutile TiO .

关键词： Ti3+-doped TiO2     photocatalytic CO2 conversion     visible light irradiation    

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Synthesis, physicochemical characterizations and catalytic performance of Pd/carbon-zeolite and Pd/carbon-CeO

Zeinab JAMALZADEH, Mohammad HAGHIGHI, Nazli ASGARI

《环境科学与工程前沿（英文）》 2013年 第7卷 第3期   页码 365-381 doi: 10.1007/s11783-013-0520-5

摘要： In this work, xylene removal from waste gas streams was investigated via catalytic oxidation over Pd/carbon-zeolite and Pd/carbon-CeO nanocatalysts. Activated carbon was obtained from pine cone chemically activated using ZnCl and modified by H PO . Natural zeolite of clinoptilolite was modified by acid treatment with HCl, while nano-ceria was synthesized via redox method. Mixed supports of carbon-zeolite and carbon-ceria were prepared and palladium was dispersed over them via impregnation method. The prepared samples were characterized by X-ray diffraction (XRD), field emission scanning electron microscopy (FESEM), Brunauer-Emmett-Teller surface area (BET), Fourier transform infrared spectroscopy (FTIR) and thermogravimetric (TG) techniques. Characterization of nanocatalysts revealed a good morphology with an average particle size in a nano range, and confirmed the formation of nano-ceria with an average crystallite size below 60 nm. BET analysis indicated a considerable surface area for catalysts (~1000 m ·g ). FTIR patterns demonstrated that the surface groups of synthesized catalysts are in good agreement with the patterns of materials applied in catalyst synthesis. The performance of catalysts was assessed in a low-pressure catalytic oxidation pilot in the temperature range of 100°C–250°C. According to the reaction data, the synthesized catalysts have been shown to be so advantageous in the removal of volatile organic compounds (VOCs), representing high catalytic performance of 98% for the abatement of xylene at 250°C. Furthermore, a reaction network is proposed for catalytic oxidation of xylene over nanocatalysts.

关键词： Pd/carbon-CeO2     Pd/carbon-zeolite     pine cone     ZnCl2     catalytic oxidation     xylene    

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Effect of TiO 2 loading on the activity of V/TiO 2 -Al 2 O 3 in the catalytic oxidehydrogenation of ethylbenzene

Xiaohong LI, Wenying LI,

《化学科学与工程前沿（英文）》 2010年 第4卷 第2期   页码 142-146 doi: 10.1007/s11705-009-0233-2

摘要： TiO-AlOmixed oxides with different compositions ranging from 40wt-% to 95wt-% of TiO were prepared by sol-gel method and impregnated with different amounts of VO. Supports and catalysts were characterized by X-ray diffraction (XRD), physisorption, temperature preprogrammed reduction (H-TPR), and ammonia temperature programmed desorption (NH-TPD). TiO content in the support had obvious effect on the crystal structure, texture characteristic, acid property, and catalytic activity in dehydrogenation of ethylbenzene (EB) with carbon dioxide. The highest catalytic activity was acquired when the TiO content was 50 wt-%.

关键词： desorption     different     TiO-AlOmixed     physisorption     ethylbenzene    

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A comparison of the catalytic hydrogenation of 2-amylanthraquinone and 2-ethylanthraquinone over a Pd

Enxian Yuan, Xiangwei Ren, Li Wang, Wentao Zhao

《化学科学与工程前沿（英文）》 2017年 第11卷 第2期   页码 177-184 doi: 10.1007/s11705-016-1604-0

摘要： The hydrogenation of 2-ethylanthraquinone (eAQ), 2- -amylanthraquinone (taAQ) and their mixtures with molar ratios of 1:1 and 1:2 to the corresponding hydroquinones (eAQH and taAQH ) were studied over a Pd/Al O catalyst in a semi-batch slurry reactor at 60 °C and at 0.3 MPa. Compared to eAQ, TaAQ exhibited a significantly slower hydrogenation rate (about half) but had a higher maximum yield of H O and a smaller amount of degradation products. This can be ascribed to the longer and branched side chain in taAQ, which limits its accessibility to the Pd surface and its diffusion through the pores of the catalyst. Density functional theory calculations showed that it is more difficult for taAQ to adsorb onto a Pd (111) surface than for eAQ. The hydrogenation of the eAQ/taAQ mixtures had the slowest rates, lowest H O yields and the highest amounts of degradation products.

关键词： hydrogenation     hydrogen peroxide     anthraquinone     Pd catalyst     AO process    

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Interfacial charge transfer and photocatalytic activity in a reverse designed BiO/TiO core-shell

《能源前沿（英文）》 2021年 第15卷 第3期   页码 732-743 doi: 10.1007/s11708-021-0772-x

摘要： In this study, the electronic and photocatalytic properties of core-shell heterojunctions photocatalysts with reversible configuration of TiO2 and Bi2O3 layers were studied. The core-shell nanostructure, obtained by efficient control of the sol-gel polymerization and impregnation method of variable precursors of semiconductors, makes it possible to study selectively the role of the interfacial charge transfer in each configuration. The morphological, optical, and chemical composition of the core-shell nanostructures were characterized by high-resolution transmission electron microscopy, UV-visible spectroscopy and X-ray photoelectron spectroscopy. The results show the formation of homogenous TiO2 anatase and Bi2O3 layers with a thickness of around 10 and 8 nm, respectively. The interfacial charge carrier dynamic was tracked using time resolved microwave conductivity and transition photocurrent density. The charge transfer, their density, and lifetime were found to rely on the layout layers in the core-shell nanostructure. In optimal core-shell design, Bi2O3 collects holes from TiO2, leaving electrons free to react and increase by 5 times the photocatalytic efficiency toward H2 generation. This study provides new insight into the importance of the design and elaboration of optimal heterojunction based on the photocatalyst system to improve the photocatalytic activity.

关键词： photocatalysis     core-shell     heterojunction     H2     TiO2     Bi2O3    

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配位不饱和Au-O-Ti3+活性位点的构建及其在低温丙烯气相环氧化反应中强化氢气效率的研究 Article

宋钊宁, 闫昊, 袁俊聪, 马宏飞, 曹建琳, 王永祥, 王强, 彭冲, 邓风, 冯翔, 陈德, 杨朝合, 胡永康

《工程（英文）》 2023年 第25卷 第6期   页码 144-156 doi: 10.1016/j.eng.2023.01.008

摘要：

自1998年以来，人们广泛认为Au/Ti基催化剂的Au-O-Ti4+位点是在相对高温条件下丙烯气相环氧化反应的活性位点，但该类催化剂的H2有效利用率普遍较低值得注意的是，该活性位点主导反应时，最佳温度可从200 °C显著降低至138 °C，并使催化剂保持前所未有的43.6%的H2有效利用率、90.7%的环氧丙烷（PO）并且利用原位紫外-可见光谱（operando UV-vis）技术研究了Ti-OOH反应中间体的动态演化过程，结果表明，在Au-O-Ti3+活性位点上的Ti-OOH的生成速率比在Au-O-TiTi3+位点促进了Au和Ti3+之间的电子转移，从而增强了催化剂对O2的吸附能力，有效促进H2O22有效利用率提供了新的思路，而且为低温下丙烯直接气相环氧化反应的工业化推进开辟了新的机会。

关键词： 丙烯环氧化     H2有效利用率     Au/Ti双功能催化剂     配位不饱和Ti位点     密度泛函理论    

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Solar photocatalytic decomposition of two azo dyes on multi-walled carbon nanotubes (MWCNTs)/TiO 2 composites

Huilong WANG, Shuqin LIU, Hui WANG, Wenfeng JIANG,

《环境科学与工程前沿（英文）》 2010年 第4卷 第3期   页码 311-320 doi: 10.1007/s11783-010-0237-7

摘要： Multi-walled carbon nanotubes (MWCNTs)/TiO composite photocatalysts with high photoactivity were prepared by sol-gel process and further characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), Fourier transform infrared (FT-IR), and UV-vis absorption spectra. Compared to pure TiO, the combination of MWCNTs with titania could cause a significant absorption shift toward the visible region. The photocatalytic performances of the MWCNTs/TiO composite catalysts were evaluated for the decomposition of Reactive light yellow K-6G (K-6G) and Mordant black 7 (MB 7) azo dyes solution under solar light irradiation. The results showed that the addition of MWCNTs enhanced the adsorption and photocatalytic activity of TiO for the degradation of azo dyes K-6G and MB 7. The effect of MWCNTs content, catalyst dosage, pH, and initial dye concentration were examined as operational parameters. The kinetics of photocatalytic degradation of two dyes was found to follow a pseudo-first-order rate law. The photocatalyst was used for seven cycles with photocatalytic degradation efficiency still higher than 98%. A plausible mechanism is also proposed and discussed on the basis of experimental results.

关键词： sol-gel     multi-walled carbon nanotubes (MWCNTs)/TiO2 composite     photocatalysis     azo dye     solar irradiation    

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Preparation and characterization of SO42-/TiO2 and S2O82-/TiO2 catalysts

MA Xuedan, GUO Daishi, JIANG Qizhong, MA Zifeng, MA Zhengfei, YE Weidong, LI Chunbo

《化学科学与工程前沿（英文）》 2007年 第1卷 第1期   页码 45-49 doi: 10.1007/s11705-007-0009-5

摘要： Nanosized solid superacids SO/TiO and SO/TiO, as well as MCM-41-supported SO/ZrO, were prepared. Their structures, acidities, and catalytic activities were investigated and compared using XRD, N adsorption-desorption, and in situ FTIR-pyridine adsorption, as well as an evaluation reaction with pseudoionone cyclization. The results showed that SO/TiO and SO/TiO possess not only nanosized particles with diameters <7.0 nm, a BET surface greater than 140 cm/g and relatively regular mesostructures with pores around 4.0 nm, but also a pure anatase phase and strong acidity. Different from the Lewis acid nature of SO/ZrO/MCM-41, SO/TiO and SO/TiO exhibit mainly Br¢nsted acidities. The strongest Br¢nsted acid sites were produced on SO/TiO promoted with HSO, while Lewis acid sites on SO/TiO even stronger than those on SO/ZrO/MCM-41 were generated when persulfate solution was used as sulfating agent. Because of their distinct acid natures, SO/TiO and SO/TiO exhibited catalytic activities for the cyclization of pseudoionone that were much higher than that of SO/ZrO/MCM-41. It can be concluded that the existence of more Br¢nsted acid sites was favorable for proton participation in the cyclization reaction.

关键词： exhibit     Different     persulfate     adsorption-desorption     catalytic    

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Plasmonic Au nanoparticles supported on both sides of TiO2 hollow spheres for maximising photocatalytic

Jianwei Lu, Lan Lan, Xiaoteng Terence Liu, Na Wang, Xiaolei Fan

《化学科学与工程前沿（英文）》 2019年 第13卷 第4期   页码 665-671 doi: 10.1007/s11705-019-1815-2

摘要： A strategy of intensifying the visible light harvesting ability of anatase TiO hollow spheres (HSs) was developed, in which both sides of TiO HSs were utilised for stabilising Au nanoparticles (NPs) through the sacrificial templating method and convex surface-induced confinement. The composite structure of single Au NP yolk-TiO shell-Au NPs, denoted as Au@Au(TiO , was rendered and confirmed by the transmission electron microscopy analysis. Au@Au(TiO showed enhanced photocatalytic activity in the degradation of methylene blue and phenol in aqueous phase under visible light surpassing that of other reference materials such as Au(TiO by 77% and Au@P25 by 52%, respectively, in phenol degradation.

关键词： TiO2 hollow spheres     plasmonic Au nanoparticles     confinement     visible light     photocatalytic degradation    

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Preparation of lignin/TiO2 nanocomposites and their application in aqueous polyurethane coatings

Dongjie Yang, Shengyu Wang, Ruisheng Zhong, Weifeng Liu, Xueqing Qiu

《化学科学与工程前沿（英文）》 2019年 第13卷 第1期   页码 59-69 doi: 10.1007/s11705-018-1712-0

摘要： A simple method using a water soluble lignin quaternary ammonium salt (LQAS) and TiO has been developed for the preparation of lignin/TiO nanocomposites in an aqueous medium under mild conditions. The LQAS/TiO nanocomposites contain well-dispersed small particles with excellent ultraviolet (UV) shielding abilities and good compatibilities with waterborne polyurethane (WPU). When the LQAS/TiO nanocomposites were blended with WPU, the UV absorbance and the tensile ductility of the WPU increased significantly. The composite WPU hybrid film containing 6 wt-% LQAS/TiO nanocomposite had the highest visible light transmittance and had excellent ultraviolet aging properties. After 192 h of UV light irradiation, the tensile strength of the composite film was above 8 MPa and the elongation at break was 800%. This work highlights new possibilities for the utilization of alkali lignin.

关键词： lignin     TiO2     nanocomposite particle     polyurethane film    

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All-inorganic TiO/CsAgBiBr composite as highly efficient photocatalyst under visible light irradiation

《化学科学与工程前沿（英文）》 2023年 第17卷 第12期   页码 1925-1936 doi: 10.1007/s11705-023-2344-6

摘要： In recent years, limited photocatalysis efficiency and wide band gap have hindered the application of TiO2 in the field of photocatalysis. A leading star in photocatalysis has been revealed as lead-free Cs2AgBiBr6 double halide perovskite nanocrystals, owing to its strong visible light absorption and tunable band gap. In this work, this photocatalytic process was facilitated by a unique TiO2/Cs2AgBiBr6 composite, which was identified as an S-cheme heterojunction. TiO2/Cs2AgBiBr6 composite was investigated for its structure and photocatalytic behavior. The results showed that when the perovskite dosage is 40%, the photocatalytic rate of TiO2 could be boosted to 0.1369 min–1. This paper discusses and proposes the band gap matching, carrier separation, and photocatalytic mechanism of TiO2/Cs2AgBiBr6 composites, which will facilitate the generation of new ideas for improving TiO2’s photocatalytic performance.

关键词： Cs2AgBiBr6 nanocrystals     visible-light photocatalyst     Cs2AgBiBr6/TiO2 heterojunction    

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Promoting effect of Zr on the catalytic combustion of methane over Pd/γ-Al

Hongbo NA,Tianle ZHU,Zhiming LIU,Yifei SUN

《环境科学与工程前沿（英文）》 2014年 第8卷 第5期   页码 659-665 doi: 10.1007/s11783-013-0613-1

摘要： The effect of Zr on the catalytic performance of Pd/γ-Al O for the methane combustion was investigated. The results show that the addition of Zr can improve the activity and stability of Pd/γ-Al O catalyst, which, based on the catalyst characterization (N adsorption, XRD, CO-Chemisorption, XPS, CH -TPR and O -TPO), is ascribed to the interaction between Pd and Zr. The active phase of methane combustion over supported palladium catalyst is the Pd /Pd mixture. Zr addition inhibits Pd aggregation and enhances the redox properties of active phase Pd / Pd . H reduction could effectively reduce the oxidation degree of Pd species and regenerate the active sites (Pd / Pd ).

关键词： Pd-Zr/Al2O3     methane     catalytic combustion     catalyst regeneration    

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标题 作者 时间 类型 操作

Efficient dechlorination of 2,4-dichlorophenol in an aqueous media with a mild pH using a Pd/TiO

Jiangkun DU,Jianguo BAO,Wei HU

期刊论文

Effective regeneration of thermally deactivated commercial V-W-Ti catalysts

Xuesong SHANG, Jianrong LI, Xiaowei YU, Jinsheng CHEN, Chi HE

期刊论文

An electrochemical process that uses an Fe

Chaojie Jiang, Lifen Liu, John C. Crittenden

期刊论文

Facile synthesis and enhanced visible-light photocatalytic activity of Ti

Xiaojie Zhang,Lei Wang,Shuqing Chen,Yi Huang,Zhuonan Song,Miao Yu

期刊论文

Synthesis, physicochemical characterizations and catalytic performance of Pd/carbon-zeolite and Pd/carbon-CeO

Zeinab JAMALZADEH, Mohammad HAGHIGHI, Nazli ASGARI

期刊论文

Effect of TiO 2 loading on the activity of V/TiO 2 -Al 2 O 3 in the catalytic oxidehydrogenation of ethylbenzene

Xiaohong LI, Wenying LI,

期刊论文

A comparison of the catalytic hydrogenation of 2-amylanthraquinone and 2-ethylanthraquinone over a Pd

Enxian Yuan, Xiangwei Ren, Li Wang, Wentao Zhao

期刊论文

Interfacial charge transfer and photocatalytic activity in a reverse designed BiO/TiO core-shell

期刊论文

配位不饱和Au-O-Ti3+活性位点的构建及其在低温丙烯气相环氧化反应中强化氢气效率的研究

宋钊宁, 闫昊, 袁俊聪, 马宏飞, 曹建琳, 王永祥, 王强, 彭冲, 邓风, 冯翔, 陈德, 杨朝合, 胡永康

期刊论文

Solar photocatalytic decomposition of two azo dyes on multi-walled carbon nanotubes (MWCNTs)/TiO 2 composites

Huilong WANG, Shuqin LIU, Hui WANG, Wenfeng JIANG,

期刊论文

Preparation and characterization of SO42-/TiO2 and S2O82-/TiO2 catalysts

MA Xuedan, GUO Daishi, JIANG Qizhong, MA Zifeng, MA Zhengfei, YE Weidong, LI Chunbo

期刊论文

Plasmonic Au nanoparticles supported on both sides of TiO2 hollow spheres for maximising photocatalytic

Jianwei Lu, Lan Lan, Xiaoteng Terence Liu, Na Wang, Xiaolei Fan

期刊论文

Preparation of lignin/TiO2 nanocomposites and their application in aqueous polyurethane coatings

Dongjie Yang, Shengyu Wang, Ruisheng Zhong, Weifeng Liu, Xueqing Qiu

期刊论文

All-inorganic TiO/CsAgBiBr composite as highly efficient photocatalyst under visible light irradiation

期刊论文

Promoting effect of Zr on the catalytic combustion of methane over Pd/γ-Al

Hongbo NA,Tianle ZHU,Zhiming LIU,Yifei SUN

期刊论文