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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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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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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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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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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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Effects of Pd doping on N

Mingxin Dong, Jun Wang, Jinxin Zhu, Jianqiang Wang, Wulin Wang, Meiqing Shen

《环境科学与工程前沿（英文）》 2017年 第11卷 第6期 doi: 10.1007/s11783-017-0976-9

摘要： N O is a powerful greenhouse gas and plays an important role in destructing the ozone layer. This present work investigated the effects of Pd doping on N O formation over Pt/BaO/Al O catalyst. Three types of catalysts, Pt/BaO/Al O , Pt/Pd mechanical mixing catalyst (Pt/BaO/Al O +Pd/Al O ) and Pt-Pd co-impregnation catalyst (Pt-Pd/BaO/Al O ) were prepared by incipient wetness impregnation method. These catalysts were first evaluated in NSR activity tests using H /CO as reductants and then carefully characterized by BET, CO chemisorption, CO-DRIFTs and H -TPR techniques. In addition, temperature programmed reactions of NO with H /CO were conducted to obtain further information about N O formation mechanism. Compared with Pt/BaO/Al O , (Pt/BaO/Al O +Pd/Al O ) produced less N O and more NH during NO storage and reduction process, while an opposite trend was found over (Pt-Pd/BaO/Al O +Al O ). Temperature programmed reactions of NO with H /CO results showed that Pd/Al O component in (Pt/BaO/Al O +Pd/Al O ) played an important role in NO reduction to NH , and the formed NH could reduce NO to N leading to a decrease in N O formation. Most of N O formed over (Pt-Pd/BaO/Al O +Al O ) was originated from Pd/BaO/Al O component. H -TPR results indicated Pd-Ba interaction resulted in more difficult-to-reduce PdO species over Pd/BaO/Al O , which inhibits the NO dissociation and thus drives the selectivity to N O in NO reduction.

关键词： NOx storage reduction     Pt/BaO/Al2O3     Pd doping     N2O formation     Optimization    

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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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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H<sub>2sub>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H<sub>2sub>有效利用率、90.7%的环氧丙烷（PO）本工作通过调整处理后S-1晶种中Si-OH和Bu<sub>3sub>NH+的量，定量构建了Au-O-Ti3+活性位点。Ti3+位点促进了Au和Ti3+之间的电子转移，从而增强了催化剂对O<sub>2sub>的吸附能力，有效促进H<sub>2sub>O<sub>2sub本工作所报道的结果为强化丙烯直接气相环氧化反应的H<sub>2sub>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     H<sub>2sub>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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Simultaneous removal of NO and chlorobenzene on VO/TiO granular catalyst: Kinetic study and performance

《环境科学与工程前沿（英文）》 2021年 第15卷 第4期 doi: 10.1007/s11783-020-1363-5

摘要：

• A V2O5/TiO2 granular catalyst for simultaneous removal of NO and chlorobenzene.

关键词： NOx     Chlorobenzene     Simultaneous removal     Kinetic study     Performance prediction     V2O5/TiO2     Graphical abstract    

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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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grown TiN/N-TiO composite for enhanced photocatalytic H evolution activity

《能源前沿（英文）》 2021年 第15卷 第3期   页码 721-731 doi: 10.1007/s11708-021-0766-8

摘要： Titanium nitride (TiN) decorated N-doped titania (N-TiO2) composite (TiN/N-TiO2) is fabricated via an in situ nitridation using a hydrothermally synthesized TiO2 and melamine (MA) as raw materials. After the optimization of the reaction condition, the resultant TiN/N-TiO2 composite delivers a hydrogen evolution activity of up to 703 μmol/h under the full spectrum irradiation of Xe-lamp, which is approximately 2.6 and 32.0 times more than that of TiO2 and TiN alone, respectively. To explore the underlying photocatalytic mechanism, the crystal phase, morphology, light absorption, energy band structure, element composition, and electrochemical behavior of the composite material are characterized and analyzed. The results indicate that the superior activity is mainly caused by the in situ formation of plasmonic TiN and N-TiO2 with intimate interface contact, which not only extends the spectral response range, but also accelerates the transfer and separation of the photoexcited hot charge carrier of TiN. The present study provides a fascinating approach to in situ forming nonmetallic plasmonic material/N-doped TiO2 composite photocatalysts for high-efficiency water splitting.

关键词： photocatalytic H2 evolution     TiN/N-TiO2 composite     plasmonic effect     in-situ nitridation    

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Fabrication and photocatalytic ability of an Au/TiO<sub>2sub>

Fenghe Lv, Hua Wang, Zhangliang Li, Qi Zhang, Xuan Liu, Yan Su

《环境科学与工程前沿（英文）》 2018年 第12卷 第1期 doi: 10.1007/s11783-017-0977-8

摘要： A new type of Au/TiO /reduced graphene oxide (RGO) nanocomposite was fabricated by the hydrothermal synthesis of TiO on graphene oxide followed by the photodeposition of Au nanoparticles. Transmission electron microscopy images showed that Au nanoparticles were loaded onto the surface of both TiO and RGO. Au/TiO /RGO had a better photocatalytic activity than Au/TiO for the degradation of phenol. Electrochemical measurements indicated that Au/TiO /RGO had an improved charge transfer capability. Meanwhile, chemiluminescent analysis and electron spin resonance spectroscopy revealed that Au/TiO /RGO displayed high production of hydrogen peroxide and hydroxyl radicals in the photocatalytic process. This high photocatalytic performance was achieved via the addition of RGO in Au/TiO /RGO, where RGO served not only as a catalyst support to provide more sites for the deposition of Au nanoparticles but also as a collector to accept electrons from TiO to effectively reduce photogenerated charge recombination.

关键词： Reduced graphene oxide     Au     TiO2     Nanocomposite     Photocatalysis    

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A study on the catalytic performance of Pd/γ-Al

Ruizhi CHU, Xianyong WEI, Zhimin ZONG, Wenjia ZHAO

《化学科学与工程前沿（英文）》 2010年 第4卷 第4期   页码 452-456 doi: 10.1007/s11705-010-0522-9

摘要： A series of Pd/γ-Al O hybrid catalysts were prepared by impregnation and subsequent calcination under microwave irradiation. The catalysts were used for direct synthesis of dimethylether (DME) from syngas. The results show that calcination under microwave irradiation improved both the activity and selectivity of the catalysts for DME synthesis. The optimum power of the microwave was determined to be 420 W. Under such optimum conditions, CO conversion, DME selectivity and time space yield of DME were 60.1%, 67.0%, and 21.5 mmol·mL ·h , respectively. Based on various characterizations such as nitrogen physisorption, X-ray diffraction, CO-temperature-programmed desorption, and Fourier transform infrared spectral analysis, the promotional effect of the microwave irradiation on the catalytic property was mainly attributed to both the higher dispersion of Pd and the significant increase in the adsorption on the CO-bridge of Pd. Microwave irradiation with very high power led to the increase in CO-bridge adsorption and thereby decreased the catalytic activity, whereas the coverage by metallic Pd of the active sites on acidic γ-Al O significantly occurred under microwave irradiation with very low power, resulting in a decrease in the selectivity to DME.

关键词： Pd/γ-Al2O3     direct synthesis     dimethyl ether     calcination under microwave irradiation    

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g-CN-coated MnO hollow nanorod cathode for stable aqueous Zn-ion batteries

《化学科学与工程前沿（英文）》 2023年 第17卷 第2期   页码 217-225 doi: 10.1007/s11705-022-2214-7

摘要： Aqueous zinc-ion batteries are attracting considerable attention because of their high safety compared with conventional lithium-ion batteries. Manganese-based materials have been widely developed for zinc-ion batteries cathode owning to their low cost, high security and simple preparation. However, the severe volume expansion and poor stability during charging and discharging limit the further development of manganese-based cathodes. Herein, superior α-MnO2@g-C3N4 was successfully prepared for stable zinc-ion batteries (ZIBs) cathode by introducing g-C3N4 nanosheets. Compared with pure α-MnO2, α-MnO2@g-C3N4 has a specific capacity of 298 mAh·g–1 at 0.1 A·g–1. Even at 1 A·g–1, the α-MnO2@g-C3N4 still retains 100 mAh·g–1 (83.4% retention after 5000 cycles), implying its excellent cycling stability. The α-MnO2@g-C3N4-based cathode has the highest energy density (563 Wh·kg–1) and power energy density (2170 W·kg–1). This work provides new avenues for the development of a wider range of cathode materials for ZIBs.

关键词： α-MnO2 hollow nanorods     g-C3N4     heterojunction     aqueous Zn-ion batteries    

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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

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

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

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

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

期刊论文

Effects of Pd doping on N

Mingxin Dong, Jun Wang, Jinxin Zhu, Jianqiang Wang, Wulin Wang, Meiqing Shen

期刊论文

An electrochemical process that uses an Fe

Chaojie Jiang, Lifen Liu, John C. Crittenden

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

Simultaneous removal of NO and chlorobenzene on VO/TiO granular catalyst: Kinetic study and performance

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

grown TiN/N-TiO composite for enhanced photocatalytic H evolution activity

期刊论文

Fabrication and photocatalytic ability of an Au/TiO<sub>2sub>

Fenghe Lv, Hua Wang, Zhangliang Li, Qi Zhang, Xuan Liu, Yan Su

期刊论文

A study on the catalytic performance of Pd/γ-Al

Ruizhi CHU, Xianyong WEI, Zhimin ZONG, Wenjia ZHAO

期刊论文

g-CN-coated MnO hollow nanorod cathode for stable aqueous Zn-ion batteries

期刊论文