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Journal of the Taiwan Institute of Chemical Engineers · 2019 · IF 3.834

Direct synthesis of metal-organic frameworks catalysts with tunable acid–base strength for glucose dehydration to 5-hydroxymethylfurfural

Yunlei Zhang,Bing Li,Yanan Wei,Changhao Yan,Minjia Meng,Yongsheng Yan

Developing a green and economically viable approach for the direct synthesis of metal-organic frameworks (MOFs) catalysts with multifunctional active sites remains the key step for their applications in heterogeneous catalysis field. Herein, we report a green (aqueous solutions), mild (90 °C, atmospheric pressure), and modulated hydrothermal (MHT) approach to synthesize UiO-66-type MOFs catalysts with acid–base bi-functional sites, which were obtained via the coordination of monosodium 2-sulfoterephthalate and 2-aminoterephthalic with zirconium (Zr) ions. More importantly, a series of acid, base and acid–base catalysts with varied acid–base strengths can be readily prepared, by simply varying the ratio of organic ligands for preparing MOFs. The synthesized catalysts were characterized and their performances in glucose dehydration to produce 5-hydroxymethylfurfural (5-HMF) have been evaluated. The developed approach in this work has clearly depicted a roadmap for the facile synthesis of MOFs catalysts to facilitate their potential use in acid–base catalysis.

研究领域: 化学工程 · 催化科学
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RSC Advances · 2015 ·Vol. 6 ·期 3 ·2241-2251 · IF 3.84

Synthesis of porous Al doped ZnO nanosheets with high adsorption and photodecolorizative activity and the key role of Al doping for methyl orange removal

Xiaohua Sun,Weilong Luo,Linlin Chen,Linjie Zheng,Chao Bao,Panpan Sun,Niu Huang,Yihua Sun,Liang Fang,Lei Wang

Porous Al doped ZnO (AZO) nanosheets have been prepared as an efficient multifunctional water treatment material. Their fundamental properties were characterized by various spectroscopic testing methods. The AZO nanosheets displayed very rapid adsorption rate and high adsorption capacity for methyl orange (MO) dye. The kinetics and equilibrium of adsorption process were found to follow the pseudo-second-order kinetic and Langmuir isotherm models, respectively. Furthermore, the AZO nanosheets exhibited superior photodecolorizative activity compared with the commercial P25 TiO2 nanoparticles. It was found that Al doping increased the zeta potential of AZO nanosheets and then significantly enhanced the adsorption capacity for MO dye and, at the same time, retarded the recombination of photoexcited electron–hole pairs, and prolonged the lifetime of the photo-generated carriers, and then improved the semiconductor photocatalytic activity. In addition, the visible-light-driven dye photosensitized degradation was also an important reason for enhanced photodecolorizative activity. Therefore, AZO nanosheets are a potential multifunctional water treatment material combining highly efficient adsorption and photocatalytic degradation.

研究领域: 材料科学 · 环境化学 · 纳米技术 · 光催化 · 水处理
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2015 · IF 7.435

Comparing the degradation of acetochlor to RhB using BiOBr under visible light: A significantly different rate-catalyst dose relationship

Peng Yi-Zhu,Ma Wan-Hong,Jia Man-Ke,Zhao Xiao-Rong,David M. Johnson,Huang Ying-Ping

In this study, a weakly polar pesticide acetochlor in water was tried to degrade by BiOBr catalysts under visible light irradiation. Its degradation reaction rate increased exponentially with increasing catalyst dosage, which was significantly different from conventional photocatalytic patterns established for polar or water-soluble pollutants. Thus, the rate-dosage relationship of BiOBr/acetochlor was compared to that of BiOBr/Rhodamine B (RhB) (a typical strong polar dye pollutant in water) at different BiOBr dosages. The degradation rate of RhB increased with the BiOBr dosage and then plateaued due to more catalyst particles blocking the light into the inner solution, which is a typical behavior for heterogeneous photocatalysis of polar organic compounds in aqueous solution. While acetochlor behaved differently, its degradation rate increased exponentially with the BiOBr dosage, and no plateau was observed even up to 9.0   g/L BiOBr dosage. This special rate-dose relationship for weakly polar acetochlor was correlated with a unique adsorption property of BiOBr to acetochlor in water solution. There was a re-distribution effect that always exclude excessive acetochlor adsorbed on BiOBr surface regardless either substrates or BiOBr overdose. This finally resulted in every BiOBr particle having enough adsorption sites available for dissolved dioxygen to function thereby accelerate the degradation of weakly polar organic compounds in water.

研究领域: 环境化学 · 光催化 · 水污染控制 · 环境功能材料 · 污染物降解机制
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APPLIED SURFACE SCIENCE · 2024 · IF 6.3

Hydrophilic, self-cleaning, and recyclable La-TiO2/PAN nanofibrous membranes rapidly fabricated via electro-centrifugal spinning for photocatalytic organic pollutants

Jingying Xu,Teng Hou,Jing Zhou,Hao Ye,Yaru Wang,Lvzhu Cheng,Xianglong Li,Bin Yang

Photocatalytic fibrous membranes are regarded as one of the most proficient materials for environmental remediation because of their excellent photocatalytic activity, porous structure, and outstanding recyclability. However, the poor dispersion performance of photocatalysts in the polymer matrix and the low migration ability to the surface constrain the development of this technology. In this study, a versatile strategy was developed to facilitate the design of hydrophilic nanofibrous membranes with promising photocatalytic activity and robust recyclability by combining the loaded rare earth element La 3+ modified TiO 2 photocatalyst, introducing hyperbranched polymers as dispersants within electro-centrifugal spinning, and applying post-treatment to construct hydrophilic sites. Significantly, the removal efficiency of the fibrous membrane materials on the dye wastewater was as high as 89.34 %, and the treatment efficiency can still reach 81.68 % after five cycles. In addition, the photocatalytic mechanism for the degradation of organic pollutants was also analyzed. This work provides a new method for building advanced photocatalytic nanofibrous membranes, which is expected to be used in the treatment and remediation of environmental wastewater.

研究领域: 环境科学 · 材料科学 · 纳米技术 · 化学工程 · 光催化 · 高分子材料 · 水处理技术
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JOURNAL OF MATERIALS CHEMISTRY · 2012 ·Vol. 22 ·期 15 ·7291-7299 · IF 5.968

Efficient visible-light-driven photocatalytic hydrogen production using CdS@TaON core–shell composites coupled with graphene oxide nanosheets

Jungang Hou,Zheng Wang,Wenbin Kan,Shuqiang Jiao,Hongmin Zhu,R. V. Kumar

Large-scale hydrogen production through water splitting using photocatalysts with solar energy can potentially produce clean fuel from renewable resources. In this work, photocatalytic evolution of H2 with a high efficiency was achieved using graphene oxide (GO) nanosheets decorated with CdS sensitized TaON core–shell composites (GO–CdS@TaON). The CdS@TaON core–shell nanocomposites were prepared by an ion-exchange route with assistance from a hydrothermal process on GO as the support. The TaON core–shell composites containing 1 wt% CdS nanocrystals showed a high rate of H2-production at 306 μmol h−1 with an apparent quantum efficiency (QE) of 15% under 420 nm monochromatic light. The rate of hydrogen formation was 68 times faster in comparison with the rate observed on pure TaON. The rate was further increased to 633 μmol h−1 with a high quantum efficiency of 31% when the GO–CdS@TaON hybrid composite was coupled with 1 wt% of graphene oxide and 0.4 wt% of Pt (about 141 times higher than that of the pristine TaON). This high photocatalytic H2-production activity is ascribed firstly to the presence of CdS nanocrystals that alter the energy levels of the conduction and valence bands in the coupled semiconductor system; secondly to the involvement of graphene oxide that serves as an electron collector and transporter to efficiently lengthen the lifetime of the photogenerated charge carriers from CdS@TaON composites. This investigation can open up new possibilities for the development of highly efficient TaON-based photocatalysts that utilize visible light as an energy source.

研究领域: 材料化学 · 光催化 · 能源科学 · 纳米材料 · 半导体物理 · 可再生能源
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2019 · IF 14.229

In situ exsolution of silver nanoparticles on AgTaO3-SrTiO3 solid solutions as efficient plasmonic photocatalysts for water splitting

Jinxing Yu,Lei Zhang,Jun Qian,Zhirong Zhu,Shuang Ni,Gang Liu,Xiaoxiang Xu

Starting from two wide band gap semiconductors AgTaO 3 and SrTiO 3 , we managed to reduce the band gap by forming their solid solutions, i.e. (AgTaO 3 ) 1-x (SrTiO 3 ) x (0.0 ≤ x ≤ 1.0). These solid solutions all adopt cubic perovskite structure similar to SrTiO 3 and high temperature phase of AgTaO 3 , suggesting that SrTiO 3 is helpful to stabilize AgTaO 3 in its high temperature cubic phase. Substantial improvements over photocatalytic hydrogen production were realized in these solid solutions which clearly outperform their parent compounds AgTaO 3 and SrTiO 3 . In-situ exolution of silver nanoparticles at the surface of solid solutions (x = 0.2) substantially strengthen the visible light absorption due to localized surface plasmons of these silver nanoparticles . This contributes to further improvements on both photocatalytic hydrogen and oxygen production under visible light illumination (λ ≥ 400 nm). Apparent quantum efficiency as high as ˜ 2.02% and ˜ 0.11% was achieved at solid solutions (x = 0.2) decorated with silver nanoparticles for full range (λ ≥ 250 nm) and visible light (λ ≥ 400 nm) illumination respectively. Photoelectrochemical analysis suggests that solid solutions own a better charge separation conditions than their parent compounds. Furthermore, the band edge positions of solid solutions (x = 0.2) lie approximately in the middle between AgTaO 3 and SrTiO 3 , being ideal for solar water splitting reactions.

研究领域: 材料科学 · 光催化 · 能源化学 · 半导体物理 · 纳米材料
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Molecular Catalysis · 2017 · IF 0

Highly selective hydrogenation of phenol to cyclohexanol over nano silica supported Ni catalysts in aqueous medium

J. He,X.-H. Lu,Y. Shen,R. Jing,R.-F. Nie,D. Zhou,Q.-H. Xia

Cyclohexanol is an excellent starting material for fuel production, but direct selective hydrogenation of phenol to cyclohexanol under mild conditions is a challenge. Herein we report a catalyst made of Ni nanoparticles supported on high-surface silica, which is highly active for selective formation of cyclohexanol under 1.0   Mpa pressure of hydrogen in aqueous medium without additives. Conversion of 100   mol% and selectivity up to 100% are achieved within 4   h and 1.0   MPa H 2 . Some factors such as the type of the source of silica, the loading of Ni, the reaction temperature and time, the H 2 pressure play important roles in controlling the selective hydrogenation. The generality of the 10%Ni/SiO 2 -1 catalyst for this reaction is demonstrated by selective hydrogenation of other hydroxylated aromatic compounds as well.

研究领域: 催化化学 · 有机合成 · 材料化学 · 绿色化学 · 能源化学
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ELECTROCHIMICA ACTA · 2012 · IF 3.832

Electrochemical and photoelectrocatalytic properties of TaWO6 nanosheet film

Hu Qu,Bizhou Lin,Liwen He,Xiaorong Fan,Yi Zhou,Yilin Chen,Bifen Gao

TaWO 6 nanosheet was assembled into multilayer films by a layer-by-layer deposition technology with polyethylenimine as the linker. UV–vis absorption spectra in the assembly process showed a linear enhancement of absorbance at 238   nm per deposition cycle, indicating the successful formation of multilayer composite films, which were converted into polymer-free films by the heat treatment at 400   °C for 2   h. The bandgap energy and flatband potential of TaWO 6 nanosheet were estimated to be 3.48   eV and −0.79   V vs. Ag/AgCl, respectively. The photoelectrocatalytic degradation of Rhodamine B with the TaWO 6 nanosheet electrodes demonstrated that both the oxygen anionic radicals and the dye cationic radical are essential to mineralize the dye under visible-light-driven photocatalytic conditions. It is the first time to investigate the mechanism of photoelectrocatalysis of TaWO 6 nanosheet electrode.

研究领域: 材料科学 · 物理化学 · 环境催化 · 纳米科技 · 能源材料
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Energy Technology · 2018 ·Vol. 7 ·期 5 ·1800927 · IF 3.175

Bimetallic Manganese Cobalt Phosphide Nanodots–Modified Graphitic Carbon Nitride for High-Performance Hydrogen Production

Jiacong Wu,Chunmei Li,Wenli Zhang,Juan Han,Lei Wang,Shuhao Wang,Yun Wang

It is a huge challenge for exploiting new photocatalysts with low-cost cocatalysts in place of precious metals to realize high-efficiency H 2 production from water. Herein, a new photocatalyst with a high H 2 production activity is prepared via modification of bimetallic manganese cobalt phosphide (Mn 0.67 Co 1.33 P) nanodots on graphitic carbon nitride (g-C 3 N 4 ). Moreover, the largest H 2 production rate of 113.1 μmol h −1 is obtained over the Mn 0.67 Co 1.33 P/g-C 3 N 4 -5 sample, which is about 2.75 times than that of Pt/g-C 3 N 4 -5 (41.2 μmol h −1 ). The high-performance H 2 production suggests page a page down that the modification effect of Mn 0.67 Co 1.33 P nanodots improves the visible harvest ability and separation efficiency of charge carriers. A typical example to improve the photocatalytic H 2 production performance by fabricating heterostructures using bimetallic phosphide to modify graphitic carbon nitride is provided.

研究领域: 材料科学 · 光催化 · 能源化学 · 纳米材料 · 可持续能源
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS · 2020 ·Vol. 31 ·期 11 ·8403-8412 · IF 2.22

Enhanced thermal stability and photocatalytic property of highly ordered anodized TiO2 nanotube arrays with interstitial nitrogen as dominant point defect

Wang Ting,Ma Qing,Gao Shang,Huang Mengshi

Highly regular TiO 2 nanotube arrays (TNTs) with interstitial nitrogen as the dominant point defect have been successfully prepared by annealing the as-anodized TNTs in N 2 in a temperature range of 400–650 °C. Using analysis methods that include field emission scanning electron microscopy, X-ray diffraction patterns, and Raman spectroscopy, the thermal stability of TNTs annealed in N 2 was found to be higher than that of TNTs annealed in O 2 . The interstitial nitrogen is considered as the dominant point defect in TNTs annealed in N 2 , which results in the notably improved thermal stability of the highly ordered TNTs. However, the content of hydroxyl oxygen on the surface of TNTs is significantly influenced by annealing temperature, which is closely related to photocatalytic activity. Optimized photocatalytic property of photodegradation of MO with a pseudo-first-order reaction constant k value of (5.065 ± 0.139) × 10 –2  h −1 is achieved for TNTs annealed in N 2 at 600 °C. These findings serve to provide simple and versatile guidelines to fabricate highly ordered TNTs with controllable point defects, enhanced thermal stability, and a high level of photocatalytic activity.

研究领域: 材料科学 · 纳米科技 · 光催化 · 表面化学 · 功能材料
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MATERIALS SCIENCE IN SEMICONDUCTOR PROCESSING · 2020 · IF 3.085

Accelerating carrier separation of Ag3PO4 via synergetic effect of PANI and rGO for enhanced photocatalytic performance towards ciprofloxacin

Jiaoming Wang,Xiang Yu,Xionghui Fu,Yi Zhu,Yuanming Zhang

To solve severe photocorrosion of Ag 3 PO 4 , polyaniline for transporting holes and reduced graphene oxide (rGO) for transferring electrons were co-incorporated with Ag 3 PO 4 by an in-situ precipitation procedure and a following hydrothermal method , reaching the superior carrier separation efficiency via synergetic effect of PANI and rGO. Consequently, 5% rGO/Ag 3 PO 4 /PANI exhibited the excellent photocatalytic performance of 86.2% removal rate towards ciprofloxacin (CIP) within 15 min, which was much better than Ag 3 PO 4 , Ag 3 PO 4 /PANI and many reported photocatalysts . After four consecutive cycles, the composites performed better stability with 81.0% removal rate. Generally, photocatalytic activity depended on efficiencies of light absorption ( η abs ), charge separation ( η sep ) and charge injection ( η inj ). η sep of rGO/Ag 3 PO 4 /PANI was 11.5 and 8.70 folds higher than that of Ag 3 PO 4 and Ag 3 PO 4 /PANI, while η abs and η inj of rGO/Ag 3 PO 4 /PANI were not improved compared with Ag 3 PO 4 and Ag 3 PO 4 /PANI, strongly manifesting synergetic effect of PANI and rGO on Ag 3 PO 4 accelerated the charge separation and finally enhanced the photocatalytic activity . Besides, rGO greatly improved the adsorption efficiency for CIP and the maximum adsorption capacity was enhanced to be 19.4 mg/g which was 6.88 folds than that of Ag 3 PO 4 , being advantageous to enhancing the photocatalytic activity. The work offered an excellent reference for designing and constructing photocatalysts with superior charge separation showing excellent photocatalytic performance, which were potential candidates for degrading antibiotics in environmental treatment.

研究领域: 材料科学 · 环境化学 · 光催化 · 纳米材料 · 环境污染治理 · 半导体催化 · 抗生素降解
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APPLIED SURFACE SCIENCE · 2016 · IF 3.15

Photocatalytic hydrogen production over solid solutions between BiFeO3 and SrTiO3

Lingwei Lu,Meilin Lv,Gang Liu,Xiaoxiang Xu

Constituting solid solutions has been an appealing means to gain control over various physicochemical properties. In this work, we synthesized a series of SrTiO 3 -BiFeO 3 solid solutions and systematically explored their structural, optical and photocatalytic properties. Our results show that all solid solutions crystallize in a primitive cubic structure and their band gap values can be easily tuned by adjusting molar ratios between SrTiO 3 and BiFeO 3 . Photocatalytic hydrogen production under both full range and visible light irradiation is greatly improved after forming solid solutions. The highest hydrogen production rate obtained is ∼180   μmol/h under full range irradiation (λ   ≥   250   nm) and ∼4.2   μmol/h under visible light irradiation (λ   ≥   400   nm), corresponding to apparent quantum efficiency ∼2.28% and ∼0.10%, respectively. The activity is found to be strongly influenced by surface area and light absorption. Theoretical calculation suggests that Fe contributes to the formation of spin-polarized bands in the middle of original band gap and is responsible for the band gap reduction and visible light photocatalytic activity .

研究领域: 材料化学 · 光催化 · 能源材料 · 无机固体化学 · 半导体物理 · 太阳能转化 · 表面科学
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