Journal of Environmental Chemical Engineering
·
2022
·Vol. 10
·期 6
·108837
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IF 7.968
Yumei Jian,Ye Meng,Jie Li,Hongguo Wu,Shunmugavel Saravanamurugan,Hu Li
Photocatalytic reductive conversion of bio-derivatives to biofuels and fine chemicals is an eco-friendly and energy-saving way for biomass valorization. Herein, we developed a new and high-performance protocol for control of activity/selectivity in photocatalytic reductive upgrading of biomass to biofuels at room temperature via engineering oxygen vacancy (Ov) and manipulating the exposed crystal surfaces of the TiO 2 -based catalysts, such as efficient cascade photocatalytic hydrogenation-cyclization of ethyl levulinate to γ-valerolactone in water (up to 96% yield, TOF: 112.1 h −1 ), and the selective conversion of 5-methylfurfural to 5-methylfurfuryl alcohol (90% yield) or long carbon-chain coupling products (86% yield) in methanol, respectively. The {101} crystal plane is prone to produce more Ov in situ than the {001} and {110} crystal planes. The formation of Ov was not only beneficial to the adsorption and activation of the bio-based carbonyls, but also could enhance the migration efficiency of the photo-generated carriers and effectively adjust the semiconductor band structure of the TiO 2 -based photocatalyst to promote the visible-light absorption, thus enhancing the overall reductive conversion process, as elucidated by DFT calculations. Also, the charge distribution and adsorption intensity of different exposed crystal surfaces of the photocatalyst were able to control the selectivity of the bioproducts . In addition, the optimal Ov-TiO 2− x {101} catalyst had excellent reusability and could be reused at least five times with no obvious decrease in photocatalytic performance. The strategy of selectivity control via engineering the catalyst exposed crystal surfaces and loaded Ov provides an opportunity for multi-catalytic biomass conversion to biofuels.
研究领域:
催化化学
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材料科学
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能源化学
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环境科学
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绿色化学
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表面科学
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光催化
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2017
·
IF 6.216
Hailong Li,Weilin Zhang,Jun Wang,Zequn Yang,Liqing Li,Kaimin Shih
Simultaneous nitrogen monoxide (NO) reduction and elemental mercury (Hg 0 ) oxidation in the presence of ammonia (NH 3 ) was for the first time studied on a copper oxide/titanium dioxide (CuO/TiO 2 ) catalyst at low flue gas temperatures. More than 80% NO reduction and 90% Hg 0 oxidation were concurrently achieved on the CuO/TiO 2 catalyst at 250 °C under a simulated NH 3 selective catalytic reduction (SCR) atmosphere. NO was likely oxidized on the CuO/TiO 2 catalyst to form active nitrogenous species, particularly with the aid of oxygen. The active nitrogenous species then significantly promoted Hg 0 oxidation. NH 3 itself did not affect Hg 0 conversion on the CuO/TiO 2 catalyst. The co-occurrences of NO and NH 3 led to a reduction in oxidized mercury (HgO in this work), which partially offset the Hg 0 oxidation and therefore resulted in a relatively lower Hg 0 conversion efficiency. However, compared to flue gas without NO and NH 3 , the combined presence of NO and NH 3 still enhanced Hg 0 oxidation over the CuO/TiO 2 catalyst, primarily because of the overwhelming benefit from NO. This is superior to many other SCR catalysts, including commercial vanadia-based SCR catalysts, on which an SCR atmosphere generally inhibits Hg 0 conversion.
研究领域:
环境催化
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大气污染控制
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化学工程
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材料科学
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环境化学
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工业生态学
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能源与环境技术
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2013
·
IF 5.825
Fa-tang Li,Xiao-jing Wang,Ye Zhao,Ji-xing Liu,Ying-juan Hao,Rui-hong Liu,Di-shun Zhao
A facile and green method was developed for the simultaneous doping of nitrogen, boron, and fluorine in TiO 2 by H 2 TiO 3 via a microwave-assisted route. The ionic liquid (IL) [BMIm]BF 4 serves not only as microwave absorbent but also as a dopant. The IL also shows the ability to self-assemble under microwave irradiation, which causes it to act as an inhibitor for the growth of the TiO 2 particles. The N–B–F-tri-doped TiO 2 obtained exhibits large specific surface area, small crystal size, and a mesoporous structure, and the mechanism for the formation of the N–B–F-tri-doped TiO 2 was proposed. The prepared materials exhibit excellent visible light photocatalytic activity in the degradation of organic pollutants, including methyl orange, rhodamine B, Orange G, and reactive red X, which is attributed to the presence of a Ti–B–N structure on the TiO 2 surface, inducing a narrow band gap of 2.78 eV, and the synergistic effects of N, B, and F, which improve the separation efficiency of the photo-generated electron/hole pairs. The results obtained may provide a new sight for the application of ILs in the microwave-assisted preparation of nanomaterials.
研究领域:
材料科学
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光催化
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纳米材料
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绿色化学
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环境工程
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DOI
高影响因子
DALTON TRANSACTIONS
·
2012
·Vol. 42
·期 10
·3402-3409
·
IF 3.838
Bo Chai,Tianyou Peng,Xiaohu Zhang,Jing Mao,Kan Li,Xungao Zhang
A novel nanostructured carbon/TiO2 nanocomposite photocatalyst is firstly fabricated via a facile hydrothermal process by using fullerene (C60) decorated single-walled carbon nanotubes (SWCNTs) as carbon source, which is denoted as C60-d-CNTs. The obtained nanostructured carbon/TiO2 nanocomposites are characterized by X-ray diffraction (XRD), high-resolution transmission electron microscopy (HRTEM), UV-vis diffuse reflectance spectra (DRS), Raman spectra, X-ray photoelectron spectroscopy (XPS) and photoluminescence spectra (PL), and then are used as catalysts for photocatalytic hydrogen production. It is found that the kinds and contents of various carbon nanostructured materials (such as SWCNTs, C60 and C60-d-CNTs) coupled with TiO2 can significantly enhance the photoactivity for hydrogen production, and the 5 wt% C60-d-CNTs/TiO2 nanocomposite exhibits the best performance. Experimental results suggest that the C60-d-CNTs as a novel carbon nanostructured material could be more beneficial for the photogenerated carrier separation than SWCNTs and C60 when these carbon nanostructured materials are coupled with TiO2.
研究领域:
材料科学
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纳米技术
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光催化
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氢能
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DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2023
·
IF 6.2
Hao Xu,Jian Yang,Yang Li,Fan Fu,Kang Da,Shaobo Cao,Wenting Chen,Ximei Fan
Weak visible-light capture ability, ultrahigh charge recombination rate, and poor redox ability are crucial constraints to improve the photocatalytic performance for toluene degradation under visible-light. Hence, a dual Z-scheme of Bi 2 O 3 quantum dots decorated TiO 2 /BiOBr photocatalysts (Bi 2 O 3 QDs@TiO 2 /BiOBr) were prepared by a two-step hydrothermal method . X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and transmission electron microscopy (TEM) were performed to identify the existence of Bi 2 O 3 QDs and TiO 2 that loaded on the surface of BiOBr. The introducing of oxygen vacancies in TiO 2 broadened its light absorption region to the visible-light. The constitutes of Bi 2 O 3 QDs and BiOBr were regulated and the optimized photocatalyst BT1-B10 exhibited 94.1 % of removal rate for gaseous toluene degradation after 150 min irradiation of visible-light (>420 nm) as well as good recoverability and durability. This result was obviously superior to other comparison samples. In-situ DRIFTs spectra and Gas Chromatography-Mass Spectrometry (GC-MS) were carried out to provide a possible pathway for the toluene degradation. Additionally, a dual-channel electron transfer model based on the Z-scheme was proposed, which presented desirable visible-light response region, efficient charge separation efficiency, and enhanced redox ability. Notably, hydroxyl radicals (•OH) served as the dominant active species was confirmed by electron spin resonance (ESR) and gas-phase capture tests, that was beneficial to the ring-opening of toluene degradation. This dual Z-scheme heterojunction of Bi 2 O 3 QDs@TiO 2 /BiOBr photocatalyst showed great potential for the degradation of toluene under visible-light irradiation.
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产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Kai Song,Huilin Hou,Dongdong Zhang,Fang He,Weiyou Yang
Single-atomic catalysts (SACs) have been emerging as one of potential candidates in catalysts, owing to their unique merits with extremely high specific surface area as well as remarkably exposed active sites. Herein, we develop an in-situ gas-phase cation exchange strategy for engineering single-atomic Co on the surface of TiO 2 photoanode toward solar water splitting. It is verified that the atomically-dispersed Co with Co-O coordination could optimize the surface electronic structures, enhance the light absorption, promote the photoinduced charge transfer, lower the reaction barrier and accelerate the reaction kinetics, which consequently enable the overall improved photoelectrochemical (PEC) behaviors for photoanodes. As a proof of concept, the as-constructed TiO 2 -based photoanodes deliver robust stability up to 100 h and a photocurrent density up to 1.47 mA cm −2 at 1.23 V vs. RHE, which are superior to those of pristine TiO 2 , representing their significance for potential applications.
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DOI
高影响因子
Journal of Ocean University of China
·
2023
·Vol. 22
·期 2
·469-478
·
IF 1.6
Mei Xueqiao,Li Chunhu
Photocatalyst Ag/ZnO-TiO 2 was prepared by template method. The catalyst was characterized by XRD, SEM, and UV-vis DRS. Rhodamine B (RhB) and target pollutants were used to evaluate the photocatalytic performance of the catalyst under 40 W UV-lamp. The photocatalytic degradation mechanism of Rhodamine B was discussed through free radical quenching experiment. The experimental results show that hexagonal ZnO-TiO 2 can be successfully prepared by template method, and nano Ag particles are evenly loaded on the catalyst. Under the reaction conditions of 1% catalyst input and 40 W UV-lamp, the catalytic degradation rate of RhB by Ag/ZnO-TiO 2 was 98.28%. The photocatalytic degradation mechanism of Ag/ZnO-TiO 2 was explored by free radical quenching experiment. The experimental results show that H + and ·OH play a major role in the photocatalytic degradation of RhB by Ag/ZnO-TiO 2 .
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高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 19
·55044-55056
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IF 5.8
Bi Renke,Liu Jialong,Zhou Chutong,Shen Yijie,Liu Zhe,Wang Zhiyu
The construction of heterojunctions between semiconductors is a preferred route to improve overall photocatalytic activity. In this work, a facile and feasible method was innovatively developed to one-step prepare g-C 3 N 4 /TiO 2 heterojunctions via an absorption-calcination process using nitrogen and titanium precursors directly. This method can effectively avoid interfacial defects and establish a tight interfacial connection between g-C 3 N 4 and TiO 2 . The resultant g-C 3 N 4 /TiO 2 composites exhibited prominent photodegradation efficiency for tetracycline hydrochloride (TC-HCl) under visible light and simulated-sunlight irradiation. The optimal g-C 3 N 4 /TiO 2 composite (urea content of 4 g) showed the highest photocatalytic efficiency, which can degrade 90.1% TC-HCl under simulated-sunlight irradiation within 30 min, achieving 3.9 and 2 times increases compared to pure g-C 3 N 4 and TiO 2 , respectively. Besides, photodegradation pathways based on the role of active species ·O 2 − and ·OH were identified, indicating that a direct Z-scheme heterojunction was formed over the g-C 3 N 4 /TiO 2 photocatalyst. The enhanced photocatalytic performance can be attributed to the close-knit interface contact and the formation of Z-scheme heterojunction between g-C 3 N 4 and TiO 2 , which can accelerate the photo-induced charge carrier separation, broaden the spectra absorption range, and retain a higher redox potential. This one-step synthesis method may provide a new strategy for the construction of Z-scheme heterojunction photocatalysts consisting of g-C 3 N 4 and TiO 2 for environmental remediation and solar energy utilization.
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产品关联
DOI
PubMed
高影响因子
Small
·
2023
·Vol. 19
·期 30
·2300770
·
IF 13.3
Shilin Zhang,Qingjie Wang,Peng Zhang,Jie Wang,Yue Li,Chang Lu,Muhammad Tariq Sarwar,Xiongbo Dong,Qihang Zhao,Aidong Tang,Liangjie Fu,Huaming Yang
To achieve a high separation efficiency of photogenerated carriers in semiconductors, constructing high-quality heterogeneous interfaces as charge flow highways is critical and challenging. This study successfully demonstrates an interfacial chemical bond and internal electric field (IEF) simultaneously modulated 0D/0D/1D-Co 3 O 4 /TiO 2 /sepiolite composite catalyst by exploiting sepiolite surface-interfacial interactions to adjust the Co 2+ /Co 3+ ratio at the Co 3 O 4 /TiO 2 heterointerface. In situ irradiation X-ray photoelectron spectroscopy and density functional theory (DFT) calculations reveal that the interfacial Co 2+ O Ti bond (compared to the Co 3+ O Ti bond) plays a major role as an atomic-level charge transport channel at the p-n junction. Co 2+ /Co 3+ ratio increase also enhances the IEF intensity. Therefore, the enhanced IEF cooperates with the interfacial Co 2+ O Ti bond to enhance the photoelectron separation and migration efficiency. A coupled photocatalysis-peroxymonosulfate activation system is used to evaluate the catalytic activity of Co 3 O 4 /TiO 2 /sepiolite. Furthermore, this work demonstrates how efficiently separated photoelectrons facilitate the synergy between photocatalysis and peroxymonosulfate activation to achieve deep pollutant degradation and reduce its ecotoxicity. This study presents a new strategy for constructing high-quality heterogeneous interfaces by consciously modulating interfacial chemical bonds and IEF, and the strategy is expected to extend to this class of spinel-structured semiconductors.
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DOI
PubMed
高影响因子
LWT-FOOD SCIENCE AND TECHNOLOGY
·
2023
·
IF 6
Die Zhao,Chunji Li
Microbial carotenoids and lipids are two groups of versatile biomolecules widely used in the food, fuel, pharmaceutical, and cosmetic industries. Rhodotorula glutinis is one of the best-known oleaginous red yeasts that has the remarkable capability to produce an assortment of valuable carotenoids and lipids. Here, the effects of different concentrations of TiO 2 and H 2 O 2 treatments on carotenoid and lipid production in R. glutinis ZHK were investigated. After 120 h of cultivation, the total amount of carotenoids was significantly increased in the TiO 2 (100 mg/L: 23.165 μg/gdw, 750 mg/L: 19.65 μg/gdw) and H 2 O 2 (5 mM: 21.51 μg/gdw, 10 mM: 118.858 μg/gdw) treatments than the control (6.099 μg/gdw). In contrast, as compared to the control, the relative abundance of total lipids was significantly decreased in the TiO 2 (100 mg/L) and H 2 O 2 (10 mM) treatments, respectively. In response to TiO 2 and H 2 O 2 stresses, the increased carotenoids were probably attributed to the down-regulated lipid biosynthesis flux, while the decreased lipids might be ascribed to the down-regulated fatty acid biosynthesis flux. Our results presented herein not only provide an effective strategy for modulating carotenoid and lipid biosynthesis in R. glutinis ZHK but also reveal the molecular foundation to further enhance their bioproductivity by molecular manipulation.
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高影响因子
JOURNAL OF THE CHINESE CHEMICAL SOCIETY
·
2023
·Vol. 70
·期 4
·848-856
·
IF 1.8
Xiqiang Tian,Yanping Dong,Muhammad Zahid
The excellent photocatalytic hydrogenation of 4-nitrophenol (4-NP) to 4-aminophenol (4-AP) with NaBH 4 in the aqueous medium is still a big challenge. Herein, we report a facile one-pot evaporation-induced self-assembly (EISA) method to synthesize a series of CuO/TiO 2 nanocomposites. The as-synthesized CuO/TiO 2 photocatalysts exhibit remarkable catalytic activity under direct sunlight in selective hydrogenation of 4-nitrophenol (4-NP) to 4-aminophenol (4-AP) due to the synergistic interaction of guest copper nanoparticles with host titanium dioxide (TiO 2 ) species. Especially, 5 wt% CuO/TiO 2 nanocomposite revealed superior reaction rate constant (k) value (0.306 min −1 ) when compared to 3 wt% CuO/TiO 2 (0.192 min −1 ) and 7 wt% CuO/TiO 2 (0.240 min −1 ). Moreover, several characterization techniques (XRD, TEM, N 2 adsorption–desorption isotherm, DRS, and XPS) were executed to deeply investigate the effect of copper content on the bulk and interfacial properties of the catalysts. The characterization results proved that the superior photocatalytic hydrogenation over 5 wt% CuO/TiO 2 catalyst can be ascribed to moderate CuO loading as well as even dispersion of CuO species on the surface of active TiO 2 host, which can largely improve the light absorption ability within visible light region. Besides, the 5 wt% CuO/TiO 2 catalyst exhibits remarkable recyclability and durability, retaining its superior activity (above 95%) up to several repeating cycles, proving its practical applicability for hydrogenation reactions at domestic and industrial levels.
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DOI
高影响因子
Small Structures
·
2023
·Vol. 4
·期 10
·2300137
·
IF 15.9
Jingpeng Li,Rumin Ma,Sisi Yao,Daochun Qin,Yun Lu,Yuhe Chen,Zehui Jiang,Dongjiang Yang
Plant-based flow microreactors with natural channel structures, renewable properties, and environmental friendliness have increasingly gained popularity in heterogeneous catalysis. However, firmly immobilizing the catalysts simultaneously with ease and adaptability, maintaining great effectivity and long-term stability, is still a fundamental challenge. Herein, a highly efficient and ultrastable bamboo-based catalytic microreactor (CMR) containing mesoporous TiO 2 (M-TiO 2 )-encapsulating ultrafine Pd nanoparticles (NPs) is constructed for the continuous-flow hydrogenation of nitroaromatics. The fabrication of the Pd-TiO 2 catalysts in required bamboo microchannels (Pd-TiO 2 /B CMR) mainly involves a two-step region-selective synthetic strategy with ultra-low chemical usage, fast preparation, and low catalyst loading (0.007 wt%). The M-TiO 2 films: 1) provide abundant oxygen vacancies and enough open cavities to facilitate the growth of Pd NPs; 2) improve Pd dispersion and reduce particle size; 3) allow diffusion of reactants, and 4) induce strong metal-support interactions for enhanced catalytic activity and stability. The optimized Pd-TiO 2 /B CMR demonstrates high efficiency (>97%) and excellent stability (1,000 h) for the continuous-flow hydrogenation of nitroaniline, even under intermittent operation (12 h on/12 h off for five cycles) or in a real aqueous matrix (>200 h), making it a promising candidate for Pd-catalyzed hydrogenation.
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