Nano Research
·
2022
·Vol. 16
·期 4
·4786-4792
·
IF 10.269
Zhang Jin,Gao Mengting,Wang Ruiyi,Li Xincheng,Huang Tianfen,Wang Jing,Wang Yunwei,Zheng Zhanfeng
It is fascinating to explore the distribution of CO 2 hydrogenation products regulated by heterogeneous catalysts, as both the chemical state of surface metals and structure of the support itself of the supported catalysts may affect the performance of CO 2 hydrogenation. Herein, the complete switching of CO 2 hydrogenation products from CH 4 to CO can be realized by induction of Cl into Ru/TiO 2 catalyst. Density functional theory (DFT) calculations indicated that Cl ions were mainly located on the Ru metal sites of Ru/TiO 2 catalysts. Bader charge analysis and Ru 3p X-ray photoelectron spectra (XPS) results suggested that electrons transferred from Ru to Cl, resulting in the decrease of electron density of Ru. In situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) of CO 2 hydrogenation and CO adsorption proved that with the increase of the Cl ion content, the adsorption of CO on the catalyst surface was significantly weakened, and resulted in the high CO selectivity. Our work demonstrates the role of Cl ions in regulating the distribution of CO 2 hydrogenation products, and provides new ideas for regulating other catalytic processes.
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Asia-Pacific Journal of Chemical Engineering
·
2022
·Vol. 18
·期 1
·e2840
·
IF 1.777
Qiaolin Ren,Ruirui Yang,Junying Li,Wenjun Yan,Zhongde Wang,Ailian Wu
Electrocatalytic oxidation technology has been proved as an efficient method for degradation in organic wastewater. The service lifetime and degradation efficiency of the electrode, one crucial struggle, limits the broad application of electrocatalytic oxidation technology. Herein, a Ru/Ir doped TiO 2 electrode with a long service lifetime was developed. Accelerated life experiment showed that the service life of an electrode was 33 h when the concentration of sulfuric acid was 1 M and the current density was 2000 mA·cm −2 . The influence on the phenol degradation was evaluated by researching the operating parameters. In particular, the possible mechanism of phenol removal at different pH is elucidated. It is found that acidic environment is favorable for chemical oxygen demand (COD) and phenol removal at a current density of 20 mA·cm −2 , pH 3 at 800 ppm NaCl, which can make the removal rates of phenol and COD with Ru/Ir doped TiO 2 anode up to 97.21% and 100%. In addition, it was demonstrated that the hydroxyl radicals play a foremost role in the degradation of phenol. Given the well stability and high service life, the Ru/Ir doped TiO 2 electrode holds promise for further industrial application in wastewater treatment.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Meilan Pan,Shuang-yin Tang-hu,Chenhao Ni,Haihua Chen,Bingjun Pan
Fluorine-containing fluoroquinolones are cumulative toxins and pose a grave threat to health of animals and human beings, and an effective and feasible strategy to the defluorination by breaking C-F bond to decrease toxicity is in an urgent requirement. Herein, Ti(III)-laden TiO 2 nanotube arrays (RTNA) were deliberately fabricated for electrochemical degradation and defluorination of levofloxacin (LVF). Characterizations verified that Ti(III) and oxygen vacancies were generated on RTNA via electrochemical reduction of TiO 2 nanotube arrays (TNA). The degradation kinetics of LVF on RTNA (0.85 h −1 ) was increased by about 15 times as compared with that on TNA (0.06 h −1 ); the corresponding degradation and defluorination efficiencies by RTNA were also dramatically increased. Moreover, the effect of electrolyte on the defluorination efficiency suggests the significant role of sulfate; that is, abundant sulfate radical (SO 4 -• ) was generated in the media of sodium sulfate during the electrochemical oxidation process , and it served as the dominant radical to break C-F bond for the defluorination of LVF, whereas it is not the case for hydroxyl radical (•OH) in sodium carbonate. The pathways and mechanisms of degradation and defluorination in electrolyte of sodium sulfate or carbonate were proposed and further confirmed the difference in the electrolyte-dependent degradation mechanisms.
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Nature Communications
·
2022
·Vol. 13
·期 1
·1-12
·
IF 17.694
Guo Yalin,Huang Yike,Zeng Bin,Han Bing,AKRI Mohcin,Shi Ming,Zhao Yue,Li Qinghe,Su Yang,Li Lin,Jiang Qike,Cui Yi-Tao,Li Lei,Li Rengui,Qiao Botao,Zhang Tao
Semi-hydrogenation of acetylene in excess ethylene is a key industrial process for ethylene purification. Supported Pd catalysts have attracted most attention due to their superior intrinsic activity but often suffer from low selectivity. Pd single-atom catalysts (SACs) are promising to significantly improve the selectivity, but the activity needs to be improved and the feasible preparation of Pd SACs remains a grand challenge. Here, we report a simple strategy to construct Pd 1 /TiO 2 SACs by selectively encapsulating the co-existed small amount of Pd nanoclusters/nanoparticles based on their different strong metal-support interaction (SMSI) occurrence conditions. In addition, photo-thermo catalysis has been applied to this process where a much-improved catalytic activity was obtained. Detailed characterization combined with DFT calculation suggests that photo-induced electrons transferred from TiO 2 to the adjacent Pd atoms facilitate the activation of acetylene. This work offers an opportunity to develop highly stable Pd SACs for efficient catalytic semi-hydrogenation process.
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ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Lin-Yu Zhou,Shao-Bo Cao,Liang-Liang Zhang,Guolei Xiang,Xiao-Fei Zeng,Jian-Feng Chen
Supports can widely affect or even dominate the catalytic activity and selectivity of nanoparticles because atomic geometry and electronic structures of active sites can be regulated, especially at the interface of nanoparticles and supports. However, the underlying mechanisms of most systems are still not fully understood yet. Herein, we construct the interface of Co3O4/TiO2 to boost ammonium perchlorate (AP) catalytic decomposition. This catalyst shows enhanced catalytic performance. With the addition of 2 wt % Co3O4/TiO2 catalysts, AP decomposition peak temperature decreases from 435.7 to 295.0 °C and activation energy decreases from 211.5 to 137.7 kJ mol–1. By combining experimental and theoretical studies, we find that Co3O4 nanoparticles can be strongly anchored onto TiO2 supports accompanied by charge transfer. Moreover, at the interfaces in the Co3O4/TiO2 nanostructure, NH3 adsorption can be enhanced through hydrogen bonds. Our research studies provide new insights into the promotion effects of the nanoparticle/support system on the AP decomposition process and inspire the design of efficient catalysts.
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ChemSusChem
·
2022
·Vol. 15
·期 8
·e202200188
·
IF 9.14
Chengjin Li,Xiaoxia Zhou,Qingming Zhang,Yi Xue,Zhaoyu Kuang,Han Zhao,Chung-Yuan Mou,Hangrong Chen
Graphical CO 2 to formic acid : A novel kind of Sn/TiO 2 /Si photocathode is developed for CO 2 reduction reaction (CO 2 RR), which shows excellent selectivity to HCOOH under applied potential. The improved light performance and heterojunction composite structure, together with the modulated electronic configuration, co-contribute to the high CO 2 RR performance. Using renewable energy to convert CO 2 into liquid products, as a sustainable way to produce fuels and chemicals, has attracted intense attention. Herein, a novel heterostructured photocathode composed of Si wafer, TiO 2 layer, and Sn metal particles has been successfully fabricated by combining of a facile hydrothermal and electrodeposition method. The obtained Sn/TiO 2 /Si photocathode shows enhanced light absorption performance by the surface plasmon resonance effect of Sn metal. Especially, the Sn/TiO 2 /Si photocathode together with rich oxygen vacancy defects jointly promote photoelectrochemical CO 2 reduction, harvesting a high faradaic efficiency of HCOOH and a desirable average current density (−4.72 mA cm −2 ) at −1.0 V vs. reversible hydrogen electrode. Significantly, the photocathode Sn/TiO 2 /Si also shows good stability due to the design of protecting layer TiO 2 . This study provides a facile strategy of constructing an efficient photocathode to improve the light absorption performance and the electron transfer efficiency, exhibiting great potential in the CO 2 reduction.
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JOURNAL OF NANOPARTICLE RESEARCH
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2022
·Vol. 24
·期 3
·1-22
·
IF 2.533
Yang Chunyan,Xue Ziwei,Yin Hao,Lu Ke,Liu Wei
In this work, the photodegradation of methylene blue was investigated by constructing a novel photocatalysis reactor, which was filled with aqueous foam. Nanoscale TiO 2 particles were used as photocatalyst. In order to obtain stable foam phase, cetyl trimethyl ammonium bromide (CTAB) was used as the frother, and its suitable initial concentration in the feeding solution was 0.20 g/L. Under the suitable conditions of loading liquid volume 200 mL, initial concentration of TiO 2 nano-catalysts in the feeding solution 5.0 g/L, inner diameter of foam column 18 mm, aperture diameter of gas distributor 125 μm, and circulating velocity of bulk solution 500 mL/h, the maximum degradation percentage of methylene blue was 97.6 ± 1.2%. Atomic force microscopy (AFM) analysis suggested that the entrainment effect of rising bubbles and the circulation flow of bulk solution inside the aqueous foam did not cause the conspicuous aggregation of TiO 2 nano-catalysts under the suitable conditions, but their surface roughness decreased. Meanwhile, foam entrainment had not a significant impact on the polydispersity of TiO 2 nano-catalysts. In contrast to the photodegradation of methylene blue in aqueous solution, the photocatalysis process using aqueous foam is the intensity of light received by TiO 2 nano-catalyst increases, and irradiation period is less. This work is expected to provide new insight into the rational design of photocatalysis reactor, to facilitate the harmless treatment of dyestuff wastewater. Graphical abstract
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SURFACE & COATINGS TECHNOLOGY
·
2022
·
IF 4.865
Zhuohan Chen,Xiaojing Su,Wenjian Wu,Siting Chen,Xiaofan Zhang,Yunhui Wu,Huali Xie,Kunquan Li
Natural wood, with its unique porous structure, has been widely modified for separating oil-water mixtures. However, the separation efficiency is often unsatisfactory, and little attention is focused on mitigating secondary pollution after its usable lifespan. Here, a superhydrophobic material consisting of delignified wood coated with titanium dioxide (TiO 2 ) and polydimethylsiloxane (PDMS) was prepared. The resulting PDMS@TiO 2 wood possessed outstanding superhydrophobicity, with a water contact angle of 160 o . Owing to its longitudinal channels and excellent water repellency, the wood was successfully used to separate oil-water mixtures, with a high permeation flux of up to 6111 L·m −2 ·h −1 and separation efficiency of up to 93.4%. Importantly, PDMS and other oil pollutants were capable of being largely degraded after use via photocatalysis of the TiO 2 layer, and the degradation reached 8.56 wt% within 30 days. The results from this study provide a method for fabricating functional superhydrophobic wood with photocatalytic degradation ability for efficient oily wastewater treatment.
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CERAMICS INTERNATIONAL
·
2022
·
IF 5.532
Xuan Wang,Hao Ding,Guocheng Lv,Run Zhou,Ruixin Ma,Xifeng Hou,Jianmeng Zhang,Wei Li
Generally, superhydrophilic self-cleaning coatings are prepared from semiconductors with photocatalytic properties. Organic pollutants attached to the coating surface can be degraded by its photocatalytic performance realizing a self-cleaning goal. Herein, SiO 2 –TiO 2 composite particles were fabricated by the hydrolysis and precipitation of TiOSO 4 , and SiO 2 microspheres were chosen as carriers, which are inexpensive and environmentally friendly. Then, superhydrophilic self-cleaning SiO 2 –TiO 2 coatings were fabricated by spraying the composites on the surfaces of substrates. The morphology, structure and self-cleaning performance of the SiO 2 –TiO 2 coating were characterized and tested. The results revealed that nano-TiO 2 was loaded on the surfaces of SiO 2 microspheres uniformly forming a hierarchical micro/nanostructure. The SiO 2 –TiO 2 composite particles exhibited excellent photocatalytic degradation performance, and the degradation rate of methyl orange (10 ppm) was more than 98% under UV irradiation for 40 min. Furthermore, the coating prepared with the SiO 2 –TiO 2 composite particles exhibited superhydrophilicity. A water droplet spreads completely on the coating surface in 0.35 s, and the contact angle reaches 0°. In addition, rhodamine B (RhB) and methylene blue (MB) on the coating surface can be degraded efficiently under sunlight irradiation. The SiO 2 –TiO 2 composite particles can be sprayed directly on the surfaces of concrete, brick, wood, and glass slides. Therefore, the particles showed good adaptability to different substrates. The superhydrophilic property was due to the hydrophilicity of SiO 2 and TiO 2 , the hierarchical micro/nanostructure of the SiO 2 –TiO 2 composites, and the photoinduced superhydrophilicity of TiO 2 . The above experimental results show that the as-prepared superhydrophilic self-cleaning SiO 2 –TiO 2 coating has a large application potential.
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Coatings
·
2022
·Vol. 12
·期 3
·366
·
IF 3.236
Shengping Zhang,Chen Yu,Jingyi Tan,Yuxin Wang,Zhen He
In this study, Ti/SnO2-Sb2Ox-TiO2electrodes were produced using a sol-enhanced electrodeposition technique from methanesulfonate electrolytes. The surface microstructures of Ti/SnO2-Sb2Ox-TiO2were observed, and their phase constituents were determined. The surface features were analyzed by X-ray photoelectron spectroscopy. Linear sweep voltammetry and degradation tests were also conducted to determine the degradation performance. The results show that the addition of TiO2sol affects the microstructures of Ti/SnO2-Sb2Ox-TiO2electrodes, while a uniform coating surface can be obtained at a proper sol concentration in electrolytes. Adding TiO2sol also causes deep oxidation of Sb and generates more adsorbed oxygen on the electrode surface. The favorable surface features and the well-dispersed TiO2in the coatings of 10 mL/L TiO2modified Ti/SnO2-Sb2Ox-TiO2electrodes award them the best electrocatalytic performance, and their uniform coating surface prolongs the electrode service life.Keywords:SnO2-Sb2Ox;sol-enhanced electrodeposition;organic degradation
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Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Haimeng Huang,Jianfeng Zhang,Chunmei Tang,Anyu Li,Tianmeng Zhang,Huapeng Xue,Daofeng Zhang
Photocatalytic sterilization has been recently realized as a competitive strategy for effective water purification just using sunlight, for which the new photocatalytic materials play the key role. In this study, a novel Z-scheme heterojunction material MXene/TiO 2 /Bi 2 S 3 was proposed, where TiO 2 nanoparticles and Bi 2 S 3 microspheres were uniformly distributed on the MXene nanosheets through facile hydrothermal oxidation and ultrasonic dispersion. With this Z-scheme heterojunction MXene/TiO 2 /Bi 2 S 3 , effective and quick sterilization of both Gram-negative bacteria and positive bacteria in only 120 min was realized. Especially, the apparent reaction constant for S. aureus reached 0.01659 min −1 , substantially higher than MXene and other related materials in literature. This could be ascribed to the narrow band gap (1.04 eV), the wide range of light absorption range (420 nm), and the low impedance of the as-obtained composite, facilitating the transfer and separation of photo-generated charges, which was also validated through the first-order kinetic model and DFT simulation calculations. Thus, the reactive species produced by photocatalysis effectively disrupted the defense action of the bacteria by damaging bacterial membrane structure, and reducing enzyme activity as well as cellular metabolism. This efficient and low-cost material for water disinfection has a great potential for practical applications in the future.
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Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Tangtong Ju,Yue Dai,Hailong Tang,Meiling Wang,Xiao Sun,Min Wang,Yongqing Ma,Ganhong Zheng
Direct conversion of CH 4 to high valued chemicals under mild conditions is attractive but full of challenges. Here, we present a ternary composite that consists of Ni-doped TiO 2 nanocubes (NCs) and CNTs as a new kind of catalyst (denoted as CNTs-Ni@TiO 2 NCs) for CH 4 photocatalytic conversion to C1 oxygenated products at 30 °C. Using H 2 O 2 as an oxidant, a high C1 oxygenated products yield and selectivity of 1.43 mol/(mol Ni ·h) and 95.6% can be reached in 2 h at 30 °C. The superior photocatalytic performance resulted from the synergistic effects of TiO 2 NCs, Ni species, and CNTs such as enhanced visible light absorption , improved electron/hole separation and charge transfer property, and lowered C-H bond cleavage energy required for CH 4 activation, were carefully studied. Good reusability of the catalyst was studied by recycle experiments. Possible reaction mechanism based on the radical routes were carefully discussed by combining in-situ Fourier transform infrared spectroscopy , X-ray photoelectron spectroscopy, electron spin resonance spectroscopy, radical scavenger experiments and density functional theory calculation.
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