CHEMPHYSCHEM
·
2023
·Vol. 24
·期 17
·e202300183
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IF 2.9
Yifan Ding,Fanghong Qin,Jialin Guo,Danming Gong,Qiufei Li,Xiangyi Wang,Xiuniang Tan,Haibo Liu,Zaiyin Huang
Graphical C@TiO 2-x photocatalyst with oxygen vacancy and carbon doping co-structure prepared by heat treatment is reported. It provides the possibility of regulating semiconductor photocatalysts to degrade pollutants in wastewater based on an integrated strategy. Oxygen Vacancy (OVs) and carbon doping of the photocatalyst body will significantly enhance the photocatalytic efficiency. However, synchronous regulation of these two aspects is challenging. In this paper, a novel C@TiO 2-x photocatalyst was designed by coupling the surface defect and doping engineering of titania, which can effectively remove rhodamine B (RhB) and has a relatively high performance with wide pH range, high photocatalytic activity and good stability. Within 90 minutes, the photocatalytic degradation rate of RhB by C@TiO 2-x (94.1 % at 20 mg/L) is 28 times higher than that of pure TiO 2 . Free radical trapping experiments and electron spin resonance techniques reveal that superoxide radicals (⋅O 2− ) and photogenerated holes (h + ) play key roles in the photocatalytic degradation of RhB. This study demonstrates the possibility of regulating photocatalysts to degrade pollutants in wastewater based on an integrated strategy.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Yayun Pu,Lu Jia,Qiang Huang,Xiaosheng Tang,Paramaconi Rodriguez,Limin Huang
Lowering Pt loading in the catalyst while maintaining its superior catalytic efficiency during hydrogen evolution reaction (HER) is essential for the large-scale application of water splitting. The utilization of strong metal-support interaction (SMSI) through morphology engineering has emerged as an effective strategy in fabricating Pt-supported catalysts. However, a simple and explicit routine to realize the rational design of morphology-related SMSI remains challenging. Here we report a protocol for the photochemical deposition of Pt, which benefits from the intrinsic difference in absorption capability of TiO 2 to establish proper Pt + species and charge separation domains on the surface. With a comprehensive investigation of the surface environment through experiments and Density functional theory (DFT) calculations, charge transfer from Pt to Ti, the separation of electron-hole pairs, and the enhanced electron transfer in the TiO 2 matrix were confirmed. It is reported that H 2 O molecules can be spontaneously dissociated by the surface Ti and O, generating OH stabilized by adjacent Ti and Pt. Such adsorbed OH group induces changes in the electron density of Pt, consequently favours the H adsorption and enhances the HER. Benefiting from the preferable electronic state, the annealed Pt@TiO 2 -pH9 (PTO-pH9@A) exhibits an overpotential of 30 mV to reach 10 mA cm−2 geo and a mass activity of 3954 A g-1Pt, which is 17-fold higher than the commercial Pt/C. Our work provides a new strategy for the high-efficient catalyst design by the surface state- regulated SMSI.
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COLLOIDS AND SURFACES B-BIOINTERFACES
·
2023
·
IF 5.8
Shuqing Xiang,Mingqian Wang,Li Li,Jian Shen
The gas therapy of some endogenous signaling molecules to treat diseases has caused extensive research, among which NO gas has shown great potential in fighting infection with various pathogens, promoting wound healing, etc. Here, we propose a photothermal/photodynamic/NO synergistic antibacterial nanoplatform by loading L -arginine (LA) on mesoporous TiO 2 and then encapsulating it with polydopamine . The obtained TiO 2−x [email protected] nanocomposite possesses both the excellent photothermal effect and ROS generation ability of mesoporous TiO 2 , and the release of nitric oxide (NO) from L -arginine under near-infrared (NIR) light irradiation , while the sealing layer of PDA could induce NIR-triggered NO controlled release. In vitro antibacterial experiments confirmed that the synergistic effect of TiO 2−x [email protected] nanocomposites has excellent antibacterial effects against Gram-negative and Gram-positive bacteria, while in vivo experiments showed that it has lower toxicity. It is worth noting that compared with the pure photothermal effect and ROS, the generated NO showed a better bactericidal effect , and NO had a better ability to promote wound healing. In conclusion, the developed TiO 2−x [email protected] nanoplatform can be used as a nanoantibacterial agent, which can be further explored in the related biomedical field of photothermal activation of multimodal combined antibacterial therapy.
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JOURNAL OF MEMBRANE SCIENCE
·
2023
·
IF 9.5
Jiesong Tan,Yiqing Zeng,Ze-Xian Low,Zhaochen Lin,Xinxiang Xu,Shasha Feng,Zhaoxiang Zhong,Weihong Xing
The filtration of high-temperature flue gases containing complex gas composition and oily particulate matter (PM) poses great challenges to the design of air filtration membranes. Ceramic nanofibers are potential membrane materials that possess the thermal resistance necessary for high-temperature filtration but the inherit poor brittleness limits their use. Herein, we report the fabrication of a flexible and porous Zr-doped TiO 2 nanofibrous membrane (Zr–TiO 2 NFM) for oily PM removal from high-temperature flue gas. The doping of Zr 4+ ions not only improved the mechanical strength , leading to an outstanding tensile strength as high as 1.78 MPa, but also endowed a high specific area (68.34 m 2 g −1 ). The prepared Zr–TiO 2 NFMs possessed a high filtration efficiency of 99.98% with low pressure drop of 96 Pa (industrial gas velocity of 1 m∙min −1 ) and excellent long-term stability after 5 cycles of filtration at 350 °C. Significantly, different capture and evolution behaviors of PM at 25–350 °C were discovered. Below 200 °C, the oily particles would adhere, coalesce, spread out and form oil film on fibers. Different from oily particles, the non-oily particles would attach and accumulate on the fibers when temperatures are higher than 200 °C. This study brings a new insight to deeply understanding the capture process of PM at different temperatures and designing next-generation membranes for high temperature flue gas filtration.
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APPLIED CLAY SCIENCE
·
2021
·
IF 5.467
Qiuxiang Wang,Zongxue Yu,Yuchuan Liu,Ximei Zhu,Runxuan Long,Xuyang Li
In this project, the Titanium dioxide nanowire (TiO 2 Nw) and layered double hydroxide (LDH) were introduced into the reduced graphene oxide (RGO) to make a composite material and then were assembled on the cellulose acetate (CA) membrane into photocatalytic composite membrane (RLT) through vacuum filtration with photocatalytic effect. The photocatalytic composite membrane (RLT) with high permeability and high rejection was constructed. Compared with other ratios of RLT membranes, RLT-0.5 composite membrane had a higher water flux of 432.38 L·m −2 h −1 bar −1 , and the rejection rate of dye were above 99%. In the rejection process of 10 cycles, that the rejection rate and flux of RLT-0.5 composite membrane to methylene blue (MB), malachite green (Mg) and Congo red (CR) were more stable regardless of whether there was light or no light. Of course, the rejection effect was better under light conditions, showing its excellent photocatalytic performance. In conclusion, RLT-0.5 composite membrane had excellent water purification ability and photocatalytic efficiency, which made it have a wide application in water treatment.
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NEW JOURNAL OF CHEMISTRY
·
2021
·Vol. 45
·期 47
·22123-22132
·
IF 3.591
Jing Liu,Dianming Li,Xiaofeng Liu,Jie Zhou,Hong Zhao,Nü Wang,Zhimin Cui,Jie Bai,Yong Zhao
Hydrogen evolution and dye degradation catalyzed by environmentally benign and inexpensive photocatalyst in aqueous solution is regarded as a promising avenue to effectively address the global energy and environmental crisis. It is difficult for traditional photocatalysts to perform efficient light harvesting, with conducive recycling and promoted charge separation and transport, which limit practical applications in photocatalytic conversion. In this study, a facile template-assisted coaxial electrospinning approach was explored to successfully build close contacted heterojunctions within the interface of g-C3N4 nanosheets and hollow porous TiO2 nanofibers, which significantly increased the separation efficiency of photo-induced electron–hole pairs in the visible-light region. A hollow and porous structure with abundant surface-active sites assisted in inducing multiple light reflection for more efficient light harvesting. Moreover, one dimensional TiO2/g-C3N4 composite nanofibers with a large length-to-diameter ratio would be more attractive for recovery. At the optimal g-C3N4 loading, hollow porous TiO2/g-C3N4-50% nanofibers exhibited the highest rate of hydrogen evolution and RhB degradation. The enhanced photocatalytic performance of hollow porous TiO2/g-C3N4 composite photocatalysts was mainly attributed to the synergistic effect of the hollow porous architecture and heterojunction. This work might make a significant contribution to insight into preparing hollow structure heterogenous nanofiber photocatalysts with improved activities in hydrogen generation and pollutant degradation.
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APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Cheng Liu,Yao Qin,Wei Guo,Yingzhang Shi,Zhiwen Wang,Yan Yu,Ling Wu
Enormous efforts have been devoted to exploring the influence of the materials’ morphology on photocatalytic performance, while the role of active site between them attracts less attention. Herein, three types of anatase nano-TiO 2 with different morphologies were successfully prepared for visible-light-driven photocatalytic selective oxidation of benzylamine. The material properties of the samples were systematically studied by various characterization techniques such as XRD, SEM, TEM, AFM, XPS, UV–vis DRS, ESR and in situ FTIR. Due to possessing clear advantages especially for having more active sites (coordinatively unsaturated Ti atoms and oxygen vacancies), the TiO 2 with porous structure shows more excellent photocatalytic performance than the other samples. Coordinatively unsaturated Ti atoms can chemisorb and activate benzylamine molecules via forming H-N … Ti coordination species, whose absorption property of visible light guarantees that TiO 2 samples can achieve the photocatalytic process under visible light. Oxygen vacancies can chemisorb and activate oxygen molecules to form reactive oxygen species (superoxide radical) by the reduction of photogenerated electrons. Finally, a possible synergetic mechanism based on the interaction of reactants and catalyst interfaces was proposed at the molecular level to illustrate the photocatalytic process.
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ChemCatChem
·
2021
·Vol. 14
·期 2
·e202101528
·
IF 5.686
Xue Sun,Fang Li,Zhimiao Wang,Hualiang An,Wei Xue,Yanji Wang
Graphical Nanocatalysis : Highly uniformly dispersed AgPd alloy nanoparticles were anchored on a porous TiO 2 carrier, obtained by calcining precursor and template MIL-125(Ti), and used for FA dehydrogenation, achieving excellent catalytic activity. At 60 °C, the total TOF value of Ag 2 Pd 8 /TiO 2 -M-450-catalyzed FA dehydrogenation was 2579 h −1 . TiO 2 with a disc-like morphology was prepared by direct pyrolysis of a titanium metal–organic framework [MIL-125(Ti)] in air. Highly dispersed bimetallic AgPd nanoparticles were then anchored on TiO 2 and their catalytic performance in the dehydrogenation of formic acid was systematically investigated. The Ag/Pd ratio had a significant effect on the catalyst activity, with Ag 2 Pd 8 /TiO 2 exhibiting the highest total turnover frequency value of 2579 h −1 at 60 °C under an ambient atmosphere. This excellent performance was attributed to the low-crystallinity anatase phase structure and large specific surface area of the TiO 2 carrier, the alloying effect of the AgPd nanoparticles, and abundant electron transfer between the carrier and metal alloy nanoparticles.
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Environmental Technology & Innovation
·
2021
·
IF 5.263
Xuecheng Ping,Yan Zhang,Qian Zhao,Yun Lu,Liang Hao
Flexible TiO 2 nanograss array film was prepared by simple chemical oxidation of Ti wire mesh at a low temperature of 353 K. To improve its visible-light-driven photocatalytic activity, we further carried out a low-temperature chemical reduction to introduce oxygen vacancies in the solution of ethylene glycol (EG) and ammonium fluoride (NH 4 F). The results of XPS and EPR confirmed the formation of surface and bulk oxygen vacancies was confirmed, and their concentrations increased as the reduction time increased. Compared with the as-annealed TiO 2 film, the as-reduced specimens exhibited higher visible-light-driven photocatalytic activity. When reduction time was 48h, the photocatalytic activity was increased by 15.8 times compared to the as-annealed sample. The remarkable improvement in photocatalytic activity should be ascribed to the oxygen vacancies’ introduction. The most excellent photocatalytic performance was obtained when a suitable concentration ratio of surface oxygen vacancies to bulk oxygen vacancies was reached. Low-temperature chemical reduction in the solution of EG + NH 4 F is very efficient and convenient for introducing defects such as oxygen vacancies and Ti 3 + .
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JOURNAL OF DISPERSION SCIENCE AND TECHNOLOGY
·
2021
·
IF 2.262
Sarenqiqige Bao,Haiou Liang,Chunping Li,Jie Bai
Heterojunction of TiO2 nanoparticles and BiOCl nanosheets grown on the carbon nanofibers (CNFs) were prepared by simply process that combine of electrospinning, solvothermal, and calcine. The photocatalytic activity of the as-obtained samples was evaluated by photodegradation of tetracycline (TC) in visible light irradiation (λ ≥ 420 nm). Compared with CNFs and TiO2/CNFs, BiOCl/TiO2/CNFs composites performed the best photocatalytic degradation performance (82%) and good stability. Moreover, the degradation rates of Norfloxacin, Ciprofloxacin, and Oxytetracycline are all more than 90%. Finally, trapping experiments were carried out, and a possible photocatalytic degradation mechanism was proposed.
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ChemCatChem
·
2021
·Vol. 14
·期 1
·e202101311
·
IF 5.686
Hang Yu,Ximeng Zhao,Feichao Wu,Yuhong Luo,Aizhong Jia,Yanji Wang,Jingde Li
Graphical Electrocatalysis : This work is about the development of the 3DOM Co/NPC@TiO 2-x ORR electrocatalyst. The unique TiO 2-x -based 3DOM structure and the synergistic between N, P co-doping and Co-decoration contribute to improve the ORR catalytic activity and stability. The proposed electrocatalyst exhibits an outstanding half-wave potential of 0.86 V in alkaline electrolyte. The resulting primary and flexible zinc-air batteries also deliver considerable performance. Developing efficient and durable electrocatalysts of oxygen reduction reaction (ORR) is critical for high-performance air cathodes. Herein, a novel three-dimensionally ordered macroporous oxygen-deficient TiO 2 framework embedded with N, P and Co-tridoped carbon (3DOM Co/NPC@TiO 2-x ) is elaborately designed for ORR. This unique structure offers a high surface area, good mass transfer, excellent electronic conductivity, and stability. Moreover, the experimental and theoretical studies reveal that the synergistic effect of N, P co-doping and Co-decoration is indispensable to promote the ORR performance, yielding high O 2 adsorption energy and lowering the reaction barriers simultaneously. Accordingly, the ORR catalytic activity and stability of the proposed electrocatalyst are better than Pt/C in alkaline media. The resulting primary zinc-air battery delivers a high open-circuit voltage (1.50 V) and specific capacity (820 Wh kg −1 ) at 20 mA cm −2 . This strategy, combining macroporous oxygen-deficient oxide support with binary heteroatom doping, provides a new perspective for exploiting efficacious ORR electrocatalysts.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2023
·
IF 11.4
Jiaying Xing,Qitong Xue,Jianjun Chen,Jinxing Mi,Xiaoping Chen,Jianqiang Shi,Zhiming Liu,Junhua Li
Vanadium-based catalysts play a pivotal role in the emission control of industrial NOx via selective catalytic reduction (SCR) technology. However, little attention has been paid to the potential emission of greenhouse gas N2O under complex working conditions. This work reports that a commercial V2O5/TiO2 catalyst may lead to significant N2O emission without greatly changing the outlet NOx concentration after chromium (Cr) deposition. With a Cr loading of 2 wt %, N2O concentration increased from 27.8 to 199.2 ppm at 350 °C with the value of outlet N2O/(N2O+N2) from 2.5% to 19.4%. Experimental results combined with DFT+U calculations suggest that nonselective catalytic reduction (NSCR) is the main route for N2O formation in a wide temperature range of 250 ∼ 400 °C. It is stemmed from the fact that the covalent interaction between Cr and V species on the V2O5/TiO2 surface accelerates the conversion of V4+ + Cr6+ → V5+ + Cr3+, leading to a larger proportion of surface V5+. More importantly, surface V5+ is highly related to the redox property of the V2O5/TiO2 catalyst, which is beneficial to NSCR reaction rather than the standard SCR process. The work suggests that to better inhibit the emission of greenhouse gases during the NH3–SCR process, monitoring N2O emission should be included along with the NOx concentrations, especially in complex flue gases.
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