JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Jie Xu,Hongji Li,Huimin Feng,Yuqin Ma,Dandan Wang,Jianwei Zhu
The removal of refractory organic contaminants in the environment is vital, but developing highly active catalysts with a simple synthesis process remains a challenge. Herein, NH 2 -MIL-125(Ti) (Ti-MOF) as a template, Ti 3+ -TiO x clusters of different quantities were embedded in the CdIn 2 S 4 nanosheets to construct Ti 3+ -TiO x /CdIn 2 S 4 (TiCIS) heterojunction by an in-situ self-assembly strategy, which had a hollow structure, strong visible light absorption, high separation rate of carriers, and more active sites. During the degradation experiment of Rhodamine B (RhB), TiCIS25 exhibited the best photocatalytic performance, and 98.0% of RhB was degraded within 60 min of visible irradiation. The intermediates in the RhB degradation and their ecotoxicity were analyzed, which revealed that RhB degradation was a detoxification process. The radical trapping experiments and electron spin resonance (ESR) tests indicated that e - , 1 O 2 , and ·O 2 - are the main active species for RhB degradation. Moreover, a possible photocatalytic mechanism was proposed based on electrochemical tests. The photodegradation performance of the as-prepared TiCIS catalyst under different reaction parameters (authentic water matrices, initial pH, coexisting anions, organic matter concentration, actual sunlight, reaction temperature, and multiple pollutants) and circulating experiments, as well as the photo-reduction process CO 2 , reflected that TiCIS25 possessed excellent practicability, cyclic stability, and universal applicability. Above all, TiCIS25 exhibited great potential in photocatalytic processes, and the work provided a feasible strategy for designing high-performance photocatalysts .
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2025
·
IF 11.3
Wenjie Liao,Ling Zhou,Xiaoqiang Wang,Yue Liu,Zhongbiao Wu
Both improving the activity and reducing SO3 emissions during selective catalytic reduction of NOx by the NH3 (NH3–SCR) process over commercial V–Ti-based catalysts remain a challenge. Herein, Ce and P cooperatively modified the VMo/Ti catalyst to address this challenge. Within the temperature range of 250–350 °C, the optimal VMoCeP/Ti catalyst achieved a NO conversion of more than 95% and maintained a SO2 oxidation ratio below 1.0%. The enhanced SCR activity of the modified catalyst could be attributed to the improvement in surface acidity and redox capacity by the addition of Ce and P, which would promote NH3 adsorption and activation. Meanwhile, Ce and P coaddition could regulate the surface structure of vanadyl species from predominantly polymeric to a more dimeric form, which could also promote the SCR reaction. More importantly, except for the suppressed sulfation of vanadium species, both a lower proportion of polymeric vanadyl species and the strong interactions among V–Ce–P species could raise the energy barrier of the decomposition of sulfated vanadium species into SO3, thereby inhibiting SO2 oxidation. This work provided novel insights into developing efficient SCR catalysts with low SO2 oxidation ratios for both the academic and industrial fields.
研究领域:
催化化学
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环境化学
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材料科学
·
化学工程
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CRYSTAL GROWTH & DESIGN
·
2023
·
IF 3.8
Caiyun Liu,Huihui Niu,Dexin Wang,Yanshu Liu,Amir Said,Guo Wang,Chen-Ho Tung,Yifeng Wang
Selective oxidation utilizing sunlight and O2 is a cost-effective technique for converting organic raw materials into value-added products. We present a novel Bi-doped Ti-oxide cluster (TOC), Ti19Bi2, for the selective conversion of benzyl alcohols to benzaldehydes under sunlight irradiation. It is prepared as single crystals and precisely characterized by single-crystal X-ray diffraction. A structure–activity study is performed by combining experiments and density functional theory. Bi mainly contributes to the LUMO + 1 of Ti19Bi2, with a minor effect on the band gap energy. Bi doping causes the accumulation of photogenerated electrons at Bi sites, resulting in potent reducing power and high O2 activation ability, promoting charge separation and interfacial charge transfer. The Ti19Bi2 solar system showed good activity, selectivity, substrate scope, and catalyst recyclability in the selective oxidation of benzyl alcohols. It outperforms reference TOCs free of Bi, such as Ti8O8Bz16 (Bz = benzoate) and commercial TiO2 P25. Additionally, Ti19Bi2 is effective in photocatalytic CO2/epoxide cycloaddition and dye degradation reactions.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Jing Li,Guo Lin,Fangguan Tan,Likang Fu,Biao Zeng,Shixing Wang,Tu Hu,Libo Zhang
In the context of industrialization and severe wastewater pollution, mercury ions pose a major threat due to their high toxicity. However, traditional adsorbents and common metal-organic framework (MOF) materials have limited effectiveness. This study focuses on combining magnetic materials with functionalized titanium-based MOF composite (SNN-MIL-125(Ti)@Fe 3 O 4 ) to improve mercury ion adsorption. Through comprehensive characterization and analysis, the adsorption performance and mechanism of the material were studied. The optimal adsorption of the material was achieved at pH 5, exhibiting a pseudo-second-order adsorption model and the Hill theoretical capacity of 668.98 mg/g. Hill and Tempkin models confirmed the presence of chemical and physical adsorption sites on the material surface. Thermodynamic experiments showed a spontaneous endothermic process. Despite the presence of interfering ions, the material exhibited high selectivity for mercury ions . After four cycles, adsorption performance decreased by only 8%, indicating excellent reusability. Nitrogen- and sulfur-containing functional groups played a key role in mercury ion adsorption. In conclusion, SNN-MIL-125(Ti)@Fe 3 O 4 , as a magnetic MOF adsorption material, showed potential for effective remediation of mercury-contaminated wastewater. This study contributes to the development of efficient adsorption materials and enhances the understanding of their mechanism.
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JOURNAL OF CATALYSIS
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2023
·
IF 7.3
Zijun Yang,Qiang Yu,Hua Wang,Qingfeng Ge,Xinli Zhu
Ketonization of propionic acid has been investigated on Lewis acidic TS-1 and Ti-Beta zeolites to understand the reaction mechanism and effects of pore topology and hydrophobicity. Characterizations showed that TS-1 and Ti-Beta (Si/Ti = 40) exhibited a similar acidity whereas TS-1 was more hydrophobic than the silanol-rich Ti-Beta. TS-1 showed higher activity, selectivity, stability and was more resistance to H 2 O than Ti-Beta. A combination of infrared spectroscopic, isotopic and kinetic studies showed that the molecularly adsorbed monodentate propionic acid is the most abundant reactive intermediate, and C-C coupling is the rate-determining step. The mechanism of ketonization of propionic acid at isolated tetrahedral Ti centers can be described by a Langmuir-Hinshelwood model. The turnover rate on TS-1-40 is ∼ 1.3 times higher than that on Ti-Beta-40, which is consistent with the lower fitted free activation energy, i.e., the energy difference between C-C coupling transition state and two co-adsorbed propionic acids at a Ti center. The slightly lower activation enthalpy on Ti-Beta-40 than TS-1-40 is over-compensated by much larger entropy penalty, due to more silanol groups and hydrogen bonded propionic acids in close proximity to the Ti center for Ti-Beta-40, which impose additional steric hindrance to bulkier C-C coupling complex at transition state and outweigh the difference of steric hindrance of pore confinement between MFI and BEA frameworks. This work provides insight into the ketonization mechanism on Lewis acidic zeolites, and indicates that moderate pore size with hydrophobic property promotes ketonization of carboxylic acid at isolated tetrahedral Ti centers confined in zeolites.
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Catalysts
·
2023
·Vol. 13
·期 6
·971
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IF 3.9
Chunjie Shi,Xiaofeng Yu,Wei Wang,Haibing Wu,Ai Zhang,Shengjin Liu
The catalytic activity and cyclic catalysis of different methyl benzoates were studied by using a series of Lewis solid acid catalysts. The iron-supported zirconium/titanium solid acid catalysts were characterized using FTIR, SEM, XRD, and BET. The details of catalytic activity and cyclic catalysis verified that the catalyst catalyzed the reactions of 31 benzoic acids with different substituents and methanol. In addition, the mechanism was revealed according to the microstructure, acid strength, and specific surface area of the catalysts, and the yields of methyl benzoates by the GC-MS. Zr ions had significant effects on the catalytic activity of the catalyst. A certain proportion of Fe and Ti ions additionally enhanced the catalytic activity of the catalyst, with the catalyst-specific composition of Fe:Zr:Ti = 2:1:1 showing optimal catalytic activity. A variety of substituents in the benzene ring, such as the electron-withdrawing group, the electron-donating group, large steric hindrance, and the position of the group on the benzene ring, had regular effects on the catalytic activity of the methyl benzoates. An increase in the catalyst activity occurred owing to the increases in the catalyst surface and the number of acid sites after the Fe ion was added. The catalytic activity remained unchanged after the facile recycling method was performed.Keywords:zirconium/titanium solid acid;iron-supported;methyl benzoate compounds
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COMPOSITES PART A-APPLIED SCIENCE AND MANUFACTURING
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2023
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IF 8.7
Wei Wang,Xiangyu Jin,He Huang,Shuang Hu,Can Wu,Hebing Wang,Yiwu Pan,Changqing Hong,Xinghong Zhang
Ablative thermal protection systems are considered to be one of the most promising means of protection for spacecraft re-entry, but challenges remain. Herein, efficient Ti-Si binary modified carbon fiber reinforced phenolic aerogel nanocomposites (C f /TS-PR) were originally designed based on a multi-stage construction strategy. The C f /TS-PR exhibited desirable mechanical strength , good thermal insulation with a minimum thermal conductivity of 0.0756 W/(m·K), remarkable thermal stability and outstanding ablation resistance, benefiting from the features of TiO 2 and the special structure of TiO 2 -SiO 2 coating. The linear ablation rates are as low as 0.004 and 0.003 mm/s at the heat flow of 1.0 and 1.5 MW/m 2 , respectively. The mass loss rates are as low as 0.006 and 0.009 g/s at the heat flow of 1.0 and 1.5 MW/m 2 , respectively. These results indicate that the C f /TS-PR nanocomposites can be a reliable thermal protection material for the future high-temperature service environment of ultra-high-speed vehicles and neutral rockets.
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DALTON TRANSACTIONS
·
2023
·Vol. 52
·期 11
·3517-3525
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IF 4
Shihui Wang,Zhoujun He,Ling Wu,Deling Wang,Ruiru Si,Xiyao Liu,Ruowen Liang
Due to their explicit structure, metal–organic frameworks (MOFs) have been supposed to be credible platforms to research the micro-mechanism of heterogeneous photocatalysis. In this study, amino-functionalized MOFs (MIL-125(Ti)–NH2 (denoted as MTi), UiO-66(Zr)–NH2 (denoted as UZr) and MIL-68(In)–NH2 (denoted as MIn)) with three different metal centers were synthesized and applied for the denitrification of simulated fuels under visible light irradiation, during which pyridine was used as a typical nitrogen-containing compound. The results showed that MTi had the best activity among the above three MOFs, and the denitrogenation rate increased to 80% after 4 h of visible light irradiation. On the grounds of the theoretical calculation of pyridine adsorption and actual activity experiments, it can be presumed that the unsaturated Ti4+ metal centers should be the key active sites. Meanwhile, the XPS and in situ infrared results verified that the coordinatively unsaturated Ti4+ sites facilitate the activation of pyridine molecules through the surface –N⋯Ti– coordination species. The coordination–photocatalysis synergism promotes the efficiency of photocatalytic performance and the corresponding mechanism is proposed.
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Journal of Water Chemistry and Technology
·
2023
·Vol. 45
·期 2
·164-175
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IF 0.6
Jing Meng,Geng Cong,Guan Yinyan,Gao Weichun,Ming Hao,Li Dan,Wang Nan,Liu Shiyue,Jiang Wei,Liang Jiyan,Wang Xueying
Abstract The sol-gel approach was utilized to make a copper-doped Ti/SnO 2 -Sb anode for electrochemical oxidation of norfloxacin (NOR). Sycanning electron microscopy (SEM), energy dispersive spectrometry (EDS), X-ray diffraction (XRD), linear scan voltammograms (LSV), and cyclic voltammetry (CV) were used to examine the anode’s surface morphology and electrochemical characteristics. The results show that the doped metal makes the anode coating denser and smoother, which is more conducive to resistance to electrochemical corrosion. The electrochemical degradation of NOR utilizing the constructed anode was examined in relation to reaction circumstances such as current density, pH value, and initial NOR concentration. Within the selected range of reaction conditions, the removal rate of NOR using Ti/SnO 2 –Sb–Cu electrode was significantly higher than that of blank electrode. The following were the shifting trends: NOR removal efficiencies grew with applied current density and initial NOR concentration, and reduced with increasing pH value. Water samples with different reaction times were taken and tested by UV-Vis spectrum. As can be seen from the results, with the progress of the reaction, the intensity of the characteristic peak decreased, indicating that NOR is degraded gradually. The electrochemical degradation pathways of NOR were studied using liquid chromatography coupled with mass spectrometry (LC-MS). Six intermediates were detected and a possible reaction pathway for the degradation of NOR by electrochemical oxidation was proposed.
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POLYMER SCIENCE SERIES B
·
2019
·Vol. 61
·期 2
·124-131
·
IF 0.907
Guanghong Lin,Xiang Hongping,Xi Lu,Wen Zhixia,Wang Zhaowei,Yu Junwei,Liu Xiaoxuan
Abstract A tricomponent catalyst comprising titanium tetrachloride, triisobutyl aluminum and diphenyl ether is developed for the highly cis -1,4-selective polymerization of isoprene. The influence of the content of diphenyl ether and its complexation order on polymerization, microstructure and performance of polyisoprene are studied. The polyisoprene synthesized presents high monomer conversion (91–99%). With the increasing of diphenyl ether content, intrinsic viscosity and viscosity-average molecular weight of polyisoprene increase. The molar percentage of cis -1,4-unit is almost unaffected by diphenyl ether and different complexation sequence. The polyisoprene reveals comparable T g (–61.31°C) and mechanical strengths (11.14 MPa, 667%) to commercially available LHIR-80 synthesized with neodymium. However, the viscosity and viscosity-average molecular weight of the former are lower than that of the latter, which avails the processability and maintains excellent mechanical properties.
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ACS Omega
·
2019
·
IF 2.584
Guanghui Li,Jiyang Xie,Jing Wang,Lei Xia,Yong Li,Wanbiao Hu
Lattice disorder has emerged as a novel strategy to realize visible-light photocatalytic activity, but many existing studies often involved reduction states simultaneously. Photocatalysts based on only the lattice disorder but without the reduction states are still quite lacking and challenging. To this end, we explored a new type of lattice disorder in terms of the surface atom nonstoichiometry strategy in BaTiO3. Well-dispersed tetragonal BaTiO3 nanocrystals with a uniform size (∼20 nm) and cuboid morphology were hydrothermally synthesized through controlling over t-butylamine and oleic acid. HRTEM coupled with structural evolution analysis reveals the existence of a Ti-rich layer on BaTiO3 nanocrystals with surface atom disorder, which gives an overall Ti/Ba ratio of 1.50:1. This is mainly dominated by the oriented adsorption between oleic acid and surface Ba2+ of the nucleus during solution reaction. Such a surface disorder and Ti-rich nonstoichiometry effect could facilitate the enhanced visible-light absorption with a wavelength span of 400–700 nm that enables the superior visible-light photocatalytic property, which is not subject to the reduction states. This work demonstrates a first white material presenting a new type of lattice disorder that would be helpful for a wide range of photocatalyst explorations.
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FUEL
·
2018
·
IF 4.908
Li Kang,Hongyu Liu,Huijun He,Chunping Yang
Cost-effective removal of refractory sulfur-containing compounds from oils is still a challenge. In this paper, a novel catalyst of molybdenum supported on Ti-pillared interlayer clay (Ti-PILC) was successfully prepared which performed well in oxidative desulfurization (ODS) with cyclohexanone peroxide (CYHPO) as oxidant under mild conditions. Performance of catalytic oxidation and removal of oxidation product were also studied. The oxidation rate of dibenzothiophene (DBT) reached 99.90% under the optimum reaction conditions. Mo/Ti-PILC catalyst showed higher activity than Mo/Na-MMT in ODS not only due to the pillared interlayer structure which contributed to better molybdenum dispersion and faster diffusion of reactants, but also the catalytic activity of titanium in the oxidative desulfurization of DBT. Oxidative product of sulfone which appeared as crystal in the model oil was filtered and sulfur concentration was reduced to below 10 mg/L. Catalytic activity would be almost unaffected after regenerating for 9 times, and the leaching of active species did not appear in the leaching experiment of the catalyst, which proved that it was real heterogeneous catalysis. Besides, kinetics data conformed to the pseudo-first-order equation pretty well. These results indicated that this desulfurization system was cost-effective for the removal of DBT from oils.
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