Materials Chemistry Frontiers
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2021
·Vol. 5
·期 16
·6101-6113
·
IF 6.482
Haikuo Ma,Haoyi Lin,Xiuquan Liu,Hongying Lü,Zhiguo Zhu
Fabricating hierarchical porosity in a metallosilicate zeolite crystal is a facile and efficient approach to increase the accessibility of active sites and to enhance the diffusion performance in the process of catalytic reactions, particularly those involving bulky guest organics. The straightforward and efficient synthesis of hierarchical metallosilicate zeolites was intensively limited by the high-cost mesoporogen, complicated and tedious synthesis procedures, broad mesoporous size distribution, restricted zeolite topologies, and low solid yield. Herein, an innovative hydrothermal synthesis methodology of a hierarchical heteroatom-containing zeolite, in this case of Ti-Beta, via in situ structural reconstruction was proposed. Tetraethylammonium hydroxide (TEAOH) played significant roles of not only as base source, functioning etching effect, but also as structure directing agent (SDA), reconstructing the framework structure in this hydrothermal synthesis. The mesoporosity and Ti4+ species coordinate state could be regulated by varying the TEAOH content, which was closely related to the catalytic activity in oxidative desulfurization. The optimal hierarchical Ti-Beta zeolite with a mesopore size of 7.8 nm and a high solid yield of more than 96% exhibited outstanding catalytic oxidation performance, far outperforming the hydrothermally synthesized Ti-Beta zeolite and postsynthesized Ti-Beta zeolite. This work provides a straightforward and facile methodology for rationally constructing the hierarchical Ti-Beta zeolite, which is promising to be an extension to synthesize other hierarchical heteroatom-containing zeolites without the assistance of a mesoporogen in a short time.
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MICROCHIMICA ACTA
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2021
·Vol. 188
·期 2
·1-11
·
IF 5.833
Liu Bin,Wang Baichun,Yan Yinghua,Tang Keqi,Ding Chuan-Fan
A strategy for effectively enriching global phosphopeptides was successfully developed by using ammonia methyl phosphate (APA) as a novel chelating ligand and Ti 4+ and Nb 5+ as double functional ions (referred to as Fe 3 O 4 @mSiO 2 @APA@Ti 4+ /Nb 5+ ). With the advantage of large specific surface area (151.1 m 2 /g), preeminent immobilized ability for metal ions (about 8% of total atoms), and unbiased enrichment towards phosphopeptides, Fe 3 O 4 @mSiO 2 @APA@Ti 4+ /Nb 5+ displays high selectivity (maximum mass ratio β-casein to BSA is 1:1500), low limit of detection (LOD, as low as 0.05 fmol), good relative standard deviation (RSD, lower than 7%), recovery rate of 87% ( 18 O isotope labeling method), outstanding phosphopeptide loading capacity (330 μg/mg), and at least five times re-use abilities. In the examination of the actual sample, 24 phosphopeptides were successfully detected in saliva and 4 phosphopeptides were also selectively extracted from human serum. All experiments have shown that Fe 3 O 4 @mSiO 2 @APA@Ti 4+ /Nb 5+ exhibits exciting potential in view of the challenge of low abundance of phosphopeptides.
Graphical abstract
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PubMed
高影响因子
POLYHEDRON
·
2020
·
IF 2.343
Zhongmin Liu,Cong Wang,Yongchuan Wu,Longlong Geng,Xiuling Zhang,Dashuai Zhang,Hui Hu,Yongzheng Zhang,Xin Li,Wei Liu,Ping Na
The adsorption behavior of arsenic on adsorbent have been researched widely, but chemical adsorption of arsenic is uncommon. In this work, a kind of microporous metal-organic framework (MIL-125(Ti)) with columnar morphology and uniform size was solvothermally synthesized, and its chemical adsorption behavior and mechanism of arsenic were firstly investigated by experimental and simulation study. Remarkably, ultra-fast adsorption behavior and excellent arsenic removal capability was achieved. It takes only 20 min to rapidly remove 5 mg L −1 arsenic with 0.2 g L −1 MIL-125(Ti), which is far superior to the previously reported materials. Both experimental and simulation study results show that the adsorption of arsenic obeys a new chemical adsorption mechanism. Both As(III) and As(V) can easily replace the terephthalic acid ligand via competitive coordination and bind to the Ti active site of MIL-125(Ti). In addition, the reaction energy barriers for ligand substitution by H 2 O, As(III) and As(V) are 0.46, 0.33 and 0.15 eV, respectively, which further confirming that structure reforming of MIL-125(Ti) plays a key role for chemical adsorption. The study solves the difficulty of removing low concentration of arsenic and provides molecular-level understanding of the chemical adsorption mechanism of arsenic on MIL-125(Ti).
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Catalysts
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2020
·Vol. 11
·期 1
·24
·
IF 3.52
Juan Du,Jiaxin Zhang,Tingyu Yang,Renming Liu,Zhiyi Li,Dandan Wang,Tong Zhou,Yucun Liu,Chunbo Liu,Guangbo Che
The BiOI/NH2-MIL-125(Ti) composite photocatalyst with excellent photocatalytic performance was prepared by the solvothermal method. For the BiOI/NH2-MIL-125(Ti) (BNMT) system, the contents of NH2-MIL-125(Ti) in BNMT-4, BNMT-5, BNMT-7, BNMT-9, and BNMT-10 were 4 wt %, 5 wt %, 7 wt %, 9 wt %, and 10 wt %, respectively. XRD, XPS, SEM, and TEM characterizations indicated that BiOI/NH2-MIL-125(Ti) was successfully prepared. Brunauer, Emmett, and Teller (BET) and UV–vis diffuse reflectance spectra photoelectrochemical analysis indicated that BNMT-9 can make the specific surface area and photo absorption region larger than BiOI. In addition, the separation efficiency of photogenerated carriers was improved, and the recombination efficiency was reduced. The degradation percentages of Rhodamine B (RhB) and p-chlorophenol (P-CP) reached 99% and 90% over BNMT-9 under visible light irradiation. Additionally, the catalysts had high stability. The results of the active spices trapping experiments test indicated that h+was the main active species. The possible degradation mechanism was proposed.Keywords:photocatalysis;BiOI;NH2-MIL-125(Ti);organic pollutants
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JOURNAL OF ALLOYS AND COMPOUNDS
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2020
·
IF 4.65
X.Q. Liu,C.J. Li,X. You,Z.Y. Xu,X. Li,R. Bao,J.M. Tao,J.H. Yi
Carbon nanotube reinforced aluminum matrix (CNT/Al) composites with various microstructures were fabricated by powder metallurgy via introducing nano-sized and micron-sized Ti powders into the CNT-Al system. The size-dependent effects of Ti powders on the microstructure evolution and mechanical properties were further investigated. The results reveal that the best enhancement (∼51% of UTS) was obtained by adding 80 nm sized Ti powders into the CNT/Al composite compared with the composite without Ti addition, which mainly derives from the synergistic strengthening of the homogenously dispersed CNTs, a large quantity of in-situ formed nano-sized TiAl 3 particles and fine grains. Meanwhile, it is also noted that the addition of micron-sized Ti powders can help the CNT dispersion in powder fabrication stage, and subsequently in-situ formed core-shell structured particles with different interface reaction degree in the Al matrix. Among them, 1 μm was determined to be the optimal size of Ti for the maximum formation of core-shell structured particles, which best exploits the load transfer ability of TiAl 3 shell layers at their interfaces, and finally attributes to significant strength enhancement (∼35% of UTS). This research provides a valuable reference concerning the size effects of addition metal in future fabrication of CNTs reinforced metal matrix composites with alternative microstructure.
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ANALYST
·
2020
·Vol. 145
·期 12
·4341-4351
·
IF 3.978
Fengjuan Ding,Yameng Zhao,Haiyan Liu,Weibing Zhang
Selective, sensitive and efficient phosphopeptide enrichment is significant in understanding phosphorylation-regulated processes and finding potential biomarkers. Magnetic materials have significant advantages for the separation and enrichment of modified peptides and proteins. In this work, we fabricated a core–shell magnetic Ti4+-functionalized covalent organic framework composite (denoted as Fe3O4@SiO2@TpPa-Ti4+) to selectively capture phosphopeptides in biosamples. The specific porous structure makes high surface area, which provides space and more affinity sites to binding titanium ions. The loading capacity of titanium ions was as high as 14% (wt%). Calculated by the MS results of α-casein tryptic digests, the binding capability could reach 200 mg g−1. Fe3O4@SiO2@TpPa-Ti4+ nanoparticles also demonstrate high sensitivity (above 0.2 fmol μL−1) and selectivity (α-casein : BSA = 1 : 5000). 1083 phosphopeptides were identified within two LC-MS/MS replicates with 91.8% specificity (phosphopeptides/all identified peptides). These MS results demonstrate that with the aid of the magnet, this method based on the magnetic titanium-functionalized covalent organic framework composite is applicable to achieve rapid, selective and efficient phosphopeptide analysis.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Ming Zhou,Xiao Ma,Cuiyue Ji,Lekai Zhao,Jiahao Chen,Yongdong Shi,Delong Liu,Zhaoxiang Zhong,Ze-Xian Low,Weihong Xing
Creating adsorbents that exhibit high selectivity towards pollutants, can be readily regenerated, and maintain high stability, remains a crucial challenge in water treatment technology. Herein, we present a magnetically and chemically recoverable absorbent based on Ti and Co co-substituted LaFeO 3 (La 0.9 Fe 0.55 Ti 0.3 Co 0.15 O 3 , LFTCO) with significantly enhanced adsorption properties. Notably, LFTCO exhibits a methyl blue adsorption capacity (q max ) of 2131 mg/g, setting a new record among perovskite oxides, due to the increased surface oxygen vacancy with the dual doping strategy. The selected dual-dopant consists of Fenton active Co and spin-state interactive Ti, which allows creating more oxygen vacancy and simultaneously facilitating pragmatic regeneration of the adsorbent. The new LFTCO exhibits significantly enhanced ferromagnetism (M = 7.27 emu/g), enabling rapid magnetic separation from water and subsequent Fenton-based regeneration step. We also reveal that the anchored configuration of SO 3 -defect site, through density functional theory (DFT) calculation, as the most favorable site for the adsorption process. These findings provide a pathway to creating high-performance adsorbents and shed light on the mechanistic understanding of LFTCO's enhanced adsorption properties.
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Journal of Environmental Chemical Engineering
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2023
·
IF 7.7
Zi-Ying Zeng,Dong-Dong Zhou,Shu-Tong Yang,Miao-Miao Su,Zhong-Hua Yang
This work synthesized a novel adsorbent by doping COF and MIL-125(Ti) in the nanoparticles Fe 3 O 4 . The obtained results showed that the doping of COF and MIL-125(Ti) had a positive effect on enhancing the specific surface area and adsorption capacity. Moreover, the adsorption process has been confirmed to follow the Langmuir model and pseudo-second-order kinetic, and the maximum adsorption capacity for tetracycline and tebuconazole was 138.1 mg/g and 87.73 mg/g, respectively. Finally, the adsorbent displayed an excellent adsorption performance in three kinds of actual environmental water samples. The mechanics of the adsorption process mainly involved π-π stacking interaction, hydrogen-bonding interaction, electrostatic interaction, and complexation interaction. In short, the synthesized magnetic adsorbent displayed a good application potential for removing tetracycline and tebuconazole from wastewater.
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Catalysis Science & Technology
·
2023
·Vol. 13
·期 22
·6561-6569
·
IF 5
Songlei Mo,Yong Guo,Xiaohui Liu,Yanqin Wang
The glycolysis of polyethylene terephthalate (PET) is considered as the most promising PET recycling strategy due to its mild reaction conditions and circularity. Herein, several metal-doped SBA-15 (M/SBA-15) as heterogeneous Lewis acid catalysts were investigated to screen the best catalyst and to understand the essence for their differences in PET glycolysis. It is found that the catalytic activity is positively correlated with the acid amount in different metal-doped SBA-15 and Ti/SBA-15 with different Ti loadings, with the exception of Nb/SBA-15. 4Ti/SBA-15 with abundant Lewis acid sites shows excellent PET glycolysis ability, with the yield of bis(2-hydroxyethyl) terephthalate (BHET) reaching 87.2% within 45 min at 190 °C (isolated yield 73%). While 4Nb/SBA-15 has a similar acid amount as that in 4Ti/SBA-15, but it has very low catalytic activity probably due to its strong oxygen affinity. Acetone–methanol-adsorption DRIFTS confirms its strong oxygen affinity, which would poison the acid sites by ethylene glycol (EG) and result in very low activity. This study demonstrates that PET glycolysis activity is really correlated with the amount of Lewis acid sites, but species with very strong oxygen affinity would lower its activity. Further diffuse reflection ultraviolet-visible (DR UV-vis) spectra analysis confirms that tetrahedral Ti4+ species in Ti/SBA-15 is the real active center. In addition, 4Ti/SBA-15 has good reusability and can be used in common real PET (dyed polyester fabric, PET bottles) glycolysis. These results indicate that increasing the amount of Lewis acid sites is a promising way to enhance PET glycolysis and 4Ti/SBA-15 with high activity and stability is a potential catalyst for industrial application.
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JOURNAL OF MATERIALS SCIENCE
·
2023
·Vol. 58
·期 38
·15035-15046
·
IF 4.5
Wang Xiongwei,Ma Rui-Juan,Guo Tingyu,Zhang Xuewei,Wang Hui,Zhao Xu
Abstract The hydrogen iodide decomposition reaction of the sulfur-iodine (SI) cycle is realized by electrolysis at room temperature to achieve efficient hydrogen production, while iodine is recycled throughout the SI reaction. In this work, we report a facile hydrothermal method for the synthesis of sulfur-doped titanium dioxide (S- \(\hbox {TiO}_2\) ) nanosheets with evenly distributed on the Ti foil (S- \(\hbox {TiO}_2\) /Ti). The noble metal-free S- \(\hbox {TiO}_2\) /Ti electrode demonstrates excellent electrochemical catalytic performance for iodine evolution reaction. It can deliver a high current density of 100 mA/ \(\hbox {cm}^2\) with a potential of 1.05 V, which is close to 90% of that of precious metal platinum and 5.6 times of bare Ti foil. Furthermore, the S- \(\hbox {TiO}_2\) /Ti electrode is stable in a mixed acid solution of HI and \(\hbox {H}_2\hbox {SO}_4\) . Compared to \(\hbox {TiO}_2\) /Ti, diffuse reflectance spectroscopy and ultraviolet photoelectron spectroscopy analysis evidence a reduction in the band gap and work function of S- \(\hbox {TiO}_2\) /Ti due to the doping of sulfur. Correspondingly, the current efficiency approaches to 100% under the electrolysis constant voltage 1.30 V. Eventually, the detailed mechanism to describe the improvement of the electrocatalytic performance was suggested. Graphical abstract
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CERAMICS INTERNATIONAL
·
2023
·
IF 5.2
Zhangyi Huang,Zhengwei Zhu,Mingyu Su,Yang Shi,Mao Deng,Ruichong Chen,Zhijun Wang,Zhi Zhou,Jianqi Qi,Haomin Wang
This study investigated the high-temperature oxidation behaviors of TMC ceramics. The results indicate that the high-temperature oxidation curves of the four TMC ceramics follow a parabolic law, suggesting a diffusion-controlled process. The activation energies for the oxidation of TaC, NbC, TiC, and ZrC ceramics are 105.4, 124.3, 169.3, and 78.7 kJ/mol, respectively, with oxidation rate constants at 1000 °C of 16.84, 40.45, 0.18, and 14.43 mg 2 /cm 4 ·h for each ceramic, respectively. The temperatures at which the ceramics disintegrate into fragments in high-temperature air are 800, 800, >1000, and 600 °C, respectively. The anti-oxidation performance of the four TMC ceramics ranks as follows: TiC > TaC > NbC > ZrC. In comparison to the reported high-entropy carbide ceramics, the TiC ceramic in this study demonstrates superior anti-oxidation performance due to dense TiO 2 layer formation, characterized by significantly low oxidation rates and excellent structural stability.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
·
IF 4.2
Hui Qi,Lida Wang,Wen Sun,Zhengqing Yang,Xu Chen,Jiao Yu,Wenzheng Wu,Guichang Liu
Chlorine evolution anodes are widely used in industrial electrolysis, whose electrocatalytic activity and stability need to be improved urgently in order to improve energy efficiency. In this study, Ti/IrRuSnSbOx electrodes were fabricated by thermal decomposition of hydrosol precursor solution. The microstructure and electrochemical behavior of the electrodes were investigated by material characterization and electrochemical tests. The results showed that the electrode with a total oxide loading of 1.1 ± 0.5 mg/cm2 had the lowest chlorine evolution potential (1.068 V vs SCE), the lowest Tafel slope (41.08 mV dec–1), and a long accelerating lifetime (405 h). The hydrosol process effectively improved the performance of the electrode by promoting the formation of oxygen vacancies and strengthening the stability of the solid solution structure. This study provided a facile method for preparing chlorine evolution electrodes with low cost, high activity, and high stability.
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