Small Structures
·
2022
·Vol. 4
·期 1
·2200161
·
IF 11.343
Lu Chen,Youbing Li,Ke Chen,Xiaojing Bai,Mian Li,Shiyu Du,Zhifang Chai,Qing Huang
Entropy stabilization is an effective method to design and explore MAX phases with outstanding properties via tuning constituent elements and crystal structures, which have received considerable critical attention. Currently, some medium-/high-entropy (ME/HE) MAX phases, whose A layers are composed of Al, S, and magnetic elements, are reported, while few discussions about ME/HE-MAX phases with other A elements (e.g., Sn) are conducted. Herein, fully dense ME/HE-MAX phase bulks ((TiVNb) 2 SnC, (TiVNbZr) 2 SnC, and (TiVNbZrHf) 2 SnC) are designed and synthesized because of the chemical diversity of MAX phases. The results of Rietveld refinement of X-ray diffraction, scanning electron microscopy, and high-resolution scanning transmission electron microscopy-affiliated energy-dispersive spectrometer analysis comprehensively verify the crystal structure of ME/HE-MAX phases. Both the electrical conductivity and the charge carrier mobility are significantly lower than the reported correlation ternary MAX phases, due to the electron scattering and structural defects in ME/HE-MAX phase crystal structures. Similarly, the electron contribution of thermal conductivity is gradually declining; on the contrary, the phonon plays an increasingly dominant role as temperature increases. Owing to the richness in composition of MAX phases, herein, a composition design route for discovering new MAX phases and tuning their properties is indicated.
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MATERIALS SCIENCE AND ENGINEERING A-STRUCTURAL MATERIALS PROPERTIES MICROSTRUCTURE AND PROCESSING
·
2022
·
IF 6.044
Hao Wang,Fei Chen,Jiahao Zhao,Yaojun Lin,Qiang Shen
This paper presents a method of dealloying combined molten salt electrolysis (MSE) to prepare porous Ti alloy. The oxidation produced in dealloying process can be reduced efficiently by MSE. Meanwhile, the grain grew and the second phase of acicular nanocrystals was precipitated to enhance the mechanical properties during MSE process.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
·
IF 7.312
Guanglai Mo,Linxi Wang,Jianhong Luo
It is a challenge to achieve efficient photocatalytic activity of pure MOFs. Herein, the defective NH 2 -MIL-125(Ti) with adjustable linker vacancy level was successfully created by thermal treatment. The band gaps of samples decreased and the more Ti-O clusters on the surface of the samples can be achieved as the time of thermal treatment increased from 0 to 500 min, both of which facilitated the photocatalytic activity for the reduction of Cr(VI). Moreover, the ligands from the surface to the inside of the samples were successively decarboxylated, resulting in the declined specific surface area and the increased proportion of mesoporous and the defect level. The moderate defect level in NH 2 -MIL-125(Ti) can be obtained as the time of thermal treatment was 300 min, which facilitated the separation of photogenerated charges, contributing to the highest photocatalytic activity for reduction of Cr(VI), which was 9.2 times than that of the initial MOFs. However, the excessive linker vacancy defect level in NH 2 -MIL-125(Ti) may result in the seriously affected crystal structure and the retarded separation of photogenerated charges.
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Materials Chemistry Frontiers
·
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
·
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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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
·
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
·
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
·
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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