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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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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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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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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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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SEPARATION AND PURIFICATION TECHNOLOGY
·
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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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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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2018
·Vol. 29
·期 20
·17571-17579
·
IF 2.324
Zhong Canyu,Lai Qi,Liao Xianjie,Li Yufeng,Wu Jinggao
Porous Ti-doped MoO 2 was successfully synthesized through one-pot hydrothermal method and used as an anode material for lithium ion batteries (LIBs). It delivers an initial discharge capacity of 1290 and 410 mAh/g at current density of 20 and 1000 mA/g, respectively. Electrochemical cycle test shows that the discharge capacity of 740 mAh/g can be obtained after 80 cycles at current density of 200 mA/g, with 78.06% capacity retention and almost 100% columbic efficiency. The electrochemical performances are much better than that of other MoO 2 -based materials. This could be assigned to the porous structure that increased contact areas between electrode materials and electrolytes, much faster electron transport confirmed via electrochemical impedance spectroscopy (EIS) analysis and Density functional theory (DFT) calculations.
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ACS Applied Materials & Interfaces
·
2018
·
IF 8.097
Jin-Feng Liao,Yang-Fan Xu,Xu-Dong Wang,Hong-Yan Chen,Dai-Bin Kuang
Though coating CsPbBr3 nanocrystal (NC) with an outer layer has been regarded as an effective strategy to address its instability issues, deep investigations into the electronic interaction between CsPbBr3 NC and coating layer have yet to be conducted. In this study, the dynamics of hot carrier and charge carrier of CsPbBr3 nanocrystal with various MO2 (M = Si, Ti, Sn) coating layers have been comprehensively studied. Combined transient optical characterizations (time-resolved photoluminescence and ultrafast transient absorption) and photoelectrochemical measurements reveal that coating with insulating SiO2 accelerates the hot carrier relaxation and enhances the radiative recombination by passivating surface traps, whereas efficient charge-carrier separation and extraction are observed after coating with SnO2 and TiO2. The electron injection from CsPbBr3 NC to SnO2 (1.14 × 108 s–1) is 2-fold faster than to TiO2 (5.4 × 107 s–1) owing to the lower conduction band edge and the higher electron mobility of SnO2. Particularly, the first time fabricated CsPbBr3 NC/SnO2 composite exhibits superior stability against UV light and moisture, as well as the best photocurrent response in this study. This work has implied that rational design of the coating layer for perovskite NC can not only improve the stability but also tailor the electronic and optoelectronic properties for various applications.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2019
·
IF 3.375
Yunpeng Hu,Kai Wang,Chunli Han,Tao Wang,Guangsheng Luo
A novel liquid–liquid microdispersion method for the synthesis of TS-1 has been developed by continuous preparation of the precursor. In the novel process, the solution of TBOT in n-hexane could be very uniformly dispersed into the oligomeric silicate prehydrolysis mixture to form microdroplets by a microsieve pore reactor. Due to the fast mixing and very high mass transfer performance of the microdispersion process, the Ti species could be uniformly distributed into the mixture and were more likely to condense into the oligomeric silicate precursor species rather than appear with self-condensation. The prepared samples had a minimum molar ratio of Si/Ti at 51 without extra-framework Ti species. Furthermore, the solvent of n-hexane can be recycled by simple phase separation rather than evaporation under the conditions of using isopropanol, which reduced energy consumption. This continuous microdispersion technology could be controllable and a reliable scaling-up for the preparation of TS-1.
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APPLIED ORGANOMETALLIC CHEMISTRY
·
2014
·Vol. 29
·期 1
·12-19
·
IF 2.017
Hongxu Guo,Fan Lin,Jianhua Chen,Feiming Li,Wen Weng
A metal–organic framework material, MIL-125(Ti), was solvothermally prepared and characterized using X-ray diffraction, scanning electron microscopy, Fourier transform infrared spectroscopy and surface area measurements. MIL-125(Ti) was then used as an adsorbent for Rhodamine B (RhB) removal in aqueous solution. The adsorption kinetics, adsorption mechanism, adsorption isotherm, activation energy and various thermodynamic parameters were studied in detail. The maximum adsorption capacity of MIL-125(Ti) for RhB was 59.92 mg g −1 . MIL-125(Ti) appears to be a promising material for RhB adsorption from aqueous solutions. Copyright © 2014 John Wiley & Sons, Ltd.
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JOURNAL OF MATERIALS SCIENCE
·
2015
·Vol. 50
·期 15
·5307-5317
·
IF 2.371
Lin Yuqing,Cai Yuanyuan,Qiu Minghui,Drioli Enrico,Fan Yiqun
A new aqueous sol was synthesized to prepare Ag-doped TiO 2 /Ti composite tight ultrafiltration (UF) membranes. This sol was prepared based on water (>95 wt%), for which the hydrodynamic size of 8 nm could be obtained by tuning the electrostatic and steric repulsive forces, breaking the limit of the polymeric sol–gel method to prepare tight UF membranes. For the preparation of the sol, high water content can significantly reduce the use of organic solvents and is more environment-benign. Moreover, Ag doping can considerably improve the toughness of the supported membranes to efficiently prevent the TiO 2 /Ti composite membranes from cracking and overcome the thermal expansion mismatch of ceramic membranes and their metallic supports. The prepared Ag-doped TiO 2 /Ti composite membranes presented a molecular weight cut-off of 3 kDa with a pure water flux of 24 L m −2 h −1 bar −1 and exhibited good dye removal capabilities. The proposed Ag doping method has considerable potential for the fabrication of integrated hybrid ceramic–metallic composite membranes.
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