ANALYTICAL AND BIOANALYTICAL CHEMISTRY
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2023
·Vol. 415
·期 19
·4767-4777
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IF 4.3
Zhou Xiaoyu,Zhang Hongyan,Wang Li,Wu Ren’an
The HILIC enrichment is a greatly compatible strategy for the extraction of glycopeptides in proteomics. Herein, a boric acid and fructose-1,6-diphosphate (FDP) dual-functionalized Zr-based metal–organic framework material UIO-PBA&FDP (UIO is the abbreviation for the University of Oslo, and PBA is the abbreviation for carboxy phenylboronic acid) was synthesized, characterized with the desirable excellent hydrophilicity and thus was explored for the enrichment of N-linked glycopeptides utilizing the HILIC interaction between the glycopeptides and the hydrophilic UIO-PBA&FDP at a high level of ACN concentration. A total of 359 N-linked glycopeptides corresponding to 104 glycoproteins were identified from only 1 μL of digested human serum by the enrichment of UIO-PBA&FDP, which showed a superiorly high coverage of the identified glycopeptides. The dual hydrophilic functionalized UIO-PBA&FDP could be an efficient HILIC material for the enrichment of N-linked glycopeptides from complex biological samples.
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高影响因子
Advanced Science
·
2023
·Vol. 10
·期 10
·2206877
·
IF 15.1
Lu Chen,Youbing Li,Biao Zhao,Shanshan Liu,Huibin Zhang,Ke Chen,Mian Li,Shiyu Du,Faxian Xiu,Renchao Che,Zhifang Chai,Qing Huang
Electromagnetic (EM) wave pollution is harmful to human health and environment, thus it is absolutely important to develop new electromagnetic wave absorbing materials. MAX phases have been attracted more attention as a potential candidate for electromagnetic wave absorbing materials due to their high conductivity and nanolaminated structure. Herein, two new magnetic MAX phases with multiprincipal elements ((Ti 1/3 Nb 1/3 Ta 1/3 ) 2 FeC and (Ti 0.2 V 0.2 Nb 0.2 Ta 0.2 Zr 0.2 ) 2 FeC) in which Fe atoms replace Al atoms in the A sites are successfully synthesized by an isomorphous replacement reaction of multiprincipal (Ti 1/3 Nb 1/3 Ta 1/3 ) 2 AlC and (Ti 0.2 V 0.2 Nb 0.2 Ta 0.2 Zr 0.2 ) 2 AlC MAX phases with Lewis acid salt (FeCl 2 ). (Ti 1/3 Nb 1/3 Ta 1/3 ) 2 FeC and (Ti 0.2 V 0.2 Nb 0.2 Ta 0.2 Zr 0.2 ) 2 FeC exhibit ferromagnetic behavior, and the Curie temperature ( T c ) are 302 and 235 K, respectively. The dual electromagnetic absorption mechanisms that include dielectric and magnetic loss, which is realized in these multiprincipal MAX phases. The minimum reflection loss (RL) of (Ti 1/3 Nb 1/3 Ta 1/3 ) 2 FeC is −44.4 dB at 6.56 GHz with 3 mm thickness, and the effective bandwidth is 2.48 GHz. Additionally, the electromagnetic wave absorption properties of the magnetic MAX phases indicate that magnetic loss also plays an important role besides dielectric loss. This work shows a promising composition-design strategy to develop MAX phases with good EM wave absorption performance via simultaneously regulating dielectric and magnetic loss together.
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JOURNAL OF MOLECULAR STRUCTURE
·
2022
·
IF 3.841
Wei Qin,Xue Han,Junwei Wang,Xie Wang,Jianli Zhang
To design some excellent extractants for the separation of Zr(Ⅳ) and Hf(Ⅳ), a novel set of polyamidoamine dendrimers peripherally modified with salicylaldehyde (Abbreviated as PAMAM-SA) have been synthesized. UV-vis absorption and fluorescent spectrometry were used to study the selectivity of G.1.0, G2.0, G3.0 and G4.0 PAMAM-SA on Zr(Ⅳ) and Hf(Ⅳ) compared with other metal ions, and their extraction/separation performance on Zr(Ⅳ) and Hf(Ⅳ) was also investigated under different pH solutions. The results show that these dendrimers have superior selectivity on Zr(Ⅳ) and Hf(Ⅳ) as compared with Ca 2+ , Mg 2+ , Fe 3+ and Ni 2+ ions. The binding stoichiometry of G1.0, G2.0, G3.0 and G4.0 PAMAM-SA dendrimers with Zr(Ⅳ) is 1:4, 1:8, 1:10, 1:16 molar ratio determined by fluorescent titration respectively and the molar ratio of these dendrimers with hafnium is similar to that of zirconium. Both of the maximum extraction efficiency (EE%) on Zr(Ⅳ) and the separation coefficient (β Zr/Hf ) are following the order of G2.0-PAMAM-SA > G1.0-PAMAM-SA > G3.0-PAMAM-SA > G4.0-PAMAM-SA, and the maximum EE% on Zr(Ⅳ) is up to 98.9% and furthermore the β Zr/Hf is 1.52 for G2.0-PAMAM-SA at lower acid concentration compared with the reported extractants. The favorable higher EE% and β Zr/Hf indicate that G2.0-PAMAM-SA may be potentially employed as a highly selective and efficient extractant to enhance separating zirconium from hafnium.
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Journal of CO2 Utilization
·
2022
·
IF 8.321
Linmeng Huo,Lin Wang,Jingjie Li,Yanfeng Pu,Keng Xuan,Congzhen Qiao,Hao Yang
The disadvantage of Ce/Zr metal oxide as catalyst for direct synthesis dimethyl carbonate (DMC) from CO 2 and methanol is low DMC formation rate because of its low specific surface area and active sites. In this work, it can be improved by highly uniform dispersion cerium doped Zr-based metal-organic frameworks (UiO-66 MOFs), which were synthesized via a modified hydrothermal method. The as-prepared catalysts have been extensively characterized using XRD, BET, FT-IR, SEM, TEM, TGA, NH 3 -TPD, CO 2 -TPD, XPS techniques. Experimental evaluation results indicated that the highly uniform dispersed Ce-doped UiO-66 MOFs exhibited markedly improved catalytic performance than traditional Ce/Zr metal oxide catalyst. The highest yield of DMC catalyzed by Ce-UiO-66–2 was 0.295% (reaction time was 12 h; reaction temperature was 140 °C; reaction pressure was 11 MPa). Then, it was found that doping of Ce atoms into the zirconium lattice to produce UiO-66 MOFs could effectively increase the number of acidic and medium basic sites than UiO-66 (none Ce), thus could greatly enhance the catalytic performance. Moreover, using 2-cyanopyridine as dehydrating agent, the DMC yield could be further raised greatly. Last, based on reported literature and our results, a possible reaction mechanism over Ce-UiO-66-X was proposed.
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APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Juan Zhu,Shuang-Bao Li,Bao-Xu Jiang,Yu-Teng Zhang
Zirconium-based metal-organic polyhedra (ZrMOPs) have gained significant attention owing to their well-defined cavities, stability and potential applications. Herein, a novel composite membrane (PDA/ZrT-1-NH 2 /PVDF) was developed by incorporating amino-functionalized ZrMOP (ZrT-1-NH 2 ) into polydopamine (PDA) and trimesoyl chloride (TMC) cross-linking system. Notably, the cationic ZrT-1-NH 2 cages were immobilized onto the membrane surface by a simple vacuum filtration method, which thus endowed the surface positive charge for the membrane. A pre-prepared composite membrane was used to remove Cr(VI) from the wastewater. The effects of pH, contact time, initial Cr(VI) concentration, temperature, coexisting ions competition and reusability were investigated in batch experiments. The results revealed the as-prepared composite membrane exhibited high removal efficiency of 96.6 % for Cr(VI) ions within 5 min. In addition, the adsorption rate was very fast, reaching adsorption equilibrium in less than 30 min. Finally, a possible adsorption mechanism was proposed. The adsorption process was dominated by physical adsorption accompanied by a partial reduction of Cr(VI) to Cr(III).
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Small
·
2023
·Vol. 19
·期 45
·2304096
·
IF 13.3
Pei Jia,Qiushuang Wu,Boyang Sun,Li Wang
The elaborate defect-engineering of luminescent metal-organic frameworks (MOFs) allows them with enhanced sensing performance. A modulator-induced defect formation strategy is adopted in this paper, and the impact of the open-metal sites on sensing process is rationalized. It is demonstrated that the defect level can be tuned to a remarkable extent by controlling the amount of modulator. When a particular defect concentration is reached, the UiO-66-xFA can be acted as highly sensitive ratiometric fluorescence probes for chlortetracycline (CTE) determination with an ultralow detection limit of 9.9 n m . Furthermore, by virtue of the obvious variation in fluorescence chromaticity of probes from blue to yellow, a sensory hydrogels-based smartphone platform is proposed for visible quantitation of CTE by identifying the RGB values. A delicate device integrated with UV lamp and dark cavity has been developed for avoiding inconsistencies of ambient light and visual errors. Finally, the sensor obtains satisfactory results in the detection of actual seafood samples, with no significant differences from those of liquid chromatography−mass spectrometry. This approach anticipates a novel route to sensitize optical sensors through the design and synthesis of moderate defects in luminescent MOFs.
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RENEWABLE ENERGY
·
2023
·
IF 8.7
Hewei Yu,Jichao Sun,Xiuxiu Chen,Bing Wang,Xiaohui Liang,Mingjie Gao,Hongyu Si
A novel acid-base bifunctional Zn/Ca–Zr catalyst has been synthesized successfully for biodiesel production from palm oil and acidified oil. The influence of synthetic factors on the catalytic activity of resulting Zn/Ca–Zr were discussed. Furthermore, the FAMEs yield was optimized to achieve the maximum value using the Taguchi approach. Results showed that the catalyst synthesized using a metal stoichiometric ratio of 4 : 4: 4, hydrothermal conditions, and activation temperature of 850 °C exhibited the best activity. The highest FAMEs yield was found to be 94.9% under the conditions of 5 wt% catalyst dosage, methanol/palm oil molar ratio of 20, and temperature of 170 °C at 3 h. The contribution percentage indicated that the methanol/oil molar ratio had the most significant effect on the FAMEs yield. Moreover, the Zn/Ca–Zr catalyst can catalyze the simultaneous esterification and transesterification of acidified palm oil with a 95.1% FAMEs yield and 93.3% acid reduction rate. And a 78.2% FAMEs yield can be maintained after four repeated cycles. Molecular simulations indicated the active site of Zn was more easily attacked by FFAs for esterification, while the active site of Ca was retained to adsorb methanol for transesterification, which explained the catalyst's acid-base bifunctional characteristics.
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ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Jing Liu,Heguo Li,Bin Yan,Chao Zhong,Yue Zhao,Xuan Guo,Jinyi Zhong
Developing high-performance protective materials is important for soldiers and civilians who are exposed to the atmosphere of highly toxic chemical warfare agents (CWAs). Polyelectrolyte membranes are promising candidates with excellent chemical resistance and moisture permeability, but they cannot efficiently degrade CWAs. Here, we design and prepare a hybrid membrane through in situ growth of catalytically active zirconium-based metal–organic frameworks (Zr-MOFs) on a polyelectrolyte membrane mediated by biofilm-inspired curli nanofibers (CNFs). Superior to the bare polyelectrolyte membrane, the prepared MOF-808@CNF-PQ hybrid membrane exhibits improved rejection of the nerve agent simulant dimethyl methyl phosphonate (DMMP) vapor and permeation of the water vapor by 113 and 45%, respectively. The water/DMMP selectivity of the hybrid membrane reaches 498.6, approximately 13 times that of the commercial polyelectrolyte membrane Nafion 117. In addition, the hybrid membrane possesses appreciable catalytic activity for the hydrolysis of the nerve agent simulant dimethyl 4-nitrophenyl phosphate (DMNP) with a half-life of ∼38 min. Nanomechanical characterization results based on atomic force microscopy (AFM) techniques demonstrate the critical role of CNFs in mediating Zr-MOF nucleation and the dominant effect of electrostatic interactions on self-assembly of CNFs on polyelectrolyte base. It is also confirmed that the Zr-MOF toppings serve as the key components in physically adsorbing and chemically degrading the DMNP molecules through multiple strong intermolecular interactions. Our work offers a rational strategy to develop advanced membranes toward efficient chemical protection, moisture permeation, and catalytic detoxification against CWAs.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2022
·
IF 5.876
Yanghuan Huang,Haocheng Zhang,Lou Gao,Tianlan Yan,Yueer Yan,Yahong Zhang,Yi Tang
A series of Zr–Al-MWW zeolites with different Zr state and layer-stacking structure are successfully synthesized via direct grafting zirconocene dichloride onto the external silanols of three kinds of MWW zeolites, i.e. MCM-22 with multilayered structure, ITQ-2 (through layer delaminated route) and OL-MWW (by direct hydrothermal synthesis) with oligolayered structure. The structure, porosity and state of grafted Zr species are distinctly different among the three Zr–Al-MWW zeolites. Zr-OL-MWW possesses the highest content of single Zr atoms with an ideal micro-meso-macro pore system, while Zr-MCM-22 and Zr-ITQ-2 contain two kinds of Zr species (ZrO 2 clusters and single Zr atoms) coexisting in various proportions. The high dispersion of single Zr atoms on OL-MWW can be assigned to the large amount of external silanols of OL-MWW. The as-prepared three bi-functional Zr–Al-MWW zeolites are used for the cascade Meerwein-Ponndorf-Verley (MPV) reduction and etherification (ETH) reaction. Among them, Zr-OL-MWW shows dramatically higher conversion of cinnamaldehyde and yield of 1-cinnamyl 2-propyl ether than Zr-MCM-22 and Zr-ITQ-2, owing to the higher catalytic activity of Lewis acid centers from single Zr atoms, as well as more integrated framework Al sites as Brønsted acid centers with good accessibility. This study offers a simple and efficient strategy to construct Lewis-Brønsted acidic zeolites with exposed heteroatom sites and integrated framework structure, which will provide especial potential in the catalytic conversion of macromolecules.
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FUEL
·
2022
·
IF 8.035
Qiuju Fu,Dandan Liu,Weijing Niu,Shuo Zhang,Ruihua Chen,Yujia Wang,Pengze Zhao,Huimin Jiang,Yanchao Zhao,Lingzhi Yang,Liting Yan,Haiyan Wang,Xuebo Zhao
The highly efficient production of furfuryl alcohol (FFA) from biomass-derived furfural (FFR) is attracting increasing attention due to its wide application in the production of value-added chemicals. Zr-based MOF-808 is promising for liquid catalytic transfer hydrogenation (CTH) of FFR to FFA in terms of possessing a great number of Lewis-acid sites. Herein, a series of defective MOF-808 (D x -MOF-808) samples were prepared via a competitive coordination-removal strategy by modulating with benzoic acid (HBC). HBC was introduced as the temporary ligand for competing with formal ligand 1,3,5-benzenetricarboxylic acid (H 3 BTC) to coordinate with metal clusters and then it was removed with methanol to obtain the D x -MOF-808. The results showed that HBC serves not only as a temporary ligand participating in the synthesis of MOF-808 to obtain defective structure but also as a modulator controlling the particle size by terminating the growth of crystals. By changing the amount of HBC addition, the degree of ligand deficiency and the number of exposed Zr sites can be well regulated. Especially, excellent performance of FFR conversion (99%), FFA selectivity (94.4%) and FFA formation rate (48.6 mmol·g −1 ·h −1 ) was achieved over D 40 -MOF-808 sample with 2-propanol as a hydrogen donor under mild conditions (90 °C, 2 h), ranking it the best among the reported catalysts. Detailed characterizations proved that the high activity of D 40 -MOF-808 was jointly influenced by the high surface area, the high content of exposed Zr metal sites and ligand deficiency.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
IF 6.371
Qiong Li,Hao Qian,Tianyang Zheng,Xiaoyuan Sun,Yunfei Liu,Yinong Lyu
The cation displacement closely related to the local symmetry and corner-connected oxygen octahedral rotation are the structural origin of macroscopic properties in ABO 3 perovskite oxides. This work describes in detail the relationship between microstructure and macroscopic properties in 0.78BT-0.12CT-0.1BZS ceramic, which achieves the enhanced strain of 0.19 % with a hysteresis of 6.56 %. The atomic level structure is revealed by aberration corrected scanning transmission electron microscope (AC-STEM). The AC-STEM HAADF images reveal the coexisting of polar nanoregions with O and T symmetries. Such a microstructure has a lower energy barrier, facilitating dynamic polarization rotation flexibly under external stimuli. The AC-STEM ABF image reveals the existence of the BO 6 octahedral rotation, with rotation patterns of the a 0 b 0 c 0 and a - b + c - , and rotation angles are quantitatively measured. The BO 6 octahedral rotation and cation displacement are found to be consistent, the greater octahedral rotation with greater cation displacements. These results have important implications for understanding the structural origin of the excellent properties in ferroelectrics .
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Li Xia,Wenxi Zhou,Yifan Xu,Zhengqiang Xia,Xinzhi Wang,Qi Yang,Gang Xie,Sanping Chen,Shengli Gao
The introduction of rich-electron ligands is a promising strategy to improve the ligand-to-metal charge transfer (LMCT) ability of metal–organic frameworks (MOFs) for efficient photocatalytic CO 2 reduction reactions (CO 2 RR), while the resulting impaired Lewis acid sites go against stable bonding with CO 2 and hinder the electron transfering to CO 2 . It is thus the key to search a trade-off between increasing LMCT and frustrating Lewis acid. Herein, the ferrocene (Fc) modified UiO-66 series MOFs, NH 2 -UiO-66-Fc, have been prepared to optimize LMCT for boosting CO 2 RR through a simple solvent-assisted ligand incorporation (SALI) method. Theoretical calculation and systematic experiments, including photoelectrochemical measures, in situ electron paramagnetic resonance, fluorescence probe analysis and X-ray photoelectron spectroscopy indicate that with increasing Fc content, the LMCT energy of MOFs significantly decreases from 2.66 to 2.10 eV based on the established electron transfer double-channel mechanism, while the Lewis acidity of Zr sites reduces with the CO 2 adsorption energy ( E ad ) ranging from −1.061 to −0.632 eV. Through introducing an optimal Fc content, NH 2 -UiO-66-Fc (2.0) integrating satisfactory LMCT ability and Lewis acidity shows superior photocatalytic CO 2 RR performance (CO yield: 90.65 μmol·g −1 ·h −1 ), about 13 times higher than that of the unmodified MOF and superior to most reported pristine MOF photocatalysts. DFT calculation demonstrates that the excellent performance of NH 2 -UiO-66-Fc (2.0) is attributed to the lowest energy barrier of 1.50 eV for the rate-limiting step of *COOH formation. In this work, such a simple post-modification strategy for facilitating the whole electron transfer path of photocatalytic CO 2 RR will provide a new way to construct high-performance MOFs-based CO 2 RR photocatalysts.
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