JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Jiangyan Song,Yongyi Yu,Xiaoshuai Han,Weisen Yang,Wenbin Pan,Shaoju Jian,Gaigai Duan,Shaohua Jiang,Jiapeng Hu
Herein, we used a one-pot method to fabricate a novel MOF-on-MOF adsorbent, namely MOF(Zr)-on-MOF(Ce). The adsorbent demonstrated a high maximum fluoride-ions capture capacity of 164.47 mg g −1 . The morphology, elemental distribution, pore size distribution, and thermal stability were studied using SEM-EDS, XRD , BET, and TGA . The influence of the temperature, solution pH, fluoride concentration, and coexisting ions was explored using intermittent experiments. The results suggested that MOF(Zr)-on-MOF(Ce) had a fast capture rate for fluoride. MOF(Zr)-on-MOF(Ce) maintained an excellent fluoride removal performance over a wide pH range with an initial fluoride concentration of 20 mg L −1 . The optimal effect was obtained at a pH of 4, but a high removal efficiency of 94% was maintained even at a pH of 9. Interference experiments showed that only the PO 4 3– had an adverse inhibition influence. The field experiments demonstrated that MOF(Zr)-on-MOF(Ce) can keep the safety threshold levels of fluoride in drinking water . The Langmuir and pseudo-second order kinetic models were well fitted for the defluoridation process, demonstrating that the adsorption of fluoride ions on MOF(Zr)-on-MOF(Ce) was dominated by monolayer chemisorption . With the further characterization and kinetic thermodynamic studies indicates that the removal mechanism involves ion exchange, electrostatic interactions and complexation effect.
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Yue Yin,Ruolin Lv,Xiaoyang Li,Lu Lv,Weiming Zhang
Bimetallic Fenton catalyst has attracted widespread attention in refractory organics removal. Herein, we firstly investigated the influence of ZrO 2 structure features on H 2 O 2 activation in Zr-Fe bimetallic catalyst. The results show that the heterojunction structure will be formed after high temperature calcination , which makes the ability of Zr-Fe bimetallic catalyst to activate H 2 O 2 for bisphenol A degradation is 3.1 times higher than that of α-Fe 2 O 3 without Zr doping. Through characterization and density functional theory, it was identified that compared to (1 1 0) interface, the adsorption energy of H 2 O 2 on iron sites at (1 1 0)-(1 0 0) interface reduced by 1.27 kJ mol −1 , while the Fe–O bond length in the stable configuration of Fe-OOH increased by 0.16 Å, which was beneficial to the association and dissociation of H 2 O 2 on iron sites. Besides, the surface -OH of amorphous ZrO 2 in Zr-Fe bimetallic catalyst synthesized under low temperature conditions could promote HO 2 • /O 2 •- formation through the surface electron transfer, accelerating the Fe(III) reduction. In conclusion, this study reveals the influence of environment-friendly ZrO 2 structure features on H 2 O 2 activation, proposes a new insight into strengthening the synergistic effect between bimetals, and provides a reference for the structural optimization of bimetallic catalysts.
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2021
·
IF 8.198
Qiang Yu,Yonghua Guo,Xiaoxia Wu,Zijun Yang,Hua Wang,Qingfeng Ge,Xinli Zhu
Ketonization reactions provide a feasible approach to remove oxygen and increase carbon chain length for conversion of biomass derived carboxylic acids. However, the reaction suffers from fast catalyst deactivation and low ketone selectivity. In this work, Lewis acidic heteroatom Ti-, Zr-, Ce-, and Sn-Beta zeolites were prepared using a two-step post-synthesis method and applied in vapor phase ketonization of propionic acid at 350 °C. Among these zeolites, Zr-Beta shows both the highest activity and selectivity. Characterizations indicate that Zr prefers the vacant tetrahedral site when the Zr content is < 7%, corresponding to the maximal fraction of vacant sites produced from dealumination of the parent H-Beta with a Si/Al ratio of 19. Extraframework Zr may also form at a Zr content ≥ 7%. The tetrahedrally coordinated framework Zr species (mainly in the structure of open sites) show Lewis acidic characteristic, and their density can be linearly correlated with the ketonization activity, indicating that these sites are active sites for ketonization. In contrast to rapid deactivation of H-Beta, the 7% Zr-Beta is stable for ketonization over 60 h, maintaining a conversion of ∼50% and a 3-pentanone selectivity > 96% at a space time of 2 h. The amount of coke deposition on Zr-Beta is about 1/3 of that on H-Beta, and the structure of Zr-Beta is preserved after 60 h of reaction. The results of this work indicate that Zr-Beta zeolite is a promising catalyst for ketonization with good stability and high selectivity toward ketone.
✓ 已验证
产品关联
DOI
高影响因子
ANALYTICA CHIMICA ACTA
·
2020
·
IF 5.977
Linjie Wang,Zhi Hu,Shuwen Wu,Jianming Pan,Xuechao Xu,Xiangheng Niu
Phosphorylation is a common process for regulating protein functions. Studies have confirmed that many human diseases are associated with the abnormal phosphorylation of proteins. Hence, uncovering the phosphorylation state of proteins turns to be of much importance for biomedicine and clinical practice. In this work, we report a simple but efficient colorimetric sensor array for the quantification and identification of phosphorylated proteins by using a Zr-based MOF as a peroxidase mimic. Thanks to its unique dipyridyl-based ligands, the proposed MOF is able to exhibit favorable catalytic activity to stimulate the chromogenic reaction of H 2 O 2 and 3,3′,5,5′-tetramethylbenzidine. When phosphorylated proteins are in presence, they can anchor onto the nanozyme surface via the strong interaction between phosphate groups in proteins and Zr nodes in the MOF, resulting in the inhibition of the nanozyme’s activity and the suppression of the chromogenic reaction. Based on this principle, our colorimetric sensor array enabled the facile quantification of phosphorylated proteins. Given that proteins with different phosphorylation states would affect the catalytic activity of the MOF nanozyme in different degrees, we further integrated the array with principal component analysis for the successful identification of phosphorylated and non-phosphorylated proteins.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Inorganic Chemistry Frontiers
·
2021
·Vol. 8
·期 24
·5186-5194
·
IF 6.569
Yan Zhang,Yanjie Liang,Shihai Miao,Dongxun Chen,Shao Yan,Jingwei Liu
A series of Cr3+-doped BaMSi3O9 (M = Zr, Sn, Hf) near-infrared emitting phosphors with tunable luminescence properties have been successfully synthesized by using a simple solid-state reaction method. The developed BaMSi3O9:Cr3+ phosphors show a broad near-infrared emission band ranging from 650 nm to 1200 nm with a peak wavelength longer than 800 nm and a full width at half maximum (FWHM) of more than 155 nm upon blue light excitation. The optimized phosphor also demonstrates good thermal stability, whose emission intensity at 150 °C can retain about 59% of its initial intensity at room temperature. The near-infrared LED prototypes constructed by combining the BaMSi3O9:Cr3+ phosphor with a blue LED chip give a maximum output power of 12.19 mW at a drive current of 320 mA. By using the fabricated near-infrared LED device as a lighting source, night-vision lighting and blood vessel imaging of human fingers and arms are successfully realized, demonstrating the great potential of BaMSi3O9:Cr3+ phosphors for near-infrared LED applications.
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2019
·
IF 3.375
Ruiqi Zhang,Zhen Wang,Zixin Zhou,Di Li,Tiefeng Wang,Ping Su,Yi Yang
In this research, the magnetic UiO-66-NH2 composites were prepared and applied as adsorbents for the effective removal of salicylic acid (SA) and acetylsalicylic acid (ASA) from aqueous media. The as-prepared adsorbent inherits both the excellent properties of metal organic frameworks and the magnetic separation property of magnetic material, which makes the magnetic UiO-66-NH2 composite exhibit a rapid separation rate and high capacity. The adsorption kinetics were well fitted with the pseudo-second-order model, and the adsorption isotherm could be well explained using the Langmuir isotherm. The dominant mechanism for adsorption of SA and ASA was hydrogen-bonding, the affinity of carboxyl groups with Zr–O clusters, and electrostatic interactions. The high adsorption capacities, easy separation process, fast adsorption kinetics, and satisfactory reusability of the magnetic UiO-66-NH2 give it fantastic potential as adsorbents for adsorptive separation of pharmaceutical contaminants from aqueous media.
✓ 已验证
产品关联
DOI
高影响因子
ACS Omega
·
2019
·
IF 2.584
Junjie Zhu,Linbo Wu,Zhiyang Bu,Suyun Jie,Bo-Geng Li
UiO-66-NH2, a zirconium-based functional metal–organic framework (MOF), was postsynthetically modified via Schiff base reaction between aldehyde groups in glutaraldehyde and amino groups in UiO-66-NH2 and CO2-preabsorbed polyethyleneimine (PEI). The resulting PEI-modified MOFs, abbreviated as PEIC@UiO, were characterized with 1H NMR, Fourier transform infrared, powder X-ray diffraction, Brunauer–Emmett–Teller, scanning electron microscopy, and thermogravimetric analysis and evaluated as CO2 adsorbents. In comparison with pristine UiO-66-NH2, the PEIC@UiO adsorbents have reduced specific surface area (7–150 m2/g) but maintained the same crystal structure. Particularly, the PEIC96@UiO adsorbent exhibited significantly improved CO2/N2 adsorption selectivity (48 vs 25) and higher CO2 adsorption capacity (3.2 vs 2.7 mmol/g). The adsorbent also displayed moderate desorption energy (68 kJ/mol CO2), superior moisture endurance, and recyclability, which are very desirable for practical applications.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CATALYSIS LETTERS
·
2019
·Vol. 149
·期 7
·1845-1855
·
IF 2.372
Wang Tao,Hu Aiyun,Xu Guangzhi,Liu Chen,Wang Haijun,Xia Yongmei
Furfural (FAL) is one of the most important biomass-derived platform compounds. The catalytic transformation of FAL was investigated with three porous Zr–thiophenedicarboxylate hybrids for the production of furfuryl alcohol (FOL). Three Zr-based catalysts, including DUT-67(Zr), DUT-68(Zr) and DUT-69(Zr) were synthesized through a facile assembly of 2,5-thiophenedicarboxylate acid with ZrCl 4 using the acetic acid as a modulator under hydrothermal conditions. These catalysts were also characterized using FT-IR, XRD, SEM, TEM, N 2 adsorption–desorption, XPS and TG. The specific surface area of the DUT-69(Zr) is smaller than that of the DUT-68(Zr) and slightly larger than that of the DUT-67(Zr), but it has a relatively large pore volume and pore diameter. Although all three catalysts showed excellent catalytic activity towards the catalytic transfer hydrogenation of FAL into FOL, the DUT-69(Zr) material has slightly higher catalytic activity than the other two catalysts. Besides, considering the cost of catalyst preparation, the DUT-69(Zr) material was used as the optimal catalyst and studied in detail. A high FOL yield of 92.2% at 95.9% FAL conversion was achieved at 120 °C for 4 h over DUT-69(Zr). Meanwhile, the DUT-69(Zr) could be reused more than six times with a minor decrease in catalytic activity. Finally, a plausible mechanism for catalytic transfer hydrogenation of carbonyl compounds to produce corresponding alcohols was presented based on the results of the experiments and previous reports. Graphical Abstract
✓ 已验证
产品关联
DOI
高影响因子
Analytical Methods
·
2018
·Vol. 11
·期 1
·36-43
·
IF 2.073
Shun-Hua Wu,Shu Wang,Wen-Le Fang,Xiao-Feng Guo,Hong Wang
In this study, we synthesized metal–organic frameworks (MOFs) UiO-67-bpydc using H2bpydc as ligands and Zr6 clusters as vertexes. Due to the protonation of the bipyridine group, UiO-67-bpydc shows pH-dependent fluorescence (365 nm/530 nm) in the pH range from 1 to 9, which shows its feasibility as a wide-range pH sensor. Further study indicated that UiO-67-bpydc exhibits stability, reusability, selectivity and has an excellent linear relationship in the pH range 4.0–6.5, and the mechanism of the UiO-67-bpydc fluorescence intensity with the variation of pH has been studied in detail. This MOF-based fluorescent sensor has been applied to specifically detect the pH of solutions in the presence of the body fluid matrix. Compared with reported pH-MOF sensors, UiO-67-bpydc can be practically applied in real samples and is easily prepared with excellent stability in different buffer solutions.
✓ 已验证
产品关联
DOI
高影响因子
CHEMISTRY OF MATERIALS
·
2017
·
IF 9.466
Jian Yang,Xiaojing Chen,Yongsheng Li,Qixin Zhuang,Peifeng Liu,Jinlou Gu
For practical biomedical applications, the stabilization of nanoscale metal–organic frameworks (NMOFs) in the presence of phosphate is of prime importance but remains a significant challenge because of the inevitable and strong driving force between metal clusters and phosphate species to form metal-phosphate in physiological environments. Through shielding Zr-NMOFs within the continuous phospholipid bilayers (PBLs), herein, we figured out a unique way to protect the vulnerable coordination bonds in their frameworks from the attack of phosphate. To exemplify the facility of constructing PBLs on Zr-NMOFs core, a porphyrinic NMOF of PCN-223 (standing for a platform with broad biological applications) was elaborated using a triethylamine (TEA)-modulated strategy. TEA could not only control the phase transformation of porphyrinic MOFs to achieve pure-phase PCN-223 crystals but also minimize their particles size down to sub-200 nm. Negative-stained TEM, FT-IR and XPS techniques revealed that PBLs could be closely coated onto the surface of nanoPCN-223, thanks to the strong Zr–O–P chemical complexation between Zr-NMOFs and phospholipid. The resultant coated nanoPCN-223 exhibited significantly enhanced phosphatic-resistance in phosphate buffer solution (PBS) and presented exceptional stability in harsh chemical environments. Furthermore, the MOFs-supported PBLs could effectively provide a stable biocompatible interface for subsequent cell culture and improve their biocompatibility, cellular uptake efficiency and real biostability of NMOFs in cellular environments. This study offers an alternative system for forming stable PBLs supported on NMOFs, and represents the first example of stabilizing Zr-NMOFs free from the attack of phosphate species in biological media.
✓ 已验证
DOI
高影响因子
Catalysis Science & Technology
·
2016
·Vol. 6
·期 14
·5543-5553
·
IF 5.287
Xin Zhao,Lei Huang,Supawadee Namuangruk,Hang Hu,Xiaonan Hu,Liyi Shi,Dengsong Zhang
A novel Zr–CeVO4/TiO2 catalyst was developed for the selective catalytic reduction (SCR) of NO with NH3. Both TiO2 nanosheets (TiO2-NS) and nanoparticles (TiO2-NP) with different crystal facets were used as supports for the catalyst. It was found that the TiO2-NS-supported catalyst showed much better activity, stability and H2O/SO2 durability than the TiO2-NP-supported catalyst. In particular, the catalyst loading amount was much lower than those of previously reported vanadate-based SCR catalysts. The crystal structures and morphologies were analysed by X-ray diffraction (XRD), Raman spectroscopy and (high-resolution) transmission electron microscopy ((HR)TEM). The redox properties, surface active species and acid sites of the catalysts were investigated through hydrogen temperature-programmed reduction (H2-TPR), X-ray photoelectron spectroscopy (XPS), ammonia and nitrogen oxide temperature-programmed desorption (NH3-TPD and NOx-TPD) and in situ diffuse reflectance infrared Fourier transform spectroscopy (in situ DRIFTs) experiments. The improved activity at lower temperature was due to the presence of more active oxygen species and Brønsted acid sites, as well as the formation of NO2 on the surface of the TiO2 nanosheets which have exposed (001) facets. The enhanced stability and H2O/SO2 durability of Zr–CeVO4/TiO2-NS was due to the limited formation of NH4NO3 and (NH4)2SO4/NH4HSO4. The excellent low operation temperature, low vanadium content and absence of WO3(MoO3) in this catalyst indicated that it has promising potential as a SCR catalyst for practical applications.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2016
·
IF 4.179
Jian He,Hu Li,Yanxiu Liu,Wenfeng Zhao,Tingting Yang,Wei Xue,Song Yang
A series of mesoporous acid–base bifunctional Zr/B mixed oxides with different molar ratios were prepared by a sol–gel method, and developed for conversion of ethyl levulinate (EL) to γ -valerolactone (GVL) by using alcohol as hydrogen source. The morphological structures and physico-chemical characteristics of the synthesized materials were identified by various techniques. A high GVL yield of 88.5% was achieved from EL in 2-propanol when Zr 1 B 1 was used. And acid–base sites played a synergic role in synthesizing GVL from EL as evident by poisoning experiments. Furthermore, the catalyst could be reused several times without significant loss of its catalytic activity.
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）