Advanced Science
·
2023
·Vol. 10
·期 31
·2304149
·
IF 15.1
Qiuyu Ye,Enxian Yuan,Jin Shen,Mingli Ye,Qin Xu,Xiaoya Hu,Yun Shu,Huan Pang
CsPbX 3 perovskite nanocrystal (NC) is considered as an excellent optical material and is widely applied in optoelectronics. However, its poor water stability impedes its study in enzyme-like activity, and further inhibits its application in biomimetic cascade catalysis. Herein, for the first time, the oxidase-like and ascorbate oxidase-like activities of an amphiphilic polymer capped CsPbX 3 are demonstrated, and its catalytic mechanism is further explored. Furthermore, an all-nanozyme cascade system (multifunctional CsPbBr 3 @Zr-metal organic framework (Zr-MOF) and Prussian blue as oxidase-like and peroxidase-like nanozyme) is constructed with a portable paper-based device for realizing the dual-mode (ratiometric fluorescence and colorimetric) detection of ascorbic acid in a point-of-care (POC) fashion. This is the first report on the utilization of all-inorganic CsPbX 3 perovskite NC in biomimetic cascade catalysis, which opens a new avenue for POC clinical disease diagnosis.
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Advanced Sustainable Systems
·
2022
·Vol. 6
·期 3
·2100321
·
IF 6.737
Pei-dong Wu,Hu Li,Zhen Fang
Bimetallic synergy and carbon–nitrogen doping can contribute to enhanced catalytic activity due to the strong electronic state and unique geometrical structure. In this work, a series of biomass-derived Co-M bimetallic C N doped catalysts (Co-M@Chitosan-X; M = Zr, Ni, Fe, Cu, In; X denotes the molar percentage of M) are prepared via simple oil bath reflow and annealing. The Co-Zr@Chitosan-X catalysts are determined to contain alloys (Co-Zr), metal-carbon bonds (Co-C, Zr-C), metal-nitrogen bonds (Co-N, Zr-N), and metal oxides (Co 3 O 4 , ZrO 2 ) through a series of characterizations, in which graphite-coated alloys and metal oxides are found to be the catalytically active species. The doping of the second metal results in a significant enhancement for the number of active sites in the catalyst, and the d-band center is shifted toward a deviation from the Fermi energy level. Among the tested catalysts, Co-Zr@Chitosan-20 exhibits superior catalytic activity for the reductive amination of biobased levulinic acid to 5-methyl-2-pyrrolidone in 99.3% selectivity and 92.8% yield. This non-noble metal bimetallic synergistic catalytic protocol opens an avenue for efficiently producing biomass-derived nitrogenous chemicals.
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NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 6
·2653-2661
·
IF 3.925
Long Jin,Feng Liu,Jian-hua Wu,San-Jian Ma,Juan-Hong Li,Yong-Jing Tian,Xin Liu,Zi-Xia Lin
A novel improved Fenton system named MHACF-UiO-66(Zr) was constructed under normal temperature and pressure based on the reduction of FeIII accelerated by hydrogen. The regeneration of FeII was enhanced by Pd/UiO-66(Zr). The hydroxyl radical could be continuously generated using only trace level FeII. 10 mg L−1 4-chlorophenol could be thoroughly degraded in the initial conditions of 75 mL min−1 H2, pH 3, 20 mM H2O2, 2 g L−1 Pd/UiO-66(Zr) and 20 μM FeII. Moreover, the removal efficiency of 15 mg L−1 sulfamethazine could be maintained at least more than 94% under the same conditions. The activity of the solid catalyst could be maintained after 6 consecutive reaction cycles. This provides new insight for improving the inherent shortcomings of the Fenton reaction, which generates large amounts of iron sludge.
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Journal of Water Process Engineering
·
2022
·
IF 7.34
Xu Chai,Huaqi Dong,Zenggao Zhang,Zhaoyang Qi,Jie Chen,Zhixian Huang,Changshen Ye,Ting Qiu
Due to natural and production activities, mercury contamination has become one of the major environmental problems in the world. Adsorption is one of the important means to solve this problem. However, most of the commercially available adsorbents exhibit relatively low adsorption capacity and slow kinetics. Therefore, a novel 4,6-diamino-2-mercaptopyrimidine-functionalised Zr-based metal-organic framework (UiO-66-DMP) was synthesised in this study. The UiO-66-DMP was characterised through X-ray diffraction, scanning electron microscopy, energy dispersive spectrometry , X-ray photoelectron spectroscopy, Fourier-transform infrared spectrometry, and thermogravimetric analysis . The potential of the UiO-66-DMP as a superior adsorbent for Hg(II) removal and the corresponding mechanisms were evaluated through batch experiments under different conditions and density functional theory calculations. Benefitting from its high specific surface area and multiple adsorption sites, the maximum Hg(II) adsorption capacity achieved in this study was 822.00 mg·g-1, which is the highest Hg(II) adsorption capacity reported to date. In addition, under the interference of Ca(II), Cd(II), Co(II), Mg(II), Mn(II), Ni(II), Cr(III), Cu(II), Zn(II) and other coexisting ions, the UiO-66-DMP could still maintain the high selective adsorption capacity for Hg(II). According to the characterization analysis and DFT calculation results, the adsorption of Hg(II) onto the UiO-66-DMP was dependent on electrostatic and covalent interactions between metal ions and abundant functional groups on the UiO-66-DMP surface.
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Particuology
·
2021
·
IF 3.067
Suyu Zhou,Xiaojing Guo,Xi Yan,Yan Chen,Wanzhong Lang
Lithium ion sieve (LIS) has attracted great attention due to its high adsorption selectivity towards Li + . Herein, a new type of Zr-doped Ti-LIS (HZrTO) was synthesized by a simple calcination method. The adsorption capacity increased from 56.3 mg g −1 (before doping) to 93.2 mg g −1 after doping in LiOH solution (lithium 1.8 g L −1 ). The adsorption isotherm and adsorption kinetics of HZrTO accord with the Langmuir isotherm and the pseudo-second-order kinetic equation, respectively. Batch experiments showed that HZrTO has good stability and selectivity. In addition, HZrTO was granulated via epoxy resin (E-12), and the obtained granular adsorbent showed good adsorption capacity, excellent stability and high selectivity towards Li + .
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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.
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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.
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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.
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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.
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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.
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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.
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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.
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