Advanced Sustainable Systems
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2022
·Vol. 6
·期 3
·2100321
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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
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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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Inorganic Chemistry Frontiers
·
2021
·Vol. 8
·期 24
·5186-5194
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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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Particuology
·
2021
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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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APPLIED CATALYSIS B-ENVIRONMENTAL
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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
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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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PubMed
高影响因子
International Journal of Applied Ceramic Technology
·
2024
·
IF 1.8
Shuaijun Yang,Mei Wang,Yetong Lv,Huilin Sheng,Yexia Qin
Oxidation resistance is crucial to the potential applications of high-entropy carbides (HECs) at elevated temperatures. Here, we realize the exploration of (Hf, Ta, Zr, Cr)C high-entropy carbides (HEC-TM, TM = Hf, Zr, Ta, and Cr) with good oxidation resistance by optimizing their compositions. To be specific, 21 kinds of HEC- x TM ( x = 0–25 mol%) samples are fabricated by a high-throughput ultrafast high-temperature sintering technique, followed by oxidation testing at 1673 K for 30 min. Among all the HEC samples, the as-fabricated HEC-0Zr samples are proved to possess the best oxidation resistance with an oxidation depth of only 53 µm. Further study on isothermal oxidation kinetics demonstrates that the as-fabricated HEC-0Zr samples follow a linear oxidation law. The good oxidation resistance of the as-fabricated HEC-0Zr samples is believed to result from the (Ta, Me) 2 O 5 phase with a low melting point, which can promote the densification of the oxide layer. This research opens up a new way for efficiently discovering new HECs for extreme applications.
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NEW JOURNAL OF CHEMISTRY
·
2024
·Vol. 48
·期 45
·19220-19228
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IF 2.7
Peng Lu,Qianwen Hu,Kui Wang,Shiyong Chen,Zongxiao Li,Xinjie Chen,Chuang Xing,Yanhong Wang,Ce Du
The efficient CO2 conversion to light olefins through hydrogenation is a feasible strategy to achieve carbon neutrality goals. Herein, a series of bimetallic Zn–Zr/supports are synthesized by a conventional impregnation method. We demonstrate that different supports endow catalysts with various specific surface areas, pore sizes, chemical adsorption performances, and acid densities. The effects of different support-loaded Zn–Zr coupled with SAPO-34 on CO2 hydrogenation to light olefins are investigated systematically. The CO2 conversion of Zn–Zr/Q10-SAPO-34, Zn–Zr/Q50-SAPO-34, Zn–Zr/γAl2O3-SAPO-34, Zn–Zr/MgO-SAPO-34 and Zn–Zr/S-1-SAPO-34 is 11.4%, 9.2%, 24.0%, 8.8%, and 16.2%, respectively, with corresponding light olefin selectivity of 39.0%, 28.1%, 30.4%, 4.8%, and 14.7%, respectively. Significantly, γAl2O3 is more conducive to CO2 conversion, while Q10 tends to produce light olefins. This work provides an effective reference for support selection in CO2 hydrogenation to light olefins.
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NEW JOURNAL OF CHEMISTRY
·
2025
·
IF 2.5
Dan Wang,Wenjing Cai,Qiuxiang Feng,Feng Cao,Qianli Zhang,Qiang Xu,Li Li,Jie Liu
To develop porous solid-state materials for effective capture of radioactive iodine in both vapor and solution phases is of great importance. In this work, a Zr/Ti-based bimetallic metal-organic framework (AO-UiO-66-ZrTi11) was synthesized via a simple solvothermal method using 2, 5-bis (allyloxy)terephthalic acid, ZrCl4 and Cp2TiCl2. This MOF solid was fully characterized and extensively evaluated for its I2 capturing performance. AO-UiO-66-ZrTi11 demonstrated significantly enhanced I2 uptake capacity, achieving as high as 2.46 g·g-1 for iodine vapor and 1084.4 mg·g-1 for iodine/cyclohexane solution. Kinetic studies of iodine adsorption from solution revealed rapid kinetics, with the process fitting well to the pseudo-second order kinetic model. The superior adsorption performance of AO-UiO-66-ZrTi11 for iodine can be attributed to its unique bimetallic structural features and functional groups. This work provides valuable insights for the further development of efficient adsorbents towards capturing radioactive iodine.
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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.
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