CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Zhen Wang,Ying Fang,Ying Yang,Bo Qiu,Haipu Li
A rational design of high-performance catalysts with peroxymonosulfate (PMS) activation and arsenic adsorption capacities for the removal of p -arsanilic acid ( p -ASA) is in high demand but remains a significant challenge. Herein, vacancies-rich metal–organic frameworks (MOFs) were constructed by room-temperature co-precipitation procedure, and the magnetic CoFe encapsulated in N -doped carbon nanotubes (CoFe- N -CNTs) were prepared using MOFs template by an annealing process under a nitrogen atmosphere. The synthesis conditions of CoFe- N -CNTs were optimized by tuning Fe/Co ratio and carbonization temperature. The CoFe- N -CNTs/PMS system showed favorable removal performance, achieving complete degradation of 46 μM p -ASA within 3 min and a total arsenic removal efficiency of 98% within 30 min at 0.1 g/L catalyst and 400 μM PMS. The degradation rate ( k obs ) and total arsenic removal efficiency towards p -ASA by CoFe- N -CNTs/PMS system were 6.7 and 2.7 times of those in the MOFs without vacancies-derived catalyst/PMS system, respectively. CoFe- N -CNTs/PMS system exhibited robust and efficient performance over a broad range of pH (4.5–9.0) and in different water matrices. Scavenging experiments and electron paramagnetic resonance (EPR) results demonstrated that non-radical singlet oxygen ( 1 O 2 ), sulfate radicals (SO 4 − ), hydroxyl radicals ( OH), and superoxide (O 2 − ) were involved in p -ASA decomposition. Electron transfer and direct oxidative transfer process (DOTP) also contributed to p -ASA degradation. High-performance liquid chromatography coupled with inductively coupled plasma mass spectrometry (HPLC-ICP-MS) analysis indicated that the arsenic moiety was cleaved from p -ASA in the form of As(III) and then rapidly oxidized to As(V). X-ray photoelectron spectroscopy (XPS) analysis indicated the removal of inorganic arsenic followed the mechanism of the inner-sphere complex. This study highlights the in-situ synthesis of CoFe- N -CNTs with outstanding activities for catalytic degradation and arsenic removal of organoarsenicals.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
·
IF 9.965
Guoqing An,Chang'an Wang,Hongyi Gao,Ge Wang,Yibin Luo,Zhiyuan Liu,Changjiu Xia,Siqi Liu,Xinxin Peng,Zhixiang Cheng,Xingtian Shu
Titanosilicate-1 zeolites (TS-1) as one of the most commonly used catalysts for alkene epoxidation , construction of hierarchical pores as well as elimination of anatase to promote mass transportation and avoid invalid decomposition of hydrogen peroxide are always desirable yet challenging goals. Here, a novel and unique Ti-based metal organic frameworks (MOFs)-induced synthetic strategy for fabricating anatase-free hierarchical TS-1 was first proposed. All the components of MOFs perform different functions: the uniformly distributed Ti nodes replace conventional tetrabutyl titanate (TBOT) to serve as sole Ti source for constructing zeolite crystal; the separated ligands can be embedded in the zeolite framework and act as template to in situ build hierarchical pore structure ; the coordination interaction between Ti nodes and ligands can efficiently avoid the anatase generation by balancing the forming rates of Ti-OH and Si-OH. This synthetic strategy is of general applicability, and two different synthetic routes including traditional hydrothermal process and steam assisted crystallization (SAC) procedure are successfully adopted. The obtained hydrothermal TS-1 and SAC anatase-free samples all possess abundant intercrystalline mesopores of 20–50 nm and even macropores between 50 and 150 nm, improving the conversion over 25 % for 1‑hexene epoxidation than TS-1 sample prepared by conventional route. The influences of the amount of Ti MOFs precursor and the crystallization process are studied in detail, and possible synthesis mechanisms are proposed. This MOFs-induced strategy might open up an avenue for the rational design of ideal and hierarchical zeolite to boost the catalytic efficiency.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Miaomiao Li,Junwei Yuan,Guan Wang,Liujun Yang,Junxia Shao,Hua Li,Jianmei Lu
The key to efficient treatment of organic pollutants in water is to improve their mass transfer efficiency and reaction efficiency. Herein, a one-step construction of new metal-organic frameworks (MOFs) using 4, 4′, 4″, 4″-(pyrene-1, 3, 6, 8-tetrayl) tetra-benzoic acid as a photosensitizer ligand and Ti-In as bimetallic centers has been constructed. The results exhibited that increased specific surface area was obtained by Ti-In-MOF(1:1), which improved the adsorption performance of 50 ppm bisphenol A to 38% and facilitated it complete degradation upon light irradiation in 20 min, being much faster than that of single In/Ti-MOFs. For Ti-In-MOF(1:1), the In-MOF parts enhanced the adsorption capability, meanwhile the Ti-MOF parts based on infinite Ti-O chains realized the effective separation of photogenerated carriers. A synergistic role of adsorption and degradation achieved rapid mass transfer and excellent catalytic degradation performance. This investigation will provide a novel MOF construction strategy for efficient catalytic application in environmental pollutants.
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Journal of CO2 Utilization
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2022
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IF 8.321
Chengyuan Duan,Yuming Xie,Meili Ding,Yi Feng,Jianfeng Yao
Integrating dual Lewis acid and base as well as rational hierarchical pore structure in one catalyst is favorable to significantly boost the CO 2 cycloaddition reaction at mild conditions. In this regard, carbonized melamine sponge (CMS) featuring a highly porous network, rich nitrogen doping and excellent photothermal capability is employed as the ideal host for the construction of CMS@MOFs (namely, MIL-88-NH 2 and ZIF-8-NH 2 ) composites with diverse acid-base properties. Results show that all the obtained composites exhibited a satisfactory CO 2 adsorbing capacity (33–54 cm 3 /g) and delivered a remarkable yield of target cyclic carbonate at either mild thermal conditions (0.1 MPa CO 2 and 80 o C) or under light irradiation (light intensity: ~350 mW/cm 2 ) at room temperature. Even with diluted CO 2 (15 vol. % CO 2 ), high yields of 80–82 % are achievable. Moreover, the used catalysts can be easily recycled from reaction systems, leading to a good recyclability .
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Journal of Environmental Chemical Engineering
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2022
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IF 7.968
Fei Yu,Junyao Pan,Yiyao Li,Yidi Yang,Zhi Zhang,Jiayang Nie,Jie Ma
Due to the high dependence on tetracycline in the daily production and life of human beings, its abuse problem is serious, which affects the safety of the ecological environment. How to effectively remove residual tetracycline in the environment is an urgent problem to be solved. In this study, HKUST-1 was successfully composited with rice husk and wheat straw biochar by hydrothermal method, and then combined with κ-carrageenan and calcium alginate by cross-linking replacement method to prepare a novel modified biochar composite gel. Through a series of static adsorption experiments, the adsorption of TC on the two modified biochar composite gels reached equilibrium within 24 h and was dominated by chemical adsorption , and the maximum adsorption capacities for TC could reach 313.00 and 396.09 mg·g −1 , respectively. The adsorption mechanism of TC on the modified biochar composite gels is mainly hydrogen bonding, electrostatic attraction, metal-organic complexation and π-π interaction. At the same time, the dynamic adsorption process was simulated through a fixed-bed column experiment, and the results showed that the modified biochar composite gels as a new type of adsorption material can be effectively applied to the removal of organic pollutants in actual sewage, providing basic support for future practical application research.
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Chemistry-An Asian Journal
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2022
·Vol. 17
·期 14
·e202200161
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IF 4.839
Bo Ling,Yaguang Wang,Ruo Mi,Di Wang,Hongqi Chen,Xiaohu Li,Ye Zhang,Lun Wang
Graphical NaGdF 4 ,Yb,Er@NaGdF 4 ,Yb,Tm@NaYF 4 core@shell@shell three-layer structure of upconversion nanoparticles coated with Fe−TCPP metal-organic frameworks nanocomposite was designed and constructed for multimodal imaging and synergetic chemodynamic therapy/photodynamic therapy of tumors. Here, NaGdF 4 ,Yb,Er@NaGdF 4 ,Yb,Tm@NaYF 4 core@shell@shell three-layer structure of upconversion nanoparticles (UCNPs) coated with Fe−Tetrakis (4-carboxyphenyl) porphine (TCPP) metal-organic frameworks (Fe-MOFs) nanocomposite (UCNPs@MOFs) was designed and constructed for multimodal imaging and synergetic chemodynamic therapy (CDT)/photodynamic therapy (PDT) of tumors. The UCNPs@MOFs were successfully applied for tumor cells imaging in vitro and in vivo in near-infrared (NIR) region. The doped Gd was used as contrast agent for the magnetic resonance imaging (MRI) of mouse tumors. The luminescence in the UV-vis region was absorbed by the Fe-MOFs to produce singlet oxygen ( 1 O 2 ) for PDT. The Fe 3+ doped in the MOFs can catalyze H 2 O 2 to produce oxygen and hydroxyl radical (⋅OH). Hydroxyl radical is used in CDT and cooperates with the 1 O 2 of PDT. Based on the CDT/PDT synergistic effects, the UCNPs@MOFs nanocomposite had obviously enhanced tumor inhibitory efficiency in vivo. These results described that the asprared UCNPs@MOFs nanocomposite have great potential in the effective multimodal imaging and treatment of tumors.
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Biosensors-Basel
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2023
·Vol. 13
·期 5
·508
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IF 5.4
Ya Yang,Wenhui Ji,Yutao Yin,Nanxiang Wang,Wanxia Wu,Wei Zhang,Siying Pei,Tianwei Liu,Chao Tao,Bing Zheng,Qiong Wu,Lin Li
Rapid and accurate detection of changes in glucose (Glu) and hydrogen peroxide (H2O2) concentrations is essential for the predictive diagnosis of diseases. Electrochemical biosensors exhibiting high sensitivity, reliable selectivity, and rapid response provide an advantageous and promising solution. A porous two-dimensional conductive metal–organic framework (cMOF), Ni-HHTP (HHTP = 2,3,6,7,10,11-hexahydroxytriphenylene), was prepared by using a one-pot method. Subsequently, it was employed to construct enzyme-free paper-based electrochemical sensors by applying mass-producing screen-printing and inkjet-printing techniques. These sensors effectively determined Glu and H2O2concentrations, achieving low limits of detection of 1.30 μM and 2.13 μM, and high sensitivities of 5573.21 μA μM−1cm−2and 179.85 μA μM−1cm−2, respectively. More importantly, the Ni-HHTP-based electrochemical sensors showed an ability to analyze real biological samples by successfully distinguishing human serum from artificial sweat samples. This work provides a new perspective for the use of cMOFs in the field of enzyme-free electrochemical sensing, highlighting their potential for future applications in the design and development of new multifunctional and high-performance flexible electronic sensors.Keywords:Ni-MOFs;paper-based sensors;electrochemical sensor;non-enzymatic catalysis;hydrogen peroxide;glucose
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Yu Guan,Guolang Zhou,Lin Li,Yexin Jiang,Jingzhou Yin,Cheng Liu,Lili Zhang,Qiaofeng Han,Edison Huixiang Ang
This research focused on creating oxygen vacancy-enriched copper-doped LaFeO 3 perovskite using a Prussian blue MOF template. This new material, LFO-Cu, showed outstanding Bisphenol A (BPA) degradation with 98 % efficiency in just 30 min, ten times faster than pure LaFeO 3 (LFO). Moreover, the LFO-Cu/peroxymonosulfate (PMS) system worked effectively at pH levels from 4 to 10, breaking down various pollutants (TC, PhOH, MV, MB), and removing 85 % TOC in BPA and 50 % in TC. Density Functional Theory (DFT) calculations revealed that copper strengthened the catalyst-PMS interaction, leading to the generation of highly reactive oxygen species (ROS), primarily singlet oxygen ( 1 O 2 ) and superoxide radicals (O 2 – ·). A degradation pathway was proposed, showing less toxic intermediates than BPA. In summary, copper-doped oxygen-rich vacancy MOFs-derived perovskite has significant potential for improving refractory organic mineralization.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2023
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IF 8.2
Chaoqun Zhang,Qi He,Wenbin Luo,Jian Du,Yehan Tao,Jie Lu,Yi Cheng,Haisong Wang
The commercial graphene for Li ion batteries (LIBs) has high cost and low capacity. Therefore, it is necessary to develop a novel carbon anode. The cellulose nanowires (CNWs), which has advantages of low cost, high carbon content, is thought as a good carbon precursor. However, direct carbonization of CNWs leads to low surface area and less mesopores due to its easy aggregation. Herein, the metal-organic frameworks (MOFs) have been explored as templates to prepare porous carbon due to their 3D open pore structures. The porous carbon was developed with the coordination effect of CNWs and MOFs. The precursor of MOFs coordinates with the −OH and − COOH groups in the CNWs to provide stable structure. And the MOFs was grown in situ on CNWs to reduce aggregation and provide higher porosity. The results show that the porous carbon has high specific capacity and fast Li + /electronic conductivity. As anode for LIBs, it displays 698 mAh g −1 and the capacity retention is 85 % after 200 cycles. When using in the full-battery system, it exhibits energy density of 480 Wh kg −1 , suggesting good application value. This work provides a low-cost method to synthesize porous carbon with fast Li + /electronic conductivity for high-performance LIBs.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
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IF 8.6
Deng Pan,Yanan Wang,Han Li,Yuzhe Zhang,Qian Liang,Man Zhou,Zhongyu Li,Song Xu
The conversion of the greenhouse gas CO 2 represents a pragmatic and environmentally friendly approach. However, the substantial energy demands of the reaction hamper its widespread application. Here, we designed an efficient catalyst prepared by Ce-MOF and ZIF-67 precursor, namely Co/CeO 2 , for photothermal CO 2 methanation under light and auxiliary heating. CeO 2 synthesized by Ce-MOF has a good structure and abundant oxygen vacancies, meanwhile, Co has abundant active sites and strong adsorption capacity and is well-dispersed on CeO 2 . As a result, the catalyst exhibits high CH 4 yield of 885.27 mmol⋅g −1 ⋅h −1 and CO yield of 24.5 mmol⋅g −1 ⋅h −1 . Moreover, it has good selectivity and catalytic durability. Through the analysis of the reaction pathway under the conditions of photothermal catalysis, the hydrogenation reaction of formate can efficiently generate CH 4 and H 2 O due to the promotion of hot carriers. This work demonstrated the advantages of photothermal co-catalysis and provides a potential strategy for efficient CO 2 reduction.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Kaini Yang,Xiangyu Wang,Iseult Lynch,Zhiling Guo,Peng Zhang,Lisi Wu
Nano zero-valent iron (NZVI) is an ideal material for treating chromium (VI). However, the NZVI's low loading and corrosion susceptibility in acidic Cr-containing industrial wastewater is the most pressing issue. Therefore, it is necessary to explore a method to construct novel NZVI composites with high loading, corrosion resistance, and outstanding activity. In this study, green 2-mercaptobenzimidazole (MBI) was employed for the first time as a corrosion inhibitor for NZVI to form a protective coating through chemisorption, thus blocking the corrosion of NZVI by reaction medium. Meanwhile, a novel multiphase green crystallization-assisted pore formation freeze-drying method was constructed to synthesize UiO-66-NH 2 regulated 3D network porous polyacrylonitrile (PAN) cryogel film for stabilizing NZVI, which is intended to remove Cr(VI) effectively and without secondary contamination. The synthesized MBI-Fe 0 @MOF/PAN possessed prominent activity, corrosion resistance, and considerable NZVI loading (45.9 mg/g). The Cr(VI) removal could still reach 82.7 % after 6 cycles, and the level of total dissolved iron ions was lowered to 0.255 mg/L. MBI-Fe 0 @MOF/PAN for rapid removal of Cr(VI) may be ascribed to the synergistic reaction of rapid protonation of MBI and strong reduction of NZVI. This study constructed the MBI corrosion-resistant interface and 3D PAN cryogel film concepts not only to broaden the horizons of designing efficient NZVI catalytic materials but also to promote the development of treatment technologies for acidic Cr-containing industrial wastewater.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 51
·110901-110912
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IF 5.8
Ai Huiying,Zhang Zhiyong,Ji Yuxi,Xu Lei,Fu Ming-Lai,Yuan Baoling
Excessive phosphorus in water would cause eutrophication and deterioration of the ecological environment. Herein, the La-MOFs/Al 2 O 3 composite was successfully prepared by the in situ hydrothermal synthesis method for granulation, which was conducive to exerting the phosphate adsorption capacity and facilitating practical application. The materials were characterized by SEM, EDX, XRD, BET, FTIR, and Zeta. In addition, the adsorption performance of La-MOFs/Al 2 O 3 was evaluated through adsorption kinetics and isotherms, showing that the Langmuir adsorption capacity was 16.34 mgP·g -1 (25 °C) and increased with the water temperature. Moreover, the batch influence experiments of intimal pH, adsorbent dosage, coexisting ions, and stability tests were performed to analyze the potential for practical applications and verified through the natural micro-polluted water samples from Houxi River and Bailu Lake (China). The results indicated that the La-MOFs/Al 2 O 3 was suited to a wide pH range of 4 to 10 and the phosphate removal efficiency remained above 70% after continuous use for four times, exhibiting excellent stability. It also had excellent selectivity in the presence of SO 4 2- , Cl - , NO 3 - , and HCO 3 - , only decreased to 70.24% at high HCO 3 - ion concentration of 60 mg/L, respectively. And the La-MOFs/Al 2 O 3 had excellent adsorption of total phosphorus, phosphate, and organic phosphorus in the actual river and lake water and completely removed dissolved phosphorus. Finally, a phosphate adsorption mechanism model involved in electrostatic interaction and ligand exchange was proposed. Therefore, La-MOFs/Al 2 O 3 could be considered to be an excellent phosphorus adsorbent for application in the actual water environmental remediation. Graphical abstract
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