INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2021
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IF 3.764
Ju Liu,Dandan Hao,Huiwen Sun,Yu Li,Jianlin Han,Bo Fu,Jiancheng Zhou
In this Article, a hybrid foam was fabricated through the integration of amine-functionalized Fe-MOF (MIL-101-NH2) into cellulosic matrix. The existence of enormous group linkages and ionic bonding interactions among the composite foam network leads to a uniform dispersion of MIL-101-NH2 and high affinity between the MOF and cellulose skeleton. As-prepared hybrid foams were utilized as photocatalysts to reduce toxic hexavalent chromium ions (Cr(VI)) under visible light. Optimal performance was observed over CM-1 (with a MIL-101-NH2 and nanocellulose mass ratio of 1:1). When compared to pure MOF nanoparticle counterparts, the CM-1 foam presented preferable and more efficient Cr(VI) removal performance. The reasons could be attributed to the hierarchal pore structure and uniform MOF loading. Moreover, the flexible foams could be easily separated from the solution and preserved more than 80% removal efficiency of Cr(VI) after 10 runs. This work would shed light on how to construct high-efficiency photocatalysts for environmental governance from sustainable materials.
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Catalysis Science & Technology
·
2021
·Vol. 11
·期 19
·6507-6515
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IF 6.119
PanPan Xu,Liuxue Zhang,Xu Jia,Hao Wen,Xiulian Wang,Suqing Yang,Juxian Hui
Compared to the current commercial three-step production process involving low phenol yield, low atomic efficiency, and the formation of explosive intermediates, the direct oxidation of aromatic hydrocarbon to more desirable and important chemical industry intermediate such as phenol offers a more attractive and challenging pathway. Here, we report the selective photocatalytic hydroxylation of benzene to phenol using NH2-MIL-88/PMo10V2-3 as the catalyst and H2O2 as a mild oxidant. Heteropoly acid (PMo10V2) was immobilized to metal–organic frameworks (NH2-MIL-88), where PA anions play an essential role in anchoring NH3+ cations to form stable heterogeneous photocatalysts. The reaction offered a high selectivity of 99% with a yield of 24% for phenol under optimum reaction conditions. Comprehensive characterizations and experiments disclosed a multistep reaction mechanism in which high dispersion of PMo10V2, the production of hydroxyl radical(˙OH) and the formation of V5+/V4+ redox pairs are responsible for the activity of the reaction in the presence of electrons (e−). The recycling experiments were essential in confirming the reusability of the catalyst, and FT-IR characterization analysis also proved the integrity of NH2-MIL-88/PMo10V2-3 after three cycles. This work provides potential applications in the green and highly efficient photocatalytic synthesis of other organic compounds and other environmental applications.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Guanglai Mo,Linxi Wang,Jianhong Luo
It is a challenge to achieve efficient photocatalytic activity of pure MOFs. Herein, the defective NH 2 -MIL-125(Ti) with adjustable linker vacancy level was successfully created by thermal treatment. The band gaps of samples decreased and the more Ti-O clusters on the surface of the samples can be achieved as the time of thermal treatment increased from 0 to 500 min, both of which facilitated the photocatalytic activity for the reduction of Cr(VI). Moreover, the ligands from the surface to the inside of the samples were successively decarboxylated, resulting in the declined specific surface area and the increased proportion of mesoporous and the defect level. The moderate defect level in NH 2 -MIL-125(Ti) can be obtained as the time of thermal treatment was 300 min, which facilitated the separation of photogenerated charges, contributing to the highest photocatalytic activity for reduction of Cr(VI), which was 9.2 times than that of the initial MOFs. However, the excessive linker vacancy defect level in NH 2 -MIL-125(Ti) may result in the seriously affected crystal structure and the retarded separation of photogenerated charges.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2021
·
IF 5.816
Chengbao Liu,Dongchen Shen,Zhengkai Tu,Song Li
Li + doping is regarded as an effective strategy to enhance the room-temperature hydrogen storage of metal-organic frameworks (MOFs). In this work, Li + is doped into both MIL-100(Fe) and MIL-100(Fe)/graphene oxide (GO) composite, and it is demonstrated that the hydrogen uptake of Li + doped MIL-100(Fe)/GO (2.02 wt%) is improved by 135% compared with Li + doped MIL-100(Fe) (0.86 wt%) at 298 K and 50 bar, which is ascribed to its higher isosteric heat of adsorption (7.33 kJ/mol) resulting from its more accessible adsorption sites provided by doped Li + ions and ultramicropores. Grand canonical Monte Carlo (GCMC) simulation reveals that Li + ions distributing in the interface between MIL-100(Fe) and GO within MIL-100(Fe)/GO composite is favorable for hydrogen adsorption owing to the increased number of adsorption sites, thus contributing to the enhanced hydrogen storage capacity. These findings demonstrate that MIL-100(Fe)/GO is a more promising Li + doping substrate than MIL-100(Fe).
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2021
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IF 4.539
Weifeng Li,Tao Zhang,Li Lv,Yanxiao Chen,Wenxiang Tang,Shengwei Tang
A novel strategy of room-temperature synthesis of MIL-100(Fe) with organic amine as deprotonating agent was proposed. The as-prepared solid product was denoted as R-MIL-100(Fe). The material was systematically characterized via XRD , FT-IR, XPS and SEM. The effects of operation parameters such as initial fluoride concentration, reaction time, initial pH and co-existing anions on the fluoride adsorption performance of the synthesized R-MIL-100(Fe) were studied. The maximum fluoride adsorption capacity of R-MIL-100(Fe) was as high as 23.53 mg/g at 298 K in the fluoride solution. The results indicate that the adsorption process of fluorine on R-MIL-100(Fe) belongs to surface adsorption and intraparticle diffusion . An excellent fluoride adsorption performance of R-MIL-100(Fe) was observed in a wide pH range of 4–10. The co-existing anions including Cl - , NO 3 - and SO 4 2- almost had no negative effects on the adsorption performance of R-MIL-100(Fe). However, the present of CO 3 2- or HCO 3 - brought an obvious reduction of F - adsorption capacity of R-MIL-100(Fe). Thermodynamic study results illustrate that the adsorption process was an exothermic chemisorption . Chemical combination of iron and fluorine was confirmed by FT-IR and XPS. The strong combination brings the excellent F - adsorption performance of MIL-100(Fe). R-MIL-100(Fe) was successfully regenerated and recycled five cycles with an excellent regeneration ability and recyclability.
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JOURNAL OF MEMBRANE SCIENCE
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2020
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IF 7.183
Ao-Shuai Zhang,Shen-Hui Li,Ali Ahmad,Heng Mao,Li-Hao Xu,Zhi-Ping Zhao
High porosity and large pore volume of MIL-101 MOF makes it a potential material to be used in membrane separation technology . However, the extra-large pore size and natural hydrophilicity restrict its application in the organic perm-selective pervaporation process. To overcome this issue, Herein, we successfully synthesized ILs@MOFs composite by modifying MIL-101 via coordinative covalent grafting of designed hydrophobic ionic liquids (ILs). Later on, synthesized ILs-modified MIL-101 was embedded into poly (ether-block-amide) (PEBA) polymer to fabricate mixed matrix membranes (MMMs) for ethyl acetate perm-selective pervaporation. Incorporation of ILs within the cages and over the surface of MIL-101 not only successfully tuned the pore structure and surface properties of MIL-101 but also inhibits the formation larger aggregates with no obvious defects in resultant MMMs. Moreover, molecular simulation verified that the grafted ILs endowed MIL-101 with better adsorption ability for ethyl acetate and improved interfacial compatibility with PEBA. The optimized MMMs exhibited outstanding separation performance for 5 wt% feed solution at 30 °C, with a separation factor of 207.6 and normalized total flux of 51.8 kg·μm·m −2 ·h −1 . Compared with the pure PEBA membrane, the separation factor and ethyl acetate flux increased by 205.7% and 129.5%, respectively, while the MMMs embedding original MIL-101 showed a decrease in separation factor. This study may inspire the design and construction of high-performance MMMs by employing modification in porous nanomaterial microstructure.
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CHEMOSPHERE
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2021
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IF 7.086
Liu-Xi Yang,Jia-Cheng E. Yang,Ming-Lai Fu
In this study, porous magnetic CoFe 2 O 4 nanocrystals (NCs) were successfully synthesized by using bimetal-organic framework (MOF) as a precursor, and used as catalysts to activate peroxymonosulfate (PMS) for the removal of chloramphenicol (CAP) in the solution. The structure and physicochemical properties of CoFe 2 O 4 NCs were thoroughly examined by a series of characterization techniques. The results revealed as-synthesized CoFe 2 O 4 had a nanorod-shaped structure with high specific surface area (83.00 m 2 g −1 ) and pore volume (0.31 cm 3 g −1 ). Furthermore, the degradation efficiency (100%) and the removal of total organic carbon (68.09%) were achieved after 120 min with 0.1 g/L CoFe 2 O 4 NCs, 2 mM PMS and 10 mg/L CAP at pH of 8.20. In addition, effects of catalyst dosage, PMS dosage, initial pH values, CAP concentration and co-existing anions as well as natural organic matters in the solution on the degradation efficiencies were studied and all the removal can be well fitted with pseudo-first-order kinetic model (R 2 > 0.96). Sulfate radicals (SO 4 •− ) and hydroxyl radicals (HO•) were proved to be two main reactive species for CAP removal in CoFe 2 O 4 /PMS system based on quenching experiments. CAP was degraded by the main pathways of dichlorination, denitration, decarboxylation , hydroxylation, ring cleavage and chain cleavage on CoFe 2 O 4 /PMS system through high performance liquid chromatograph-mass spectrometry analysis. We believe that this study would be very meaningful to promote the applications of MOFs-derived catalysts on the SO 4 •− based advanced oxidation processes (SR-AOPs) for the environmental remediation.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2021
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IF 7.963
Yawen Cai,Jinghua Feng,Xiaoli Tan,Xin Wang,Zhimin Lv,Weiwei Chen,Ming Fang,Haining Liu,Xiangke Wang
The efficient decontamination of pertechnetate ( 99 TcO 4 − ) is an essential task for managing radioactive 99 Tc in nuclear wastes . Perrhenate, (ReO 4 − ), as a nonradioactive analog, exhibits almost identical physicochemical properties as 99 TcO 4 − . Herein, a novel magnetic amine-functionalized MIL-101(Cr) (NH 2 -MIL-101(Cr)@Fe 3 O 4 ) was prepared and used to efficiently remove ReO 4 − from solution for the facile magnetic separation. A series of environmental parameters were considered to investigate the adsorption performance of NH 2 -MIL-101(Cr)@Fe 3 O 4 . Experimental results suggested that NH 2 -MIL-101(Cr)@Fe 3 O 4 has reached a satisfied adsorption capacity (~401 mg/g) and a very fast adsorption kinetics at pH 7.0. The selectivity for ReO 4 − was maintained even in the presence of interfering anions with relatively high concentrations. ReO 4 − were mainly captured by N-donor sites of the surface-decorated amine via complexation and were trapped in the cavities of modified MIL-101(Cr). NH 2 -MIL-101(Cr)@Fe 3 O 4 exhibits satisfactory adsorption performance for ReO 4 − and can be conveniently separated from wastewaters after adsorption.
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POLYHEDRON
·
2020
·
IF 2.343
Zhongmin Liu,Cong Wang,Yongchuan Wu,Longlong Geng,Xiuling Zhang,Dashuai Zhang,Hui Hu,Yongzheng Zhang,Xin Li,Wei Liu,Ping Na
The adsorption behavior of arsenic on adsorbent have been researched widely, but chemical adsorption of arsenic is uncommon. In this work, a kind of microporous metal-organic framework (MIL-125(Ti)) with columnar morphology and uniform size was solvothermally synthesized, and its chemical adsorption behavior and mechanism of arsenic were firstly investigated by experimental and simulation study. Remarkably, ultra-fast adsorption behavior and excellent arsenic removal capability was achieved. It takes only 20 min to rapidly remove 5 mg L −1 arsenic with 0.2 g L −1 MIL-125(Ti), which is far superior to the previously reported materials. Both experimental and simulation study results show that the adsorption of arsenic obeys a new chemical adsorption mechanism. Both As(III) and As(V) can easily replace the terephthalic acid ligand via competitive coordination and bind to the Ti active site of MIL-125(Ti). In addition, the reaction energy barriers for ligand substitution by H 2 O, As(III) and As(V) are 0.46, 0.33 and 0.15 eV, respectively, which further confirming that structure reforming of MIL-125(Ti) plays a key role for chemical adsorption. The study solves the difficulty of removing low concentration of arsenic and provides molecular-level understanding of the chemical adsorption mechanism of arsenic on MIL-125(Ti).
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Catalysts
·
2020
·Vol. 11
·期 1
·24
·
IF 3.52
Juan Du,Jiaxin Zhang,Tingyu Yang,Renming Liu,Zhiyi Li,Dandan Wang,Tong Zhou,Yucun Liu,Chunbo Liu,Guangbo Che
The BiOI/NH2-MIL-125(Ti) composite photocatalyst with excellent photocatalytic performance was prepared by the solvothermal method. For the BiOI/NH2-MIL-125(Ti) (BNMT) system, the contents of NH2-MIL-125(Ti) in BNMT-4, BNMT-5, BNMT-7, BNMT-9, and BNMT-10 were 4 wt %, 5 wt %, 7 wt %, 9 wt %, and 10 wt %, respectively. XRD, XPS, SEM, and TEM characterizations indicated that BiOI/NH2-MIL-125(Ti) was successfully prepared. Brunauer, Emmett, and Teller (BET) and UV–vis diffuse reflectance spectra photoelectrochemical analysis indicated that BNMT-9 can make the specific surface area and photo absorption region larger than BiOI. In addition, the separation efficiency of photogenerated carriers was improved, and the recombination efficiency was reduced. The degradation percentages of Rhodamine B (RhB) and p-chlorophenol (P-CP) reached 99% and 90% over BNMT-9 under visible light irradiation. Additionally, the catalysts had high stability. The results of the active spices trapping experiments test indicated that h+was the main active species. The possible degradation mechanism was proposed.Keywords:photocatalysis;BiOI;NH2-MIL-125(Ti);organic pollutants
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2020
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IF 7.864
Yi Ren,Mengqi Shi,Weiming Zhang,Dionysios D. Dionysiou,Junhe Lu,Chao Shan,Yanyang Zhang,Lu Lv,Bingcai Pan
A novel Fenton-like catalyst was synthesized by immobilizing nano-Fe2O3 (nFe2O3) on MIL-53(Cu). The pseudo-first-order rate constant of bisphenol A degradation in the nFe2O3/MIL-53(Cu)/H2O2 system reached 0.0123 min–1, while the values in MIL-53(Cu)/H2O2 and nFe2O3/H2O2 systems were only 0.0026 and 0.0040 min–1, respectively. The characterization of nFe2O3/MIL-53(Cu) reveals that the supreme catalytic activity of this material could be ascribed to iron–copper synergy, smaller size, and better dispersion of nFe2O3 particles. Moreover, a method of trapping Cu(I) by neocuproine was developed, which could shield Cu(I) from interacting with iron and H2O2, and thus allow quantitative differentiation of the contribution to the enhanced catalytic activity by each of the factors. Using this method, 19% of the enhancement was determined to be contributed by synergistic effect, while 24% of the enhancement was due to the smaller size and better dispersion of the nFe2O3 particles on MIL-53(Cu) support. In addition, the performance of nFe2O3/MIL-53(Cu) only dropped 10.7% after five treatment cycles in real wastewater, showing good potential in practical application. We believe this study sheds light on the tailored design of Fenton-like catalysts and elucidates the catalytic mechanisms of supported bimetallic catalysts.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2020
·
IF 3.573
Qiqi Zhou,Guijian Liu
The presence of sulfa antibiotics in water is becoming increasingly serious and actions need to be taken to establish an effective wastewater purification process for their removal. MIL-101(Cr)@AC was prepared by incorporating activated carbon into the MIL-101(Cr) framework to reduce unused voids in MIL-101. MIL-101(Cr)@AC has a high specific surface area and was successfully synthesized and activated with urea. In this study, the adsorptive removal of the sulfonamide antibiotic, sulfacetamide (SA), from wastewater was studied using urea-activated MIL-101(Cr)@AC for the first time. High SA adsorption efficiency was observed, and an adsorption equilibrium was reached within approximately 60 min. The adsorption kinetics and isotherm records were best fitted using the Langmuir model and a pseudo-second-order model, respectively. Therefore, according to the result of adsorption, a possible mechanism was proposed. Hydrogen bonding between −NH2 on the grafted urea-MIL-101(Cr)@AC and −SO2 groups in SA resulted in an increase in adsorption efficiency. In addition, urea-MIL-101(Cr)@AC exhibited excellent reusability, which is attractive for potential applications in adsorbing SA from wastewater.
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