Membranes
·
2021
·Vol. 12
·期 1
·34
·
IF 4.106
Yushu Zhang,Hongge Jia,Qingji Wang,Wenqiang Ma,Guoxing Yang,Shuangping Xu,Shaobin Li,Guiming Su,Yanqing Qu,Mingyu Zhang,Pengfei Jiang
The preparation, characterization and gas separation properties of mixed matrix membranes (MMMs) were obtained from polyimide capped with ionic liquid and blended with metal-organic frameworks (MOFs). The synthesized MOF was amine functionalized to produce UiO-66-NH2, and its amino group has a higher affinity for CO2. Mixed matrix membranes exhibited good membrane forming ability, heat resistance and mechanical properties. The polyimide membrane exclusively capped by ionic liquid exhibited good permselectivity of 74.1 for CO2/CH4, which was 6.2 times that of the pure polyimide membrane. It is worth noting that MMM blended with UiO-66-NH2demonstrated the highest ideal selectivity for CO2/CH4(95.1) with a CO2permeability of 7.61 Barrer, which is close to the 2008 Robeson upper bound. The addition of UiO-66-NH2and ionic liquid enhanced the permselectivity of MMMs, which may be one of the promising technologies for high performance CO2/CH4gas separation.Keywords:mixed matrix membrane;metal-organic frameworks;polyimide;gas separation
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NEW JOURNAL OF CHEMISTRY
·
2021
·Vol. 45
·期 37
·17332-17338
·
IF 3.591
Xue Bai,Bo Liu,Wei Zhang,Yang Wang,Yu Yu,Yang Yang,Jianping Guo
A porous Cu2O/TiO2 hybrid photocatalyst with n-type Cu2O decorated on the mesoporous TiO2 derived from MIL-125 was designed through the in situ Cu2+ ion reduction strategy. Under UV-vis light irradiation, the Cu2O/TiO2 composite with 4.2 wt% of Cu2O displayed the highest hydrogen evolution rate of 14.39 mmol h−1 g−1, which was about 9.6 and 24.8 times that of the original mesoporous TiO2 and pure Cu2O, respectively. The enhancement in photocatalytic activity can be mainly attributed to the type-I band structure formed, which can efficiently enhance the photoexcited charge carrier mobility across the phase interfaces of the Cu2O/TiO2 composite, as evidenced by the UV-DRS spectra, Mott–Schottky curves, and XPS analysis. Besides, the narrow band gap of Cu2O, conducive to the absorption of visible light, and the high specific surface of TiO2 were also found to contribute to the photoactivity enhancement. This work will provide a new perspective for the study of type-I photocatalysts.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·
IF 5.816
Kang Ye,Ziye He,Fengxi Wu,Yumin Wang,Lu Wang,Yong Cheng,Ying-Hua Zhou
Development of an efficient catalyst for ammonia preparation through electrochemical nitrogen fixation is significant and desirable to relieve the tremendous energy-consumption by the conventional Haber-Bosch process. Herein, the abundant oxygen vacancy-containing CuCeO 2 @NC composite (denoted as Cu-doped CeO 2 nanoparticles supported on carbon nitride) was fabricated by annealing melamine-incorporated metal-organic framework (MOF) of CuCe-BTC (BTC = 1,3,5-benzenetricarboxylic acid) under the reducing atmosphere of 10% H 2 /Ar. The optimized composite of Cu 0·1 CeO 2 @NC achieved a high selectivity and an outstanding electrocatalytic activity with NH 3 yield rate of 44.5 μg h −1 mg cat. −1 at −0.5 V versus a reversible hydrogen electrode , surpassing most of the reported electrocatalysts and its analogues without copper and nitrogen atoms as dopants . The favorable performance of Cu 0·1 CeO 2 @NC would be ascribed to the synergistic effect of the rich oxygen vacancies and the optimal electrical structure induced by heteroatom doping, further confirmed by X-ray photoelectron spectroscopy (XPS), electron paramagnetic resonance (EPR) spectroscopy, and Raman spectra . Moreover, the great electrochemical selectivity and durability for the longtime electrolysis had been demonstrated. This work offered an insight that the electrocatalytic performance would be regulated by heteroatomic dopants and oxygen vacancy toward MOF-derived materials.
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Reaction Chemistry & Engineering
·
2021
·Vol. 7
·期 2
·275-283
·
IF 4.239
Yan Zhang,Bi-Cong Wang,Po Wang,Xiao-Jie Ju,Mao-Jie Zhang,Rui Xie,Zhuang Liu,Wei Wang,Liang-Yin Chu
Uniform hydrogel microparticles with MOF nanoparticles for molecular co-confinement of cascade enzymes are developed by droplet microfluidics to achieve enhanced stability and reusability under harsh conditions. Water-swollen polyacrylamide hydrogel is used for constructing the microparticles; while microporous zeolitic imidazolate framework-8 (ZIF-8) nanoparticles are incorporated in the hydrogel networks for multi-enzyme co-confinement. With the ZIF-8 nanoparticles as armour, the multiple enzymes in the microparticles show good stability for efficient biocatalytic cascades under harsh conditions. This is demonstrated by using glucose oxidase (GOx) and horseradish peroxidase (HRP) as typical cascade enzymes. The hydrogel microparticles with both GOx and HRP confined in their ZIF-8 nanoparticles exhibit enhanced stability for efficient biocatalytic cascades and storage, after treatment under harsh conditions involving high temperature, UV light, and protease. Moreover, the hydrogel microparticles allow easy recycling and good reusability after repeated treatment at high temperature (80 °C). This work provides a simple and efficient strategy to create multiple-enzyme-loaded microcarriers with good stability and reusability for biocatalytic cascades.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2021
·
IF 4.539
Qun Liu,Kun Xu,Guangxu Hu,Fanming Zeng,Xiao Li,Chun Li,Yu Zhang
MIL-101(Cr)/polyacrylamide/chitosan (named as MIL-101(Cr)/PAM/CSA) composite aerogel with large surface area is synthesized by incorporating MIL-101(Cr) into polyacrylamide/chitosan composite aerogel and used for efficient 2, 4-Dichlorophenoxyacetic acid adsorption. MIL-101(Cr)/PAM/CSA and polyacrylamide/chitosan composite aerogels exhibit good underwater superelastic properties with multi-level network synergistic cross-linking. After introducing MIL-101(Cr) with the mass loading of 30%, the specific surface area of the composite aerogels enlarge from 58.15 m 2 g −1 to 310.94 m 2 g −1 . MIL-101(Cr)/PAM/CSA exhibits high adsorption capacity of 302.45 mg g −1 for 2, 4-Dichlorophenoxyacetic acid (2, 4-D) and stable recycling capability. This work provides a general and effective method to synthesize composite aerogel with underwater superelastic properties, hierarchical pores and large surface area, promising to realize regeneration after compression with reduced solvent usage and costs.
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Nanoscale
·
2021
·Vol. 14
·期 5
·1796-1806
·
IF 7.79
Wenyan Yin,Milin Zhang,Jingyuan Liu,Khaled Tawfik Alali,Jing Yu,Jiahui Zhu,Peili Liu,Rumin Li,Jun Wang
Electrochemical sensors using ionic liquids as electrolytes for oxygen detection are now getting more and more attention. Recently, an ionic liquid combined with an electrochemically active catalyst system has become popular for boosting the sensing performance of oxygen sensors. In this work, the imidazolyl-based ionic liquid 1-butyl-2,3-dimethylimidazole bis((trifluoromethyl)sulfonyl)imide [Bmmim][TFSI] is first prepared by a facile two-step method. Subsequently, a transition metal and N-codoped porous carbon oxygen reduction electrochemical catalyst Cu–N/C is synthesized by calcining the Cu-doped ZIF-8 precursor and then blending it in different ratios with the ionic liquid [Bmmim][TFSI] as composite electrolytes for oxygen detection. The composite electrolyte Cu–N/C/[Bmmim][TFSI] exhibits increased responses in cyclic voltammetry (CV) and chronoamperometry (CA) relative to that of the pure ionic liquid. Furthermore, the CV and CA data show that 6% Cu–N/C/[Bmmim][TFSI] has the optimum oxygen sensing response with an enhanced reduction peak current, a sensitivity of 0.1678 μA/[% O2] and a good linear fitting coefficient of 0.9991. In conclusion, the results confirm the success of using Cu–N/C as an electrochemical catalyst composed of the Cu–N/C/[Bmmim][TFSI] electrolyte for improving the responsivity, stability and sensitivity towards a wide range of oxygen concentrations.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
·
IF 7.312
Wenyan Shi,Xiaolong Han,Fang Bai,Chao Hua,Xingzhong Cao
The metal–organic framework MOF-505 particles were synthesized and incorporated into the polyethylene glycol (PEG) matrix to prepare mixed matrix membranes. A series of methods were used to characterize the structure and morphology of MOF-505 particles and membranes. The prepared MOF-505 had a well-developed pore structure, a large number of metal sites for selective adsorption of thiophene and good compatibility with polymer matrix. Accordingly, the desulfurization performance of the membrane was improved effectively. The effects of the content of MOF-505, operating temperature and feed sulfur content on membrane performance were investigated by pervaporation experiments. The membrane with 3 wt% MOF-505 showed the optimal desulfurization performance with a permeation flux of 2.66 kg/(m 2 ·h) and an enrichment sulfur factor of 8.15, which were increased by 158% and 25% versus pristine membrane, respectively.
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INORGANIC CHEMISTRY
·
2021
·
IF 5.165
Hao-Jing Ding,Ying Zhang,Xi Wang,Qiu-Ying Lin,Shu-Ming Zhang,Mei-Hui Yu,Ze Chang,Xian-He Bu
The construction and modulation of hierarchical pore structure in metal-organic frameworks (MOFs) has become a hot topic owing to the advantages of hierarchical pore MOFs (HP-MOFs) in matter storage and mass transfer related applications. Herein, we report the engineering of crystalline defect in a bimetallic MOF for the construction and tuning of HP-MOF. A microporous MOF system showing metal-center-dependent water stability, namely, {[M3F(bdc)3 tpt] (solvents)}n (M = Zn2+ and Ni2+, H2bdc = 1,4-benzenedicarboxylic acid, tpt = 2,4,6-tris(4-pyridyl)triazine), was utilized as a platform for the construction of HP-MOF. By tuning the Zn2+/Ni2+ ratio in the reactant, a bimetallic MOF with a highly tunable Zn2+/Ni2+ ratio could be obtained. The relatively labile Zn2+-based coordination bonding in the bimetallic MOF could be readily and targeted broken through water treatment for the engineering of crystalline defects-based hierarchical pore structure. The resultant HP-MOF reveals a dramatically increased pore volume with the presence of mesopore and macropore. In addition, the anionic framework of HP-MOF could be utilized for the selective adsorption of a cationic dye methylene blue, and a relatively high capacity (250 mg·g–1, five times compared with the pristine microporous MOF) could be achieved.
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Biosensors-Basel
·
2021
·Vol. 11
·期 7
·204
·
IF 5.519
Yanyan Cheng,Ling Liang,Fanggui Ye,Shulin Zhao
Metal–organic framework (MOF) nanozymes, as emerging members of the nanozymes, have received more and more attention due to their composition and structural characteristics. In this work, we report that mixed-valence state Ce-MOF (MVCM) has intrinsic haloperoxidase-mimicking activity. MVCM was synthesized by partial oxidation method using Ce-MOF as a precursor. In the presence of H2O2and Br−, MVCM can catalyze oxidative bromination of chromogenic substrate phenol red (PR) to produce the blue product bromophenol blue (Br4PR), showing good haloperoxidase-like activity. Because of the special chromogenic substrate, we constructed a ratiometric colorimetric-sensing platform by detecting the absorbance of the MVCM-(PR, Br−) system at wavelengths of 590 and 430, for quantifying H2O2, where the detection limit of the H2O2is 3.25 μM. In addition, the haloperoxidase-mimicking mechanism of the MVCM is proposed. Moreover, through enzyme kinetics monitoring, theKm(H2O2and NH4Br) of the MVCM is lower than that of cerium oxide nanomaterials, indicating that the MVCM has a stronger binding affinity for H2O2and NH4Br than other materials. This work provides more application prospects for the development of nanozymes in the field of biosensors in the future.Keywords:nanozyme;Ce-MOF;haloperoxidase-like activity;ratiometric colorimetric;hydrogen peroxide
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Chemistry-An Asian Journal
·
2020
·Vol. 16
·期 1
·64-71
·
IF 4.056
Tao Zhao,Dong Wang,Chen Cheng,Dazhong Zhong,Genyan Hao,Guang Liu,Jinping Li,Qiang Zhao
Graphical A ZIF@MIL heterostructure was successfully prepared by an in situ solvothermal method. Compared to pure ZIF-67 and MIL-100, the heterostructure possesses a larger electrochemical surface area and exhibits a remarkable catalytic performance with a low overpotential of 232 mV and a small Tafel slope of 57 mV dec −1 at 10 mA cm −2 . Although metal-organic frameworks have proven to be excellent electrocatalytic materials, their application as electrode materials remains limited. The preparation of heterostructures is considered an effective method to improve catalytic activity. Herein, we describe the design and assembly of a dual-MOF heterostructure (CoNi−ZIF-67@Fe−MIL-100, denoted ZIF@MIL). Specifically, we grew a layer of MIL-100 in situ on a bimetallic ZIF-67 surface using a solvothermal method. We demonstrate that the ZIF@MIL has remarkable OER electrocatalytic performance, requiring a low overpotential and showing a small Tafel slope, compared to pure ZIF-67 and MIL-100 in 1.0 m KOH. More importantly, it has excellent operational durability for 50 h at 100 mA cm −2 . The high catalytic activity of ZIF@MIL can be attributed to the heterostructure that can expose more active sites, the synergistic effect between ZIF-67 and MIL-100, and improvement of electron transfer ability. Our work provides a new way to design and prepare dual-MOF crystals with different structures as electrocatalysts.
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NEW JOURNAL OF CHEMISTRY
·
2020
·Vol. 44
·期 48
·21085-21091
·
IF 3.288
Hongli Zhu,Jing Huang,Huijun Chen,Xiaomiao Feng
In recent years, self-propelled micromotors have attracted great attention due to their intelligent properties. To obtain a bubble-propelled micromotor, additional catalysts are required, which are usually expensive, toxic, and unstable, and lead to uncontrolled motion. To overcome these limits, ZIF-67, as a kind of MOF material, was chosen as a micromotor precursor; porous carbon decorated with magnetic Co nanocomposites (Co@PCs) could be obtained via an annealing process involving ZIF-67. These Co@PCs were used as micromotors for drug delivery, and were mass-producible, stable, and biocompatible. Due to the presence of magnetic Co, their motion could be controlled in a magnetic field. Co@PCs carbonized at 600 °C were self-propelled at a speed of 27.68 μm s−1, which corresponded to a relative speed of about 7.92 body-lengths s−1 at a fuel concentration of 5% with a lifetime of about 60 minutes. Furthermore, Co@PCs could be used as nanocarriers for the loading and release of the anticancer drug doxorubicin.
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CHEMOSPHERE
·
2020
·
IF 5.778
Rajendran Ramachandran,Thangavel Sakthivel,Minzhang Li,Haiquan Shan,Zong-Xiang Xu,Fei Wang
Nickel-based metal-organic framework (Ni-MOF) was employed as a sacrificial template for the preparation of nickel-cobalt layered double hydroxide (NiCo-LDH) under different hydrolysis time. The template etching rate varied at different hydrolysis time, resulting in variations of the structural and morphology of NiCo-LDHs. The NiCo-LDH/10 sample showed a large specific surface area and the well-oriented larger dimension of thinner sheets due to the sufficient in-situ etching of the Ni-MOF template. The NiCo-LDH/10 was an excellent heterogeneous catalyst to activate peroxymonosulfate (PMS) for highly efficient Reactive Red-120 dye degradation. The results exhibited that the degradation efficiency of the NiCo-LDH/10-PMS catalyst was 89% for RR-120 dye within 10 min in the presence of the PMS system, which is higher than other NiCo-LDHs. Moreover, the other influencing factors such as PMS concentration, catalyst dosage, initial pH were also investigated towards degradation. The radical quenching measurement proved that the sulfate (SO 4 •− ) and hydroxyl (OH • ) had been indicated as the primary radicals. Besides, the NiCo-LDH/10-PMS catalyst showed excellent reusability even after five consecutive cycles (83.6% of the degradation efficiency). This work offer insight study on the construction of controlled morphology NiCo-LDH heterogeneous structure for high-efficiency PMS activation .
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