APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
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IF 19.503
Fang Li,Yuhui Tian,Shibiao Su,Changshui Wang,Dong-Sheng Li,Dandan Cai,Shanqing Zhang
High performance and cost-effective electrocatalysts are crucial to the oxygen evolution reaction (OER) in water splitting. Herein, we use density functional theory (DFT) calculation to systematically explore the catalytic activities of single-metallic organic frameworks (s-MOFs, such as Fe 36 C 108 O 156 ), dual-metallic organic frameworks (d-MOFs, such as Fe 26 Co 10 C 108 O 156 , Fe 30 Ni 6 C 108 O 156 ), and tri-metallic organic frameworks (t-MOFs, such as Fe 26 Ni 2 Co 8 C 108 O 156 ) for electrocatalytic OER. The DFT calculation and experimental results suggest that the OER performance could be promoted with reduced activation energy barrier and accelerated kinetics by introducing Co and Ni into the unit cell of Material of Institute Lavioisier (MIL). The optimized t-MOFs exhibited an ultra-low overpotential of only 200 mV at the current density of 10 mA cm −2 and a small Tafel slope of 34 mV dec −1 . This work proposes that the t-MOFs induced multi-metallic active sites and synergetic effect are promising strategies in designing highly efficient and robust OER electrocatalysts.
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JOURNAL OF HAZARDOUS MATERIALS
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2021
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IF 10.588
Cheng Zeng,Yan Wang,Tong Xiao,Zhicheng Yan,Jinquan Wan,Quanmo Xie
To improve the efficacy of organic pollutant removal using sulfate radicals, we designed MIP@C-Fe-Nx, a molecularly imprinted material capable of targeting the degradation of tetrabromobisphenol A (TBBPA), which can be used as both adsorbent and catalyst to recognize and degrade Tetrabromobisphenol A (TBBPA) accurately, and the final removal rate of TBBPA can reach 104.6 mg·g −1 . Based on the synergistic effects of MIP@C-Fe-Nx on the excellent organic pollutant recognition and catalytic performance, low concentrations of TBBPA can be pre-targeted, concentrated, and fixed on the surface of MIP, and degraded simultaneously in-situ by·OH and SO 4 •- which are produced by activating PS with C-Fe-Nx. Recognition experiments demonstrated that MIPs had perfect performance in recognizing and adsorbing TBBPA and debromination intermediates. The DFT calculations and HPLC-MS analysis indicated that MIP@C-Fe-Nx had a targeted recognition and accumulation for TBBPA and debromination intermediates, for example, dibromobisphenol A, monobromobisphenol A, and bisphenol A, thus avoid the formation of toxic intermediates causing secondary contamination.
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JOURNAL OF SOLID STATE CHEMISTRY
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2019
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IF 2.291
Qian-Qian Liu,Xian-Jun Weng,Ke-Fen Yue
Three novel metal-organic frameworks (MOFs) formulated as [Cd(5-mipa)(bpe) 1.5 ·0.8DMF] n ( 1 ), [Zn(5-mipa)(bpe)] n ( 2 ), and {[Ni(5-mipa)(bpe)]·0.4IPA} n ( 3 ) (IPA = iso-propyl alcohol) were successfully obtained via solvothermal reaction between the corresponding transition metal nitrates and 5-methylisophthalic acid (5-H 2 mipa), 1,2-bis(4-pyridyl)ethylene (bpe). All compounds were adequately characterized, and their structures were verified by single-crystal X-ray diffraction. The solid-state luminescence properties of three complexes were investigated at ambient temperature. 1 shows high sensitivity for Fe 3+ and nitrobenzene by the luminescence quenching effect with the low detection limit 7.0 × 10 −5 M and 6.84 × 10 −5 M, respectively, and its mechanisms have been studied in detail. Additionally, the selective adsorption of compounds 2 and 3 to anionic dyes (Methyl Orange (MO) and Congo Red (CR) and cationic dye Methylene Blue (MB) were examined. The results demonstrated that 2 and 3 showed good adsorption properties for MO and CR anionic dye molecules.
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ACS Sustainable Chemistry & Engineering
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2019
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IF 6.97
Lei Wang,Wenjing Zhi,Jing Wan,Juan Han,Chunmei Li,Yun Wang
Enhancing the stability and reusability of enzymes by encapsulating them within a powerful class of porous materials termed metal–organic frameworks (MOFs) has been demonstrated by recent studies. However, in all of these reports, the stability of MOFs under acidic conditions was a major issue for enzymes with catalytic activity at low pH. The objective of this study is to encapsulate the β-glucosidase (β-G) into the Cu-MOF due to its acidic stability, using a coprecipitation approach. Indeed, the as-prepared β-G@Cu(PABA) biocomposite with high encapsulation efficiency exhibited enhanced resistance to acidic and thermal conditions as well as organic solvents. Importantly, the β-G@Cu(PABA) biocomposite showed superior reusability, retaining 90% of activity even after 10 cycles. Using the hydrolysis of carboxymethylcellulose (CMC) as a mode, the mixture of β-G@Cu(PABA) biocomposite and coimmobilized cellulase afforded 98% glucose yield, which was twofold enhancement when compared with coimmobilized cellulose alone. The β-G@Cu(PABA) biocomposite and coimmobilized cellulase could been easily recovered and recycled to still retain 70% productivity in the eight cycles for hydrolyzing CMC. This discovery for the first time highlights the potential of Cu-MOF in preserving the enzymes under acidic conditions. The developed β-G@Cu(PABA) biocomposite by coprecipitation approach affords a valuable platform for enzyme-based industrial applications.
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MICROPOROUS AND MESOPOROUS MATERIALS
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2019
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IF 4.182
Shi-Wen Lv,Jing-Min Liu,Hui Ma,Zhi-Hao Wang,Chun-Yang Li,Ning Zhao,Shuo Wang
Nowadays efficient and rapid removal of organic dyes from wastewater is still a complicated task with great challenge. Herein, the amino groups functionalized UiO-66 (denoted as UiO-66-NH 2 ) was synthesized via a one-step process and then applied in simultaneous removal of methyl orange (MO) and methylene blue (MB) for the first time. The as-prepared UiO-66-NH 2 showed excellent adsorption ability to both MO and MB, and the maximum adsorption capacities were as high as 148.4 (MO: pH = 5, T = 25 °C) and 549.6 (MB: pH = 9, T = 25 °C) mg/g, respectively. Significantly, UiO-66-NH 2 exhibited highly pH-dependent selective adsorption for MO and MB. More interestingly, the simultaneous removal of MO and MB from the MO/MB mixture solution could be achieved by UiO-66-NH 2 under neutral condition. The adsorption mechanisms and reusability were also investigated. Overall, UiO-66-NH 2 could be a perfect candidate for removing MO and MB application in dye-containing wastewater treatment . And the results from this study also provided some new insights for the treatment of wastewater containing various dyes.
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Catalysis Science & Technology
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2019
·Vol. 10
·期 2
·315-322
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IF 5.726
Yanjing Hu,Jian Zhang,Hang Huo,Zhe Wang,Xianzhu Xu,Yulin Yang,Kaifeng Lin,Ruiqing Fan
Designing and preparing effective acid–base tandem catalysts is one of the research hotspots at present because assembling antagonistic active sites in one catalyst is still a challenge. In this work, amine-functionalized bimetallic metal–organic frameworks (MIL-101(Al/Fe)–NH2 (X)) were synthesized through a rapid reflux method and acted as acid–base bifunctional catalysts for tandem reaction (deacetalization–Knoevenagel condensation reaction). The bimetallic MOF catalysts exhibit enhanced catalytic activity when compared with monometallic catalysts either MIL-101(Al)–NH2 or MIL-101(Fe)–NH2. The superior performance of MIL-101(Al/Fe)–NH2 (X) has been attributed to the synergistic effect between Al3+ and Fe3+ ions and the hierarchical pore structure. Moreover, the as-synthesised samples showed robust stability, excellent recyclability, and durable catalytic activity.
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Nanomaterials
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2018
·Vol. 8
·期 4
·248
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IF 3.504
Fuhua Wei,Ding Chen,Zhao Liang,Shuaiqi Zhao
Using a microwave-assisted ball-milling approach, Fe-based metal-organic frameworks (Fe-MOFs) were prepared from FeSO4·7H2O and trimesic acid. Scanning electron microscopy, Fourier-transform infrared spectrometry, X-ray, and thermogravimetric analysis were utilized to characterize the thermal stability and structure of the prepared Fe-MOFs. These Fe-MOFs were used to remove organic dyes from aqueous solutions. Specifically, they removed 96.97% of 23.3592 mg/L of Congo red in a 200 mL solution within 300 min of treatment with natural light at 15 °C. Likewise, 88.21 and 70.90% of 22.7527 mg/L of Orange II and 17.8326 mg/L of Rhodamine B, respectively, were removed from 200 mL solutions within 300 min of treatment at 15 °C. At 35 °C, 99.57, 95.98, and 99.38% of 23.3855 mg/L of Congo Red, 22.7365 mg/L of Orange II, and 17.9973 mg/L of Rhodamine B, respectively, were removed from 200 mL solutions within 300 min of treatment. The adsorption kinetics were investigated and the pseudo-first-order kinetic model was found to be superior to the pseudo-second-order kinetic model. Overall, using metal-organic frameworks to treat dye wastewater was found to be inexpensive, feasible, and efficient. Therefore, this material has future prospects in research and applications in the purification of wastewater.Keywords:wastewater treatment;metal-organic frameworks;dye removal;microwave-assisted ball milling
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SENSORS AND ACTUATORS B-CHEMICAL
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2018
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IF 5.667
Hongli Zheng,Huan Yi,Hong Dai,Dandan Fang,Zhensheng Hong,Danmei Lin,Xiangqin Zheng,Yanyu Lin
Herein, an effective integrated electrochemiluminescence (ECL) bioprobe was constructed based on F-couSiPc as co-reaction accelerator of tris (2,2′-bipyridine-n,n’)-, dichloride, hexahydrate (II) (Ru(bpy) 3 2+ ) and TiO 2 MOFs as carrier for developing a competitive-type ECL strategy for the sensing of deoxynivalenol (DON). Initially, TiO 2 MOFs with high specific surface area and regular pore structure was employed to immobilize Ru(bpy) 3 2+ and Mercapto-beta-cyclodextrin (β-CD), then sensitizer of F-couSiPc was introduced into the system by encapsulating into the cup-shaped cavity of β-CD, which mainly ascribed to the supermolecular self-assembly behavior, perfectly avoiding the aggregation of F-couSiPc. Due to the shortened electronic transmission distance, reduced energy loss and less reagent consumption, the integrated ECL reaction pattern between the luminescent Ru(bpy) 3 2+ and sensitizer of F-couSiPc has shown improved luminous efficiency compared with the common intermolecular ECL reactions. Meanwhile, the (3-Aminopropyl) triethoxysilane (APTES), perylene-3,4,9,10-tetracarboxylic acid (PTCA) and carbon nanohorn (CNHs) nanohybrid (APTES-PTCA@CNHs), combing the remarkable advantages of CNHs with the desirable electronic and optical properties of PTCA, served as matrix to immobilize antigen (DON) with an increasing amount, and on account of the high affinity between the APTES and DON, a stable ECL performance was obtained. Based on the competitive immunoreactions, a facile and sensitive ECL immunosensor was constructed for the detection of DON, with excellent linear range from 0.1 pg/mL to 20 ng/mL and a detection limit of 0.03 pg/mL (S/N = 3).
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ACS Catalysis
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2015
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IF 9.312
Kui Shen,Liang Chen,Jilan Long,Wei Zhong,Yingwei Li
Although MOFs supporting noble metal nanoparticles (NPs) have been widely used in heterogeneous catalysis, they are still limited in catalytic efficiency on a per-noble-metal-atom basis. Here we developed a MOFs-templated strategy to non-noble metal @noble metal core–shell nanocatalysts, which could far surpass the traditional MOFs supporting noble NPs in catalytic properties, by using MOFs-derived metal NPs as sacrificial templates to reduce noble metal ions via galvanic replacement reaction. As a model system, Co@Pd core–shell NPs embedded in the N-doped carbon matrix (Co@Pd/NC) were synthesized with an average size of ca. 9.4 nm and a ultrathin Pd shell by using ZIF-67 and Pd(NO3)2 as the precursor and Pd source, respectively. The highly exposed Pd atom on Co nanoparticles made it an attractive catalyst with high efficiency. When being used in the hydrogenation of nitrobenzene, the Co@Pd/NC exhibited an unprecedented high activity over Pd-based catalysts, yielding 98% conversion after 45 min reaction, which was far more active than the pristine ZIF-67 and MIL-101 supporting Pd NPs (with 40% and 3% conversion after 90 min reaction, respectively) under identical conditions, suggesting its overwhelmingly better performance than MOFs supporting noble NPs. We anticipated that this strategy would form the basis for developing a new class of MOF-templated core–shell nanocatalyst with potential applications in numerous catalytic reactions.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2016
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IF 3.014
Yaqin Chen,Jiafeng Wu,Weisen Yang,Yuanyuan Fu,Rihui Zhou,Shouhui Chen,Lixue Zhang,Yonghai Song,Li Wang
Transition metal oxides@carbon(C) nanocomposites with hierarchical three-dimensional (3D) core-shell nanoarchitectures, large surface area and high electrical conductivity as anode materials for lithium ion batteries (LIBs) are very desirable. Herein, we developed a simple and feasible route to fabricate novel hierarchical 3D ball-in-ball ZnO/ZnFe 2 O 4 @C nanospheres with well-defined hollow microstructures via one-step carbonization of Zn/Fe-metal organic frameworks for the first time. The as-prepared hierarchical 3D ball-in-ball ZnO/ZnFe 2 O 4 @C nanospheres were carefully characterized by scanning electron microscopy, energy dispersive X-ray spectroscopy, X-ray photoelectron spectroscopy, X-ray powder diffraction, thermogravimetric analysis , N 2 adsorption/desorption isotherm, transmission electron microscopy and electrochemical techniques . The results showed ultrafine ZnO and ZnFe 2 O 4 nanocrystals were uniformly encapsulated by few carbon layers which was derived from in-situ carbonization of the organic ligands. Benefiting from their special hollow nanoarchitectures, ultrafine ZnO and ZnFe 2 O 4 nanocrystals encapsulated by a few carbon layers, large specific surface area and high electrical conductivity, the hierarchical 3D ball-in-ball ZnO/ZnFe 2 O 4 @C nanospheres presented high reversible capacities of 1283 and 1100 mA h g −1 after first 100 cycles and the following 100 cycles at current density of 100 and 200 mA g −1 , respectively. A high specific capacity of 155 mA h g −1 was obtained at relatively large current rates of 20 A g −1 .
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Xinxin Wang,Jianmin Zhou,Yanlin Zhu,Can Yu,Di Sun,Yuanfei Yao,Lili Feng,Piaoping Yang,Yang Zhou
Radiotherapy (RT) represents a cornerstone therapeutic approach in clinical practice for locally control of hepatocellular carcinoma (HCC). However, its efficacy in treating liver cancer is significantly hampered by radiation resistance, which attributed to the insufficient reactive oxygen species (ROS) generation within the tumor microenvironment (TME). To augment RT efficacy, we have developed a novel radiosensitizer termed PTFM. The compound has the features of meso -tetra (4-carboxyphenyl) porphine (TCPP) porphyrin metal–organic frameworks (MOF, PCN-224(Fe)) co-doped with high-atomic element Ta. Under X-ray excitation, the porous PTFM acts as a proficient radio-sensitization, absorbs X-ray energy to promote hydroxyl radicals generation for RT, thereby disrupting the redox balance and intensifying the cytotoxic effect on tumor cells. The incorporation of Fe 3+ into the macrocycle of TCPP within the MOFs shell, facilitates the reactions with GSH and H 2 O 2 in the TME, leads to ROS production that promotes ferroptosis and apoptosis, while also releases O 2 to alleviate tumor hypoxia. Furthermore, PTFM with thermo-metal serves as a dual-mode MR/CT imaging contrast agent, enabling precise RT monitoring and imaging guidance. In conclusion, the radiosensitizer we developed integrates dual-mode imaging capabilities and enhances RT sensitization for HCC through ROS-induced cell apoptosis and ferroptosis, thereby ameliorating tumor hypoxia.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2024
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IF 3.8
Douhao Yang,Ruiting Jian,Jianjun Yan,Ao Zhang,Bowen Liu,Zhongwei Liu
Defect engineering has a great effect on the properties of metal–organic frameworks (MOFs). In this study, the defective UiO-66-NH2 MOFs are successfully prepared by a rapid Ar plasma modification method. At certain experimental conditions (15 W radio frequency input power, 20 Pa working pressure, and 120 s Ar plasma modification time), the afforded UiO-66-NH2 shows significant enhancement in photocatalytic reduction of Cr(VI), and a maximum reduction efficiency of 68.5% is obtained. Advanced characterizations show that the plasma treatment generates missing-linker defects within the UiO-66-NH2 structure, which can enhance the separation of photogenerated electrons and holes and improve the photoreduction capability. The findings not only contribute to a better understanding of the relationship between the structure and performance of MOFs but also provide a simple approach for defect engineering of MOFs.
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