APPLIED ORGANOMETALLIC CHEMISTRY
·
2020
·Vol. 34
·期 12
·e5972
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IF 3.14
Huihui Song,Na Wang,Xiatong Shi,Hao Meng,Yide Han,Junbiao Wu,Junli Xu,Yan Xu,Ting Sun,Xia Zhang
Probing into the new heterostructure based on metal–organic frameworks (MOFs) and optimizing their photocatalytic efficiency under solar energy irradiation are one of hot topics in extending applications of MOFs in photocatalytic technology. Inspired by the excellent visible-light responses and photocatalytic activities of inorganic silver salts, in this work, we focused on the construction of hybrid photocatalysts involving Ag-MOF and silver cyanamide (Ag 2 NCN). Two opposite in situ synthesis routes were adopted, which are hydrothermally producing Ag-MOF in the presence of Ag 2 NCN (route A) or precipitating Ag 2 NCN in the existence of Ag-MOF (route B), and the mass ratio of Ag 2 NCN vs. Ag-MOF was optimized. The morphology and structure character show that the synthetic routes have no obvious influences on the crystal structure, but change the morphology and size of final hybrid photocatalysts. The photocatalytic degradation of Rhodamine B under simulated solar energy has been tested to evaluate the photocatalytic activities for resulting hybrids. Compared to single Ag-MOF and Ag 2 NCN, the enhanced photocatalytic rates are represented by the hybrids. The electrochemical analyses and the active species trapping experiments were conducted to clarify the photocatalytic mechanism for resulting hybrids. The good recycling photocatalytic results indicate the prospect applications of Ag-MOF based hybrid photocatalysts.
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NEW JOURNAL OF CHEMISTRY
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2020
·Vol. 44
·期 48
·21085-21091
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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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MOLECULES
·
2020
·Vol. 25
·期 20
·4673
·
IF 3.267
Zhu Ding,Xiao Min Zhang,Xue Chang,Shuo Wang,Dan-Hong Wang,Ming Hui Zhang,Tian Hao Zhang
Metal-Organic Framework (MOF) materials are often modified or functionalized, and then the crystal size and morphology of MOF materials are changed. In the process of preparing UiO-66 confined phosphomolybdic acid (PMA) composites (PU), the TiF4-modified PU (PMA + UiO-66) composite catalyst (TiF4-PU) was successfully synthesized by adding titanium tetrafluoride, and the catalytic desulfurization activity was excellent. Similarly, the reaction mechanism was investigated by means of infrared spectroscopy, Raman spectroscopy, XPS, and UV/Vis spectroscopy. The results show that the addition of TiF4not only changes the appearance and color of the catalyst, but also changes the valence distribution of the elements in the catalyst. The number of oxygen vacancies in the MOF increases due to the addition of TiF4, and more electrons are transferred from the Zr-MOF to PMA to form more Mo5+, which improved the performance of oxidative desulfurization in comparison. Thus, a stronger strong metal-support interaction (SMSI) effect is observed for TiF4-modified PU catalysts. In addition, the quenching experiment of free radicals shows that ·OH radical is the main active substance in the oxidative desulfurization reaction over TiF4-PU catalyst.Keywords:MOF materials;Raman spectroscopy;Zr-MOF;SMSI;TiF4-PU;oxidative desulfurization
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高影响因子
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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RSC Advances
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2020
·Vol. 10
·期 44
·26246-26255
·
IF 3.119
Zhu Ding,Shuo Wang,Xue Chang,Dan-Hong Wang,Tianhao Zhang
Photocatalytic nitrogen fixation has attracted extensive attention in recent years. Studies have shown that catalytic materials with O, N and other defects can effectively reduce the bond energy of NN triple bond when N2 is adsorbed on the defects. As an outstanding non-metallic catalyst, g-C3N4 has been widely studied in the field of photocatalytic catalysis, and the nitrogen-defected C3N4 shows promoted photocatalytic activity. Herein, nano-size MOF-74 particles (<20 nm) was dispersed on nitrogen-defected C3N4 thin film (∼4 nm) via a simple sol–gel method. The combination of Nano-MOF and defected film C3N4 could effectively improve the photocatalytic activity of nitrogen fixation through Z-scheme mechanism compared with pure defected film C3N4.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2020
·
IF 3.573
Yang Zhao,Jiafu Shi,Xueying Wang,Weiran Li,Yizhou Wu,Zhongyi Jiang
Porous carbon materials are highly attractive in the research field of adsorption, particularly, for treating organic pollutants in wastewater, of which the facile yet generic method is highly pursued. In our study, carbon aerogels bearing a hierarchically structured surface were prepared through direct carbonization of Biomass@metal–organic framework (MOF) composites. Briefly, MIL-53, one typical MOF material, was in situ assembled on the surface of kapok fibers, a kind of fibrous biomass with the highest hollow degree on earth, through surface-induced mineralization. After direct carbonization, the resultant carbon aerogel, termed Biomass-C@MIL-53-C, with a hierarchically structured surface, was formed. Biomass-C@MIL-53-C exerted superwater repellence with the water contact angle of >140°, which showed adsorption capacities 35–119.5 times their own weight toward various kinds of oils and organic solvents. Additionally, Biomass-C@MIL-53-C could retain 77.2–96.7% of their initial adsorption capacity after eight adsorption-squeezing cycles, outperforming its counterpart, Biomass-C aerogel. Other organic pollutants, such as dyestuffs, in wastewater could also be effectively removed by Biomass-C@MIL-53-C, showing the potential of our biomass-derived carbon aerogels in a broad range of application areas for environmental protection.
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Chemical Science
·
2020
·Vol. 11
·期 15
·3978-3985
·
IF 9.346
Jing Cao,Wenjie Ma,Kangjie Lyu,Lin Zhuang,Hengjiang Cong,Hexiang Deng
We report the design and synthesis of a titanium catecholate framework, MOF-217, comprised of 2,4,6-tri(3,4-dihydroxyphenyl)-1,3,5-triazine (TDHT) and isolated TiO6 clusters, with 2-fold interpenetrated srs topology. The dynamics of the organic linker, breaking the C3h symmetry, allowed for reversible twist and sliding between interpenetrated frames upon temperature change and the inclusion of small molecules. Introduction of 28 wt% imidazole into the pores of MOF-217, 28% Im-in-MOF-217, resulted in four orders of magnitude increase in proton conductivity, due to the appropriate accommodation of imidazole molecules and their proton transfer facilitated by the H-bond to the MOF structure across the pores. This MOF-based proton conductor can be operated at 100 °C with a proton conductivity of 1.1 × 10−3 S cm−1, standing among the best performing anhydrous MOF proton conductors at elevated temperature. The interframe dynamics represents a unique feature of MOFs that can be accessed in the future design of proton conductors.
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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
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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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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2019
·
IF 3.375
Xiao-Wei Liu,Yi-Ming Gu,Tian-Jun Sun,Ya Guo,Xiao-Li Wei,Sheng-Sheng Zhao,Shu-Dong Wang
The highly efficient separation of CH4/N2 remains a great challenge, but it is vital to make the most of diverse natural gas resources and contributes to mitigating global warming. In this work, two isostructural metal–organic frameworks (MOFs), M-MA-BPY where M is Co and Ni, were elaborately selected and synthesized to serve the purpose. These MOFs were thoroughly characterized and found to have favorable framework flexibility, endowing them with narrow and uniform pore networks suitable for the adsorptive separation of CH4/N2. Further studies revealed the M-MA-BPY MOFs’ excellent stability toward water and moist air. Pure gas adsorption experiments suggested they have decent CH4 capacities (0.92 and 1.01 mmol·g–1 for Co- and Ni-MA-BPY), prominent CH4/N2 selectivities (7.2 and 7.4 for Co- and Ni-MA-BPY, IAST selectivity with equimolar CH4/N2 gas mixture) at 298 K and 1 bar, and desirable heats of adsorption for CH4 (22.8 and 23.5 kJ·mol–1 for Co- and Ni-MA-BPY). Dynamic breakthrough experiments and multiple adsorption–desorption cycling tests for CH4/N2 binary mixtures with different gas ratios of 5:95, 15:85, 30:70, and 50:50 (v/v) confirmed the high separation performance of M-MA-BPY MOFs. Together with their relatively simple synthesis and cheap raw reagents, this work demonstrates M-MA-BPY MOFs are very promising adsorbents for the capture of methane from low-quality natural gas resources in ambient conditions.
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NEW JOURNAL OF CHEMISTRY
·
2019
·Vol. 43
·期 42
·16546-16554
·
IF 3.069
Chang Liu,Jing Qiao,Xue Zhang,Dongmei Xu,Nannan Wu,Longfei Lv,Wei Liu,Jiurong Liu
In this paper, we report the facile synthesis of CoNi/C nanocomposites derived from bimetallic metal organic frameworks for electromagnetic wave absorption applications. The effects of carbonation temperature on the phase structure, morphology and microwave absorption properties of the derived nanocomposites were thoroughly studied. Micro-structure characterization results indicated that the obtained CoNi/C composites are composed of numerous fine particles with the size of 20 nm, and in the composites, Ni, Co, and C elements are uniformly distributed. Electromagnetic wave absorption property evaluation showed that CoNi/C obtained at 650 °C outperformed those samples prepared at 500, 800 or 950 °C. The minimum reflection loss (RL) of −74.7 dB could be achieved with a thickness of 1.8 mm at 15.6 GHz. The effective absorption bandwidth (RL ≤ −10 dB) ranged from 2.9 GHz to 18 GHz. This study shows that these porous Co–Ni/C nanocomposites derived from MOFs are attractive candidates as electromagnetic (EM) wave absorbers due to the combined advantages of excellent impedance matching and strong interfacial loss between metallic NPs and porous carbon composites.
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APPLIED SURFACE SCIENCE
·
2020
·
IF 6.182
Xianglei Cao,Liugen Zhang,Tingxiang Chen,Chao Feng,Zechang Liu,Ying Qi,Wei Wang,Jide Wang
MOF based CdS-MoS 2 composite had strong photoresponse and rich catalytic sites because of the adjustable morphology and large specific surface area. The CdS-MoS 2 composite was synthesized by using the first synthesized Cd-MOF as the precursor. The hydrogen evolution activity was evaluated under simulated light source. The rate of photocatalytic hydrogen production can improve by 47 times for doping 2.5% (w/w) MoS 2 compare to pure CdS. The catalyst was analyzed by the UV/vis absorption spectra, photoluminescence spectra, time-resolved photoluminescence spectra, transient photocurrent responses, electrochemical impedance spectra, Mott-Schottky test, etc. The results revealed that the CdS-MoS 2 can greatly enhance the separation and transport efficiency of photogenerated carriers, and shift the position of conduction band for the catalyst, resulting significantly improve the production of hydrogen. This work provides a new strategy for manufacturing of photocatalyst by MOFs.
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