NEW JOURNAL OF CHEMISTRY
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2022
·Vol. 46
·期 40
·19542-19554
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IF 3.925
Xiaoqing Wang,Binhe Zhao,Zimeng Xu,Haosong Chen,Tong Ye,Jing Zhang,Xinyue Zhang,Aoqi Ji,Jionghui Li,Chunhua Xiong
A series of novel resin-based MOF composites Co-MOF@D113-N (N = 1, 6) were prepared using 2-methylimidazole, cobalt acetate and D113 resin, through the layer-by-layer self-assembly method. The Co-MOF presented an amorphous form with the inducement of resin groups and the loading capacity increased with the number of self-assembled layers. The strong anchoring effect between Co and N effectively improved the thermal stability of the composites. The adsorption experiments showed that the adsorption capacity of the Co-MOF@D113-6 resin for Cu(II) increased with temperature in the range of 283–303 K. The adsorption capacity of Co-MOF@D113-6 for Cu(II) increased under the synergistic effect of MOFs and D113. The maximum adsorption capacity of Co-MOF@D113-6 was 273.88 mg g−1. The fitting results showed that the adsorption of Cu(II) by the Co-MOF@D113-6 conformed to the pseudo-second-order kinetic model dominated by chemisorption, and also conformed to the preferential Freundlich adsorption isotherm model. A low cost resin carrier combined with a high efficiency MOF composite adsorption material provided high efficiency and low consumption for promising development.
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Inorganic Chemistry Frontiers
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2022
·Vol. 9
·期 22
·5982-5993
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IF 7.779
Yifan Pan,Dongyan Gao,Yupeng Dang,Pengcheng Xu,Dandan Han,Changling Liu,Yen Wei,Yanru Yang
Metal–organic frameworks (MOFs) with bimetallic centers are considered as promising electrode materials for supercapacitors due to the large specific surface area and potential redox sites. In this work, the internal structure evolution, electron transfer in the metal center, and the mechanism of action of the Mn dopant to enhance conductivity in electrochemical processes are discussed. Density functional theory (DFT) calculations show that the introduction of Mn ions greatly reduces the band gap of the Ni-MOF and increases the carrier concentration, confirming the electron transfer process of electrons from Ni2+ to Mn2+ through the bridging oxygen. Therefore, the optimal NiMn-MOF produces an impressive specific areal capacity of 1.89 mA h cm−2 at 1 mA cm−2. Meanwhile, a hybrid supercapacitor (HSC) based on the NiMn-MOF electrode and activated carbon (AC) can output a high specific energy of 67.5 W h kg−1 at a specific power of 84.5 W kg−1 with excellent cycling stability (capacity retention of 94% after 10 000 cycles). Taking advantage of the high-energy storage properties of the NiMn-MOF//AC supercapacitor device, a solar power generation system is further integrated for self-powered portable electronic applications. This work broadens the applicability of activity prediction for bimetallic MOF electrode materials with high electrochemical performance.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
·
IF 5.518
Jinmiao Sun,Xiaoli Li,Jiamin Li,Manman Mu,Xiaohong Yin
Bi-based semiconductors have been regarded to be an ideal platform in photocatalytic CO 2 reduction to fuels. However, the insufficient charge transfer efficiency greatly restricts their practical application. Herein, we fabricated 1D/2D hierarchical heterostructures by the hybridization of Bi 4 O 5 Br 2 and rod-like MOF-derived MoS 2 anchored in nitrogen-doped porous carbon (NPC-MoS 2 ) using Mo-MOF as a precursor followed by sulfidation and typical solvothermal process. Compared to pristine Bi 4 O 5 Br 2 nanosheet and NPC-MoS 2 nanorod , the 5 wt% NPC-MoS 2 @Bi 4 O 5 Br 2 p-n heterojunction exhibits distinctly enhanced photocatalytic activity under light illumination due to the increased light absorption capability and more effective charge transfer efficiency. X-ray photoelectron spectroscopy and photoelectrochemical analysis imply that a built-in electric field on interfaces is created to form p-n heterojunctions which drive the photoinduced electrons transferred from NPC-MoS 2 to Bi 4 O 5 Br 2 . Finally, the type-II charge transfer mechanism is proposed which promotes separation of the charges and provides suitable conduction band to reduce CO 2 much efficiently. In a word, this work provides a new insight into the establishment of hierarchical p-n heterostructures for photocatalysis .
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ELECTROCHIMICA ACTA
·
2021
·
IF 6.901
Da Wang,Ying Zhu,Weiting Yu,Zhiqiao He,Feilong Dong,Yi Shen,Tao Zeng,Xiaohui Lu,Jun Ma,Lizhang Wang,Shuang Song
Ag-based electrodes have emerged as important candidates for the industrial electrochemical CO 2 reduction reaction (eCO 2 RR) to form CO. Herein, an intrinsic versatile Ag electrode has been derived in situ from Ag-MOF on Ag foam (denoted as ER-AF), which exhibits the highest current density (57.2 mA cm −2 ) at a potential of −1.15 V vs. RHE reported to date for the formation of CO in a commonly used H-type cell. ER-AF has multiple-roles: The 3D dendrite structure promotes mass diffusion; the rich edges sites favor CO 2 adsorption and conversion, and the highly exposed (111) facet facilitates the desorption of CO. Their cooperating functions result in the remarkable performance of ER-AF in the eCO 2 RR to form CO. This work offers an effective strategy to achieve high eCO 2 RR activity and selectivity by assembling the active and stable sites together on the MOF-derived materials.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
·
IF 8.128
Ahmed Mahmoud Idris,Xinyan Jiang,Jun Tan,Zhenzhi Cai,Xiaodan Lou,Jin Wang,Zhengquan Li
Dye-sensitized system holds great potential for the development of visible-light-responsive photocatalysts not only because it can enhance the light absorption and charge separation efficiency of the systems but also because it can tune the band structure of catalysts. Herein, two-dimensional (2D) Fe-MOF nanosheets (Fe-MNS) with a LUMO potential of 0.11 V ( vs. RHE) was prepared. Interestingly, it has been found that when the 2D Fe-MNS catalyst was functionalized with visible-light-responsive [Ru(bpy)] 3 2+ as a dye-sensitizer, the electrons from the [Ru(bpy)] 3 2+ can effectively inject into the 2D Fe-MNS, which resulted in a negative shift of the LUMO potential of the 2D Fe-MNS to −0.15 V ( vs. RHE). Consequently, the [Ru(bpy)] 3 2+ /Fe-MNS catalytic system exhibits a sound photocatalytic CO 2 -to-CO activity of 1120 μmol g -1 h −1 under visible-light-irradiation. The photocatalytic CO production was further ameliorated by regulating the electronic structure of the 2D Fe-MNS by doping Co ions , achieving a remarkable photocatalytic activity of 1637 μmol g -1 h −1 . This work further supports that the dye-sensitized system is an auspicious strategy worth exploring with different catalysts for the development of visible-light-responsive photocatalytic systems.
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MATERIALS RESEARCH BULLETIN
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2021
·
IF 4.641
Jing Zhang,Jiajie Huang,Liang Wang,Peiheng Sun,Peijia Wang,Zhujun Yao,Yefeng Yang
As promising electrode materials for supercapacitors, metal-organic frameworks (MOFs) with rich porosity, large surface area and abundant redox sites have attracted increasing attention. Nevertheless, the intrinsically interior electrical conductivity and ease of agglomeration for most MOFs have largely restricted their energy storage application. In this work, we report the controlled fabrication of bimetallic NiMn-MOF nanosheets on the surface of NiCo 2 O 4 nanowire arrays to form NiCo 2 O 4 @NiMn-MOF core-shell structure and investigate the effect of Mn incorporation in Ni-MOF shell on the electrochemical performance of the hybrid arrays in supercapacitors. Benefitting from the delicately designed structures and compositions, the optimal NiCo 2 O 4 @NiMn-MOF electrode presents an extraordinarily high specific capacity of 243.0 mAh/g at 2 mA/cm 2 . We further assembled a flexible solid-state hybrid supercapacitor with NiCo 2 O 4 @NiMn-MOF and activated carbon as electrodes, exhibiting a high energy density of 48.2 Wh/kg at 1606.7 W/kg, accompanied by excellent mechanical flexibility and electrochemical durability. This work demonstrates a new approach for developing novel MOF array-based electrode materials with boosted electrochemical performance in the field of flexible energy storage devices.
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ACS Applied Materials & Interfaces
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2021
·
IF 9.229
Wenxia Dong,Zhongping Li,Wen Wen,Bin Liu,Guangming Wen
Nanomaterial selection is critical for photoelectrochemical (PEC) sensing. In this report, a novel cathodic photoelectrochemical (PEC) strategy was proposed for the detection of doxorubicin hydrochloride (Dox) and gentamicin sulfate (CN). The photocathode was synthesized by noncovalently coupling cadmium sulfide (CdS) to the porphyrin-derived metal–organic framework (CdS@PCN-224). This type of assembly created a pleasant interface for the combination of doxorubicin hydrochloride and gentamicin sulfate, resulting in a good CdS@PCN-224 donor–acceptor system. When compared to a single optoelectronic material, its photocurrent is enhanced by unprecedented nine times. This research could pave the way for the realization of PCN-224’s enormous potential in PEC sensing.
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Scientific Reports
·
2021
·Vol. 11
·期 1
·1-11
·
IF 4.38
Wang Haitao,Zou Haiyan,Liu Yingying,Liu Zhenglong,Sun Wenshuang,Lin Kunyi Andrew,Li Tielong,Luo Shuangjiang
It’s highly desired but challenging to synthesize self-supporting nanohybrid made of conductive nanoparticles with metal organic framework (MOF) materials for the application in the electrochemical field. In this work, we report the preparation of Ni 2 P embedded Ni-MOF nanosheets supported on nickel foam through partial phosphidation (Ni 2 P@Ni-MOF/NF). The self-supporting Ni 2 P@Ni-MOF/NF was directly tested as electrode for urea electrolysis. When served as anode for urea oxidation reaction (UOR), it only demands 1.41 V (vs RHE) to deliver a current of 100 mA cm −2 . And the overpotential of Ni 2 P@Ni-MOF/NF to reach 10 mA cm −2 for hydrogen evolution reaction HER was only 66 mV, remarkably lower than Ni 2 P/NF (133 mV). The exceptional electrochemical performance was attributed to the unique structure of Ni 2 P@Ni-MOF and the well exposed surface of Ni 2 P. Furthermore, the Ni 2 P@Ni-MOF/NF demonstrated outstanding longevity for both HER and UOR. The electrolyzer constructed with Ni 2 P@Ni-MOF/NF as bifunctional electrode can attain a current density of 100 mA cm −2 at a cell voltage as low as 1.65 V. Our work provides new insights for prepare MOF based nanohydrid for electrochemical application.
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APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Yuan Wang,Zhaoxian Yang,Lei Liu,Yingbo Chen
In this study, hydrophobic nanofillers (ODA-h-NCs) were firstly synthesized through surface modification of MOF-derived nanocages by octadecylamine (ODA). ODA-h-NCs were then incorporated into poly(piperazine-amide) (PA) active layer to fabricate thin-film nanocomposite (TFN) nanofiltration membranes. The effects of ODA-h-NCs dosage on PA’s properties were characterized and the membrane performances on salt rejections were evaluated. Finally, the TFN nanofiltration membrane with the optimal nanoparticle doping amount was chosen. The experimental results show that the water permeance of the constructed TFN nanofiltration membrane reaches 8.97 L/(m 2 ·h·bar) with 95.8% Na 2 SO 4 rejection when ODA-h-NCs concentration is 0.0075 wt%, which is 1.7 times that of pristine membrane. It is also testified that the prepared TFN nanofiltration membrane possesses good stability through 50-h filtration test. Although the introduction of hydrophobic ODA-h-NCs increases the PA layer thickness, ODA-h-NCs decrease the crosslinking degree of PA layer by inhibiting the piperazine diffusion rate and pathway, their unique porous nanocage structure and large surface area provide additional transport path for water molecules, which equips TFN nanofiltration membrane with higher water flux.
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Journal of the Taiwan Institute of Chemical Engineers
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2021
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IF 5.876
Yang Bai,Gongzhe Nie,Yi He,Chao Li,Xianbo Wang,Liqun Ye
Background The Fenton-like reaction is a highly potential advanced oxidation process. The photo-Fenton-like reaction formed by the combination of photocatalytic advanced oxidation process, which combines their advantages, breaks the original Fenton-like reaction rate bottleneck. Methods In this study, an ultra-thin MOF (Cu-TCPP(BA)-MOF) with porphyrin as the ligand and copper as the metal node was synthesized via a simple one-pot method for the first time. Significant Findings It activates Peroxymonosulfate (PMS) under visible light to degrade 10 mg/L Rhodamine B which can be completely degraded within 40 min. The pseudo-first-order rate constant of RhB is 0.9011 min −1 , being 5 folds larger than this for CuO as catalysts. ESR analysis shows that Cu-TCPP(BA)-MOF/PMS/vis system produces a large amount of non-radical 1 O 2 . Also under visible light, with E. coli concentration of 10 7 cfu/mL, it can be completely inactivated within 50 min. Dilution spreading plate method and Fluorescence spectroscopy confirmed the complete death of bacteria. In terms of mechanism, the ultra-thin MOF provides a large number of Cu 2+ active sites. Under visible light, the cycle between Cu 2+ and Cu + is accelerated and the pathways that produce reactive oxygen species (ROS) is changed, thereby improving the performance of contaminant treatment and sterilization.
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Analytical Methods
·
2021
·Vol. 14
·期 1
·44-51
·
IF 2.896
Lili Chen,Zihan Cheng,Xinyue Peng,Guoqiao Qiu,Li Wang
Nitroaromatic explosives pose a great threat to the environment and human safety. It is very important to design simple, highly efficient and multifunctional sensors for detecting nitroaromatic explosives. However, a few sensors can determine multicomponent nitroaromatic explosives simultaneously. Eu functionalized MOF-253 (Eu@MOF-253) hybrid material was synthesized using the post-synthetic modification method. The introduction of Eu3+ in MOF-253 caused the fluorescence peak of the ligand to show a distinct red-shift due to its polarization enhancement effect in the presence of 2,4-DNP. The emission and excitation spectra of the Eu@MOF-253 sensor showed overlap with the ultraviolet-visible (UV-vis) absorption spectra of the representative nitroaromatic explosives 2,4-dinitrophenol (2,4-DNP) and 2,4,6-trinitrophenol (TNP). Therefore, it is feasible to discriminate and quantify TNP and 2,4-DNP simultaneously. As proposed, the Eu@MOF-253 luminescent sensor was highly sensitive and selective towards TNP and 2,4-DNP. The other coexisting nitroaromatic explosives did not interfere with the determination. Upon addition of TNP, the fluorescence of the Eu@MOF-253 sensor decreased dramatically and showed an excellent quenching constant (Ksv) of 1.58 × 106. The fluorescence intensities of the Eu@MOF-253 sensor presented good linear relationships with concentrations of TNP and 2,4-DNP ranging from 0.01–100 μM and 0.01–25 μM, respectively. Low limits of detection (LOD) for both 2,4-DNP and TNP were approximately 10 nM. The determination mechanism is mainly ascribed to the internal filtration effect (IFE) and electron transfer. This work provides a practical method for the highly efficient determination of nitroaromatic explosives.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Yi Yu,Yu Cheng,Lei Tan,Xiangmei Liu,Zhaoyang Li,Yufeng Zheng,Tao Wu,Yanqin Liang,Zhenduo Cui,Shengli Zhu,Shuilin Wu
Periodontitis is a chronic inflammatory disease caused by the bacteria infection in dental plaque, which can lead to gingival recession and tooth loss, seriously endangering human oral health. Current treatments through the combination of mechanical debridement and antibiotics therapy still have the problems of gingival trauma, low treatment efficiency, long treatment cycle and bacterial resistance. Herein, we prepare an injectable ointment based on MOF-based single-atom catalysis systems with good biocompatibility and high anti-biofilm activity, which consists of PEG-400/PEG-4000 and Pt single-atom doped porphyrin metal−organic framework (PCN-222-Pt). Through theoretical screening, we find that all the metal single atoms (Pt, Au, Cu, Ru) can improve the oxidase-like activity of PCN-222, which reduce the adsorption and activation energy of O 2 . Among them, PCN-222-Pt shows strong oxidase-like and peroxidase-like activities and can produce reactive oxygen species spontaneously, which shows an excellent anti-biofilm performance (98.69% against S. aureus biofilm, 99.91% against E. coli biofilm) in vitro within 1 h. In the treatment of biofilm-induced periodontitis, the injectable PCN-222-Pt ointment showed alleviative inflammation response, reduced bone destruction and healthier gum tissue, which is superior to the clinical used Periocline. This work provides a rapid, effective, non-invasive and convenient strategy for the treatment of periodontitis without antibiotics.
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