ACS Sustainable Chemistry & Engineering
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2022
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IF 9.224
Heyu Li,Minghua Liu,Wenqi Zou,Yuancai Lv,Yifan Liu,Lihui Chen
In this study, Ni-metal–organic frameworks (MOFs) were used as precursors to obtain carbon-supported nickel composites (Ni@C) after calcination. The hydrodeoxygenation properties of the model compound and corncob lignin were investigated without an external hydrogenation source and initial pressure. Additionally, the effect of Ni@C on degradation of model compounds, corncob lignin, and benzyl phenyl ether (BPE) under different conditions was examined. The results showed that with isopropanol as the in situ hydrogen source, the conversion percentage of BPE was 90.2% and the yield of phenol was 88.3 wt % at 150 °C. The catalysts were characterized by scanning electron microscopy (SEM), X-ray diffraction (XRD), NH3 temperature-programmed desorption (NH3-TPD), X-ray photoelectron spectroscopy (XPS), and thermogravimetry (TG), and the lignin and bio-oil were characterized by gas chromatography–mass spectrometry (GC–MS) and two-dimensional heteronuclear single quantum coherence (2D-HSQC). It was found that the Ni@C catalyst with well dispersion, high support rate, and rich acid sites was successfully synthesized. In the process of degradation, the C–O ether bond in the structure of lignin was successfully broken to generate the phenolic monomer, and the high-efficiency hydrodeoxygenation of lignin was realized under mild conditions.
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NEW JOURNAL OF CHEMISTRY
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2022
·Vol. 46
·期 17
·8271-8276
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IF 3.925
Ying-Xia Du,Lian Liu,Yong-Ke Li,Rui Liu,Wang-Ting Lu,Ji-Xiang Wang,Geng Zhang,Fei-Fei Cao
The preparation of two-dimensional (2D) composite material consisting of an active metal-based phase and carbon matrix is still a challenge. Herein, the 2D bimetal Co-TCPP(Fe) metal–organic framework (MOF) is synthesized and then adopted as the precursor to prepare a 2D composite electrocatalyst for the oxygen evolution reaction (OER). After carbonization and phosphorization, the 2D MOF is transformed into a composite nanoplate formed by Fe-doped CoP nanoparticles and a carbon matrix (Fe-CoP/C). This Fe-CoP/C composite exhibits a favorable OER performance in 1 M KOH with a low overpotential of 290 mV at 10 mA cm−2, which is better than that of counterparts without Fe and 2D morphology. The in situ formed metal (oxy)hydroxide is considered to be the main active species for the OER. The improved OER performance of Fe-CoP/C could be attributed to the Fe-doping in Co (oxy)hydroxide as well as the high electrochemical surface area induced by the 2D nanoplate morphology and conductive carbon network.
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JOURNAL OF MEMBRANE SCIENCE
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2022
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IF 10.53
Jingjing Chen,Xiaoli Wu,Chongchong Chen,Yihao Chen,Wenpeng Li,Jingtao Wang
Two-dimensional lamellar membranes featuring well-defined nanochannels hold great promise for efficient organics separation. However, the extensively existed non-selective microdefects within laminate architecture would impair separation efficiency and structure stability of membranes. Herein, defect-free metal-organic framework (MOF) lamellar membrane is facilely constructed by triple-needle electrostatic atomization technology. Specifically, one needle atomizes small-sized Cu-TCPP MOF nanosheets (TCPP = meso-tetra(4-carboxyphenyl)porphyrin) to build lamellar skeleton, and the other two needles meantime atomize Cu 2+ and TCPP to secondary-assemble crystals among nanosheets. In this manner, these non-selective microdefects are subtly sutured by the regenerated crystals with identical chemical components, resulting in a defect-free MOF lamellar membrane with enhanced structural stability. Importantly, this novel secondary-assembly method highly enhances the separation efficiency and meanwhile keeps high organics permeation for MOF membrane, with rejection of 93.8% for Rose Bengal (1.2 nm) and acetone permeance of 86.9 L m −2 h −1 bar −1 . In addition, the multipoint connection between nanosheets and crystals ensures excellent surface shearing and compaction resistance for MOF membrane, permitting high and steady operation performance for over 100 h. This secondary-assembly methodology by one-step process to construct defect-free and steady lamellar membrane provides a new avenue for the development of efficient separation membranes .
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2022
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IF 7.139
Ziqi Wang,Kai Bo,Yong Wang,Yongzhen Wang
The development of ethanol oxidation reaction (EOR) catalysts with high performance is an emerging need of direct ethanol fuel cells (DEFCs). Rational design of support materials of platinum-based catalyst can significantly enhance its catalytic performance for EOR. Here, the highly porous nitrogen-doped carbon material (NC-E) from ZIF-8 was synthesized using a novel and simple method assisted by eutectic salts. Compared with the carbon material obtained from ZIF-8 by traditional calcination (NC-T) and carbon black, the NC-E with high surface area and hierarchical pore structure supported Pt–Sn catalyst exhibits improved electrochemical activity and stability.
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ACS Omega
·
2022
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IF 4.132
Xu Zhang,Zhaowei Tong,Chao Liu,Lei Ye,Yuwei Zhou,Qin Meng,Guoliang Zhang,Congjie Gao
Metal–organic framework (MOF)-based polydimethylsiloxane mixed matrix membranes applied for alcohol recovery with high permeability and selectivity are drawing more and more attention. However, the design and fabrication of high-quality and stable MOF-based mixed matrix membrane for pervaporation are still a big challenge. Herein, PDMS functionalized MOF-derived nanoporous carbon (P-ZNC) was first explored as compatible nanofiller to mutually blend with polydimethylsiloxane on PVDF substrate to fabricate defect-free mixed matrix membranes via dip-coating and thermal cross-linkng. Induced by UV illumination, hydrophobic modification of MOF-derived nanoporous carbon was successfully realized under mild conditions within one step, simplifying the operation step. By using this facile strategy, we can not only solve the existing problem of agglomeration, but also covalently cross-link MOF derivative with polymeric matrix and effectively eliminate the interface defect between polymer and nanoparticles without any extra steps. The method also gives a good level of generality for the synthesis of versatile stable nanoporous MOF-derived carbon-based mixed matrix membranes on various supports. The prepared PDMS/P-ZNC with commendable structures possessed excellent separation performance in low concentration n-butanol recovery and had a good balance between permeance, selectivity, and stability.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2022
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IF 6.371
Yanrui Hao,Hao Guo,Fan Yang,Junye Zhang,Ning Wu,Mingyue Wang,Cuiliu Li,Wu Yang
Multi-walled carbon nanotube (MWCNT)/Ni-Mn-S composites are derived from MWCNT/Ni/Mn bimetallic metal-organic framework (MOF) for supercapacitor electrodes. Electroconductive MWCNT is introduced into Ni-Mn-S to form a three-dimensional interconnected structure due to the covalent interaction between Ni atoms and C atoms. During energy storage, MWCNT serves as miniature current collector to shorten pathway of electron collection and transmission. In addition, S 2- etching agent with Kirkendall effect makes edges and surfaces of the resulted sulfide structures rougher provide more active sites and improves electrochemical performance compared with precursors. By finely adjusting Ni/Mn molar ratio, the prepared MWCNT/Ni-Mn-S composite achieves excellent properties. As-prepared MWCNT/Ni-Mn-S(3:2) exhibits high specific capacitance of 1041 mAh g −1 at 1 A g −1 and good cyclic stability. The capacitance retention reaches 83.3% after 10,000 cycles. The assembled MWCNT/Ni-Mn-S(3:2)//AC hybrid supercapacitor (HSC) also shows high energy density of 25.33 Wh Kg −1 at power density of 829 W Kg −1 and outstanding cycling stability (93.3% after 20,000 cycles), which illustrates MWCNT/Ni-Mn-S(3:2) has important potential in supercapacitor.
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APPLIED SURFACE SCIENCE
·
2022
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IF 7.392
Yueyue Ma,Mengqi Wu,Ling Li,Zhanyu Li,Xiaohui Zhao,Ruqian Lian,Wenming Zhang
In this work, we synthesized a three-dimensional porous nitrogen-doped carbon composite with a uniform dispersion of MOF-derived Co 9 S 8 nanoparticles (3D Co 9 S 8 @NPC) via a simple template method combining with in situ high temperature pyrolysis. As K-ion battery anode, the 3D Co 9 S 8 @NPC exhibits a high specific capacity of 315 mA h g −1 at 0.1 A g −1 after 200 cycles, as well as a capacity of 223 mA h g −1 at 1 A g −1 after 1000 cycles, which is superior to the performance of KIB metal sulfide-based anode materials reported previously. The excellent performance is attributed to more pore structure and active sites in 3D Co 9 S 8 @NPC, which reduce efficiently K + diffusion length and accelerate the insertion/extraction of K + . The 3D N-doped carbon matrix also speeds up electron transport and buffers the volume expansion of Co 9 S 8 . Moreover, density functional theory (DFT) calculations demonstrate that due to the small energy change of K ion on Co 9 S 8 surface, the 3D Co 9 S 8 @NPC electrode is expected to show ideal rate capability in the K-ion battery system. This work provides ideas to craft other 3D structure anodes towards high-performance metal-ion batteries.
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Xinai Zhang,Zhuanlong Wang,Xiaowei Huang,Qilin Huang,Yunbo Wen,Bin Li,Melvin Holmes,Jiyong Shi,Xiaobo Zou
Excessive residual pesticides have raised overall environmental damage and health hazard issues, thus the development of facile and sensitive means for pesticide monitoring in different environmental field is desperately needed but challenging. In this work, a flexible paper-based colorimetry beating coffee-ring effect is achieved toward sensing environmental pesticide exposure in user-friendly mode. First, to circumvent poor performance of biomolecules, robust probe is designed by imprinting metal-organic frameworks (MOFs) with specific pockets, enabling to provide “key-lock” identification and sensitive quantitative information under harsh environment. Innovatively, integrating the MOF-mediated probe with filter paper, a well-distributed sensing interface is harvested to reduce colorimetric signal fluctuation for reliable detection properties, which is ascribed to superior wetting behavior of filter paper for avoiding ring-like deposit formation. Additionally, the uniform profile is simulated by Fluent numerical software. Further exploiting smartphone-assisted image acquisition and self-adaptive signal model, the simple-to-perform system exhibits good accuracy toward ppb-level thiacloprid free of colored background interference. A low limit of detection of 0.04 μM thiacloprid (corresponding to 0.01 μg g −1 by weight) is achieved. Moreover, it allows for in-filed monitoring thiacloprid exposure in agricultural wastewater, soil, fresh vegetables with satisfactory recoveries ranging from 92.7 % to 109.0 %, verifying the broad potential applications for point-of-use tracking of environmental pesticide and eventually bringing benefits to ecosystem protection in resource-deficient settings.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Yi-Cai Jiang,Meng-Fan Luo,Zi-Nuo Niu,Si-Yuan Xu,Yue Gao,Yuan Gao,Wen-Juan Gao,Jing-Jing Luo,Rui-Lin Liu
Magnetic carbon materials as the fascinating scavenger have been used for the purification of antibiotic wastewater. However, a majority of the reported magnetic carbon adsorbents suffer from the poor adsorption capacity and costly preparation costs. Herein, we report an in-situ growth of bimetallic FeCo-metal organic frameworks (MOFs) on waste paper-derived CoFe 2 O 4 /porous carbon via a hydrothermal strategy for reinforced clearance of tetracycline. The adsorption properties and mechanisms were systematically explored. Results revealed that the adsorption isotherms obeyed the Langmuir model, and the pseudo-second-order kinetics model could be well used to describe the current adsorption behavior. The maximum Langmuir adsorption capacity of FeCo-MOF@CoFe 2 O 4 /porous carbon toward tetracycline was calculated as 909 mg g −1 , which was significantly higher than that of other reported adsorbents. The ascendant capture property of the current adsorbent was presented under a wide pH range (5.0–12.0) and had excellent resistance to humic acid. In addition, the proposed coating method can also be applied to in-situ grow FeCo-MOF on biomass-derived magnetic porous carbon to enhance removal of tetracycline. Interestingly, the tetracycline adsorbed FeCo-MOF@CoFe 2 O 4 /porous carbon as a sustainable additive was further proved to be used for fruit preservation. Overall, this work provided a new research direction for in-situ architecture of magnetic carbon-based bimetallic MOF materials to treat antibiotic sewage and fruit preservation.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2022
·
IF 6.371
Nannan Ma,Chuanqi Fei,Jing Wang,Yinling Wang
Metal-organic frameworks (MOFs) have been widely investigated as electrocatalysts for the oxygen evolution reaction (OER). However, their catalytic performance needs to be further improved. Herein, a multi-pronged approach combining multi-metallic MOFs, 2D ultrathin structures and MOF hybridization was attempted. Specifically, the nanocomposite of lamellar NiFe-BTC and nanowire-like cobalt carbonate hydroxide hydrate (CCHH) was prepared on nickel foam (NF) by a two-step method. The as-prepared NiFe-BTC/CCHH/NF nanocomposite displayed excellent OER performance with an overpotential of 270 mV at a current density of 50 mA cm −2 and good stability in 1.0 M KOH. To construct an overall water splitting electrolytic cell, the phosphorization product of CCHH/NF (P-CCHH/NF) with high catalytic activity for hydrogen evolution reaction (HER) was used as the cathode. The water splitting electrolytic cell with NiFe-BTC/CCHH/NF as anode and P-CCHH/NF as cathode was highly efficient and stable, which only needed a voltage of 1.55 V to reach a current density of 10 mA cm −2 . This multi-pronged approach is expected to inspire other researchers to design high-performance OER catalysts.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2022
·
IF 5.876
Liang Qin,Yan Li,Fenglan Liang,Lijun Li,Yuwen Lan,Zhiyong Li,Xiaoting Lu,Manqi Yang,Deyun Ma
A new microporous 2D Co-based MOF , [Co 3 (C 6 H 3 NO 2 ) 2 (cpna) 2 (DMA) 2 ] n ( 1 ) (H 2 cpna = 6-(4-carboxylphenyl)nicotinic acid; DMA = N,N-dimethylacetamide), has been synthesized and structurally characterized. Complex 1 shows a 2D network with 1D channel of 6.4 × 9.3 Å 2 along the a -axis. Activated 1 ( 1a ) exhibits selective gas adsorption for CO 2 as compared to other gas molecules ( e.g. C 2 H 2 , CH 4 , CO, N 2 ) from the experimental single-component gas-adsorption isotherm (at 273K and 298K), molecular simulation and breakthrough experiments (298K). And the adsorption selectivity (CO 2 /C 2 H 2, CO 2 /CH 4, CO 2 /CO, and CO 2 /N 2 ) was calculated with the ideal adsorbed solution theory (IAST). Activated 1 shows 9.77 wt% (2.22 mmol/g) uptake of CO2 at 1 bar and 273 K. Furthermore, the activation of 1 exhibits high ideal selectivities in adsorption of CO 2 over C 2 H 2 , CH 4 , CO, and N 2 at 298 K (1 bar), which may be attributed to the pyridyl sites on the ligands and open metal sites on the nodes of the framework. Besides, 1a could adsorb more gas molecules due to thicker layer (10.97 Å) of 2D structure.
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FOOD CHEMISTRY
·
2021
·
IF 7.514
Quanbin Fu,Bingbing Sun,Jun Fan,Minglin Wang,Xin Sun,Geoffrey I.N. Waterhouse,Peng Wu,Shiyun Ai
A novel mixed matrix of MOF@COF hybrid was firstly formed by coating of hexahedral cage structure MOF with lightweight porous COF, and applied in dispersive solid-phase extraction of the phenoxy carboxylic acids (PCAs) from water and vegetable samples. Combined with liquid chromatography-tandem mass spectrometry, an excellent method with low limits of detection (0.69–1.79 ng·L −1 /0.002–0.006 ng·g −1 ), good reproducibility (1.32%–7.02%/1.81%–6.71%), and excellent linearities (10–1000 ng·L −1 , R ≥ 0.9955/0.04–50 ng·g −1 , R ≥ 0.9966) was established. The adsorption mechanisms deduced that the π-π interaction, hydrophobic effects, hydrogen bond, and halogen bond may promote the excellent adsorption of the PCAs. Finally, the applicability of the method was verified by spiking four kinds of water and vegetable samples with PCAs, and satisfying recoveries were obtained (between 83.3% and 104.9%).
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