SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Mengfang Jiang,Xuefeng Zhang,Xiao Du,Xiaowei An,Fengfeng Gao,Xiaogang Hao,Guoqing Guan,Zhong Liu,Jun Li,Abuliti Abudula
An electrochemically induced electrode with bromide ion (Br - ) dual adsorption sites was obtained by in-situ growing of Ni-MOF derivative/NiCo layered double hydroxide (Ni-MOF(D)/NiCo LDH) composite film on the stainless-steel wire mesh via an electrodeposition-assisted solvothermal method, which exhibited excellent Br - selectivity from ionic mixture solutions of Br - , NO 3 – and I - in an electrochemically switched ion exchange (ESIX) system. The Br - extraction capacity was as high as 126.30 mg·g −1 and the separation factors of Br - /NO 3 – and Br - /I - were 8.29 and 4.83 respectively. Combining the simulation and experimental results, it was confirmed that the highly efficient selective extraction of Br - in neutral solution should be derived from the dual-site (i.e., electrochemically induced laminate metal coordination sites and interlayer anion exchange sites of NiCo LDH) adsorption. Furthermore, the electrode demonstrated superior adsorption–desorption performance and electrochemical stability because of the in-situ growth strategy, which enhanced the binding force between NiCo LDH and substrate and improved the electrical conductivity of NiCo LDH, and provided a storage space for Br - . This study served deep understanding of ions selective extraction mechanism of LDH-based materials in the ESIX process, which could be a novel reaction concept for the design of those electrodes with specific recognition sites in the applications of them in other fields such as supercapacitors, sensors and batteries.
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Nanomaterials
·
2021
·Vol. 11
·期 9
·2171
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IF 5.076
Le Wang,Pengxue Sun,Yiyu Yang,Hanzhen Qiao,Hailong Tian,Dapeng Wu,Shuoye Yang,Qipeng Yuan,Jinshui Wang
The field of enzyme cascades in limited microscale or nanoscale environments has undergone a quick growth and attracted increasing interests in the field of rapid development of systems chemistry. In this study, alcohol dehydrogenase (ADH), lactate dehydrogenase (LDH), and mesoporous silica nanoparticles (MSN) immobilized nicotinamide adenine dinucleotide (NAD+) were successfully immobilized on the zeolitic imidazolate frameworks (ZIFs). This immobilized product was named ZIF@ADH/NAD-MSN/LDH, and the effect of the multi-enzyme cascade was studied by measuring the catalytic synthesis of lactic acid. The loading efficiency of the enzyme in the in-situ co-immobilization method reached 92.65%. The synthesis rate of lactic acid was increased to 70.10%, which was about 2.82 times that of the free enzyme under the optimal conditions (40 °C, pH = 8). Additionally, ZIF@ADH/NAD-MSN/LDH had experimental stability (71.67% relative activity after four experiments) and storage stability (93.45% relative activity after three weeks of storage at 4 °C; 76.89% relative activity after incubation in acetonitrile-aqueous solution for 1 h; 27.42% relative activity after incubation in 15% N, N-Dimethylformamide (DMF) solution for 1 h). In summary, in this paper, the cyclic regeneration of coenzymes was achieved, and the reaction efficiency of the multi-enzyme biocatalytic cascade was improved due to the reduction of substrate diffusion.Keywords:confinement effect;multi-enzyme catalytic cascade;in-situ synthesis;coenzyme recycling;co-immobilization enzyme
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APPLIED SURFACE SCIENCE
·
2021
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IF 6.707
Xu Cai,Tongtong Jiang,Mingzai Wu
The sluggish oxygen evolution reaction (OER) and poor stability of oxygen electrocatalysts are main obstacles to the scale-up commercial application of rechargeable Zn-air battery. Herein, a three-dimensional (3D) multi-level architecture design is achieved by the confined growth of two-dimensional (2D) layer double hydroxides of nickel and iron (NiFe LDH) flakes on copper nanowires arrays (Cu NWs), which is epitaxially assembled on the surface of Cu foam (CF). The established Cu@Cu NW@LDH possesses stronger bonding strength between NiFe LDH and Cu NWs as well as Cu NWs and CF endowed by electroplating method. The introduction of Cu NWs not only provides abundant nucleation sites for the deposition of NiFe LDH flakes but also improves the electron conductivity of composite. The obtained Cu@Cu NW@LDH shows excellent OER catalytic activity with a potential of 1.44 V at a current density of 10 mA cm −2 and strong alkaline resistance properties in comparison with NiFe LDH on CF (Cu@LDH). As expected, the rechargeable zinc-air battery (ZAB) with Cu@Cu NW@LDH as air electrode delivers superior cycling stability (250 h at a current density of 10 mA cm −2 ). This work paves a new way to the design of 3D multi-level architecture catalysts for ZAB.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2021
·
IF 9.028
Liying Wu,Zhiqiang Sun,Yufei Zhen,Shishu Zhu,Chen Yang,Jing Lu,Yu Tian,Dan Zhong,Jun Ma
Ubiquitous oxygen vacancies (Vo) existing in metallic compounds can activate peroxymonosulfate (PMS) for water treatment. However, under environmental conditions, especially oxygenated surroundings, the interactions between Vo and PMS as well as the organics degradation mechanism are still ambiguous. In this study, we provide a novel insight into the PMS activation mechanism over Vo-containing Fe–Co layered double hydroxide (LDH). Experimental results show that Vo/PMS is capable of selective degradation of organics via a single-electron-transfer nonradical pathway. Moreover, O2 is firstly demonstrated as the most critical trigger in this system. Mechanistic studies reveal that, with abundant electrons confined in the vacant electron orbitals of Vo, O2 is thermodynamically enabled to capture electrons from Vo to form O2•– under the imprinting effect and start the activation process. Simultaneously, Vo becomes electron-deficient and withdraws the electrons from organics to sustain the electrostatic balance and achieve organics degradation (32% for Bisphenol A without PMS). Different from conventional PMS activation, under the collaboration of kinetics and thermodynamics, PMS is endowed with the ability to donate electrons to Vo as a reductant other than an oxidant to form 1O2. In this case, 1O2 and O2•– act as the indispensable intermediate species to accelerate the circulation of O2 (as high as 14.3 mg/L) in the micro area around Vo, and promote this nano-confinement electron-recycling process with 67% improvement of Bisphenol A degradation. This study provides a brand-new perspective for the nonradical mechanism of PMS activation over Vo-containing metallic compounds in natural environments.
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高影响因子
APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Lijia Dong,Shengbo Li,Yefei Jin,Baowei Hu,Guodong Sheng
In this paper, CaAl hydrotalcite or hydroxyapatite decorated invasive plant ( Solidago canadensis )-derived biochar were synthesized by co-precipitation and high temperature pyrolysis method. The three composites and bare biochar were characterized by Scanning electron microscopy (SEM), X-ray spectroscopy (EDX), the Fourier transform infrared spectroscopy (FT-IR), X-ray diffractometer (XRD), and X-ray photoelectron spectroscopy (XPS) techniques, and employed to remove Eu(III) from wastewater under a series of environmental conditions. The results indicated that the Eu(III) adsorption on BC@LDH@HAP was higher than that on BC, BC@LDH, and BC@HAP, and belonged to multi-layer adsorption, which was different from the monolayer adsorption of biochar. The adsorption could be fitted best by Langmuir model and the maximum adsorption capacity of Eu(III) on BC@LDH@HAP was up to 714 mg/g at pH ~ 6. The characterization results suggested that this excellent adsorption of BC@LDH@HAP arose from the abundant P-, C-, O-containing functional groups rather than larger specific surface area. The spectra of XPS, FT-IR, and XRD uncovered that the adsorption mechanisms of Eu(III) on BC@LDH@HAP involved surface complexation, ion exchange, and precipitation. Moreover, the absorbed Eu(III) was formed into two precipitate induced by P-containing groups and carbonate groups. This research confirmed BC@LDH@HAP is a promising material for the removal of Eu(III) in wastewater.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2021
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IF 4.539
Yuxin Xiang,Yi He,Wei Zhang,Bengang Li,Hongjie Li,Yuqi Wang,Xiangying Yin,Wenwen Tang,Zhenyu Li,Ze He
A two-step method was used to fabricate a superhydrophobic surface on steel sheet, nickel foam (NF), and stainless steel mesh (SS). The micro-nano structure of Layer Double Hydroxide (LDH) is obtained by hydrothermal method . The synergistic effect of triethoxy(octyl)silane (TTOS) and FeNi-LDH produces a superhydrophobic surface. Fourier infrared spectroscopy (FTIR), X-ray diffractometer (XRD), X-ray photoelectron spectroscopy (XPS), and scanning electron microscope (SEM) were used for structural characterization, which confirmed the synthesis and hydrophobic modification of FeNi-LDH. The time of the hydrothermal reaction was discussed, and the results showed that the water contact angle (WCA) of the superhydrophobic surface fabricated by setting the reaction time to 12 h can reach 169 ± 2°. Electrochemical tests also show that the prepared superhydrophobic surface can achieve a corrosion inhibition rate of 96.3%. In addition, the superhydrophobic NF and superhydrophobic SS prepared by the same method were tested for antifouling and oil-water separation performance. The results show that, due to the excellent non-wettability of the surface, the preparation method of this superhydrophobic surface has great potential value in the fields of anti-corrosion, anti-fouling and oil-water separation.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2021
·
IF 7.312
Zhi-Heng Lu,Ibrahim Abdelhai Senosy,Dong-Dong Zhou,Zhong-Hua Yang,Hao-Ming Guo,Xiao Liu
In this work, a novel Fe 3 O 4 @ZnAl-LDH@MIL-53(Al) composite was synthesized by a facile three-step process and utilized as an adsorbent for the removal of azole fungicides from environmental water. The characterization results revealed that double hydroxide (ZnAl-LDH) and metal organic framework (MIL-53) have been successfully tethered to the shell of Fe 3 O 4 . The main factors affecting the removal efficiencies were investigated, and results revealed that Fe 3 O 4 @ZnAl-LDH@MIL-53(Al) composite possessed high removal efficiencies for azole fungicides. Furthermore, the adsorption mechanism was investigated and including hydrogen-bonding interaction, chemisorption and π–π interaction. The adsorption kinetic was more consistent with the pseudo-second-order kinetic model, and the whole adsorption process could reach the equilibrium within 5 min. Langmuir adsorption isotherm model could describe the adsorption process most accurately, and the maximum adsorption values of azole fungicides were in the range of 43.54–71.79 mg g −1 . Meanwhile, the adsorption thermodynamics indicated that the adsorption process was exothermic and spontaneous. Hence, Fe 3 O 4 @ZnAl-LDH@MIL-53(Al) composite had a great application potential in the removal of azole fungicides from the environment.
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APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Yidong Sun,Xingpu Wang,Qiang Fu,Chunxu Pan
Photocatalytic decomposition of water for hydrogen production is considered a promising solution to address the issues of energy crisis and environmental pollution. Herein, a kind of novel hollow flower-like 0D/3D Zn 0.5 Cd 0.5 S/NiCoZn-LDH with an n-n heterojunction is synthesized via precipitation and cation-exchange methods. Photocatalytic experiments reveal that the composite photocatalyst exhibits excellent performance compared with pure Zn 0.5 Cd 0.5 S. In other words, the composite photocatalyst shows enhanced response to visible light, three-fold increased transient photocurrent, and the hydrogen production rate reaching to 1100 μmol/h/g, approximately 7.3 times higher relative to pure Zn 0.5 Cd 0.5 S. The reaction mechanism is also elucidated. Zn 0.5 Cd 0.5 S/NiCoZn-LDH shows a type II n-n heterojunction, which can effectively transfer and separate the photo-generated electrons and holes, and is beneficial for the photocatalytic hydrogen production reaction. The synthesized composite photocatalyst is prepared using a simple method, enabling future large-scale production and applications.
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CHEMICAL ENGINEERING JOURNAL
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2021
·
IF 13.273
Xiaomeng Zhang,Yang Zong,Longqian Xu,Yunfeng Mao,Deli Wu
Abiotic humification can be facilitated by iron-containing minerals or oxides, but most studies have focused on well-crystallized and stable iron phases, the catalytic effect of which is generally unremarkable. In the present study, we report an enhanced abiotic integrated polyphenol-Maillard humification reaction catalysed by Mg/Fe-layered double hydroxide (Mg/Fe-LDH) with high surface reactivity. The results demonstrated that Mg/Fe-LDH could effectively promote the humification reaction at a lower dosage compared with Fe 2 O 3 . As an iron-chelating ligand, catechol rapidly induced iron dissolution from Mg/Fe-LDH through the formation of an Fe(III)-catechol complex, which strengthened the catalytic effect of Fe(III). The photochemical behaviour of Fe(III)-catechol complex and its impact on the Fe(III)-catalysed humification process were investigated. Under light irradiation, environmentally persistent free radicals (EPFRs) originated from the Fe(III)-catechol complex were formed and stabilized in the presence of Mg/Fe-LDH particles, which inhibited the oxidation of catechol and the humification process. Hence, the formation of humic substances (HS) catalysed by Mg/Fe-LDH was more efficient under darkness. Iron redox cycling and generation of reactive oxygen species (ROS), HO• and O 2 •- , were also involved. According to transformation products (TPs) analysis, ortho -aminophenol was proposed to be a key product in the humification reaction. Self-coupling of catechol radical and ortho -aminophenol radical, ring cleavage were likely to occur in the Fe(III)-catalysed humification process. Higher relative abundance of CHO products was observed in the presence of Mg/Fe-LDH by Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS), suggesting that iron is effective on promoting C–C bonds formation. The above results provide more comprehensive insights into Fe(III)-catalysed humification and a guidance to improve the efficiency of HS formation and carbon sequestration in organic wastes utilization.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2020
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IF 16.683
Pengqi Zhu,Mengting Gao,Jin Zhang,Zhiwei Wu,Ruiyi Wang,Yunwei Wang,Eric R. Waclawik,Zhanfeng Zheng
Coordinated Ru species, Ru/LDH, were applied to the reduction of carbonyl compounds via blue light irradiation under mild (45 °C, atmospheric argon pressure), ligand-free, and additive-free conditions. LDH can act as an efficient base catalyst to assist in formation of isopropoxide, requiring no additional base, because basic OH groups form an ordered distribution on LDH surface. The coordinated Ru species containing one OH and three oxygen atoms ligands deriving from the OH groups of LDH are a crucial component, for securing the active electron-deficient Ru species that favours formation of Ru-isopropoxide. The photocatalytic activity is related to the adsorption capacity of isopropyl alcohol near the electron-deficient Ru species and the formation of Ru-isopropoxide. The strong-metal-support interactions between Ru and LDH affect the coordination and the electronic surroundings of the Ru centres and have a significant effect on the photocatalytic activity.
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Journal of Environmental Sciences
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2020
·
IF 4.302
Shengbo Li,Lijia Dong,Zuofu Wei,Guodong Sheng,Kui Du,Baowei Hu
Herein, we developed the invasive plant-derived biochar (IPB) functionalized with CaAl-LDH at five mass ratios using a physical mixture method, assessed their adsorption perform for Eu(III), and explored the relative mechanisms. Results show that the IPB successfully loaded CaAl-LDH in five composites and their Eu(III) sorption affinities were strongly affected by solution pH, contact time, temperature, and the mass ratio of LDH and IPB. All the sorpiton process for Eu(III) occurred on the heterogeneous surface of five composites and the boundary layer diffusion limited the chemical sorption rate. Interestingly, the CaAl-LDH/IPB composite with high ratio of IPB had higher sorption capacity than the one with high ratio of LDH due to larger porosity of the former. Three mechanisms containing ion exchange between Al and Eu ions, surface complexation with carboxyl- and oxygen-containing functional groups, and precipitation were involved in the Eu(III) sorption, but the dominant sorption mechanism for each CaAl-LDH/IPB composite differed with different mass ratio of CaAl-LDH and IPB. In composite with more IPB (e.g., CaAl-LDH/IPB-13), both ion exchange and surface complexes dominated the sorption process and the intensity of Eu 3+ was identified with the one of Eu 2 O 3. Whereas in composites with high LDH, ion exchange dominated the sorption and the intensity of Eu 3+ was obviously higher than the one of Eu 2 O 3 . This research will provide a new perspective for the application of the LDH/biochar materials.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
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IF 8.355
Liying Wu,Junming Hong,Qian Zhang,Bor-Yann Chen,Ji Wang,Zhengyu Dong
This first-attempt study explored interactive function of oxygen vacancies, transition metals, and surface hydroxyl groups for persulfate (PS) activation, at different pH conditions. Oxygen vacancy-rich Fe 2 Co 1 -LDHs was fabricated via calcination in hydrogen atmosphere. The Fe 2 Co 1 -LDH possessed the maximal concentration of oxygen vacancies and abundant hydroxyl groups for effective functioning according to the characterization through X-ray photoelectron spectroscopy (XPS) and electron paramagnetic resonance (EPR). The BPA-degrading efficiency in the LDHs/PS system indicated that Fe 2 Co 1 -LDH exhibited the most promising activated performance since oxygen vacancies could improve the catalytic efficiency to enhance electron transport phenomena between the Fe and Co. N 2 experiments proved that the presence of oxygen vacancies could promote the production of 1 O 2 and O 2 − . Phosphate and pH effect experiments showed the Fe 2 Co 1 -LDH/PS system stably maintained operation performance over a wide pH range for bisphenol A (BPA) removal with the effect of surface hydroxyl groups. Practical samples had little effect on the removal of BPA. According to the quenching experiments and EPR technology, SO 4 − was the main active radicals in acid and neutral conditions and apparently the OH played the crucial role at alkaline pHs. Two different major reaction routes at different pH levels in the Fe 2 Co 1 -LDH/PS system for mechanisms of BPA degradation were proposed herein. The Chemical intermediates of BPA degradation were identified by gas chromatography-mass spectrophotometry (GC–MS) analysis, and degradation pathways were proposed for system optimization.
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