Sustainable Energy & Fuels
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2021
·Vol. 5
·期 5
·1429-1438
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IF 6.367
Fu Liu,Xingzhong Guo,Yang Hou,Fan Wang,Chang Zou,Hui Yang
Electrochemical water splitting provides a prominent route towards clean energy conversion and storage, while unsuitable catalysts restrict its application. Core–shell hierarchical heterostructure materials with strong synergistic effects based on non-noble metal elements have been developed to compensate for inadequacy. In this work, a core–shell hierarchical heterostructure Co9S8/Ni3S2@NiFe-LDH electrocatalyst was prepared via hydrothermal and electrodeposition methods. The resultant Co9S8/Ni3S2@NiFe-120 electrocatalyst consists of Co9S8 substrates as the core and NiFe-LDHs as the shell, and exhibits excellent overall water splitting electrocatalytic activity with a low overpotential of 229 mV for the oxygen evolution reaction (OER), and 151 mV for the hydrogen evolution reaction (HER) and a full cell voltage of 1.62 V at 10 mA cm−2 current density. The core–shell heterostructure constructed by electrodeposition endows the catalyst with outstanding stability and low degradation in long-term catalytic processes as shown by continuous chronopotentiometry tests at current densities of 50, 100 and 200 mA cm−2 for 72 h. The as-prepared core–shell hierarchically heterostructural Co9S8/Ni3S2@NiFe-120 with high-efficiency and good-durability is a promising bifunctional electrocatalyst towards practical applications in overall water splitting.
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ACS Sustainable Chemistry & Engineering
·
2021
·
IF 8.198
Baojin Chen,Muhammad Humayun,Yadong Li,Huaming Zhang,Huachuan Sun,Ying Wu,Chundong Wang
Exploration of highly efficient bifunctional electrocatalysts for optimal hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) has been widely carried out, though it still remains a big challenge. Herein, a hierarchical CoO–Co4N@NiFe-LDH (layered-double-hydroxides) heterostructure electrode anchored on nickel foam (NF) is prepared via a developed three-step hydrothermal–nitridation–electrodeposition pathway. The fabricated CoO–Co4N@NiFe-LDH/NF electrode needs low overpotential values of 66 and 231 mV to supply a current density value of 10 mA cm–2 in aqueous solution of KOH (1 M) for HER and OER, respectively. The Tafel slopes and electrochemical impedance spectroscopy results display favorable reaction kinetics throughout the electrolysis process. Subsequently, an alkaline electrolyzer is assembled with CoO–Co4N@NiFe-LDH/NF, which serves both as the anode and cathode, yielding 10 mA cm–2 with a small voltage of 1.529 V and showing a robust stability for 28 h. Impressively, a urine-mediated electrolysis cell shows efficient catalytic activity as well, allowing to mount the sluggish OER during water splitting. To drive the urine-mediated electrolysis cell containing 0.33 M urea, a low voltage of 1.393 V is required, which is about 136 mV lower compared to the urea-free electrolysis cell. This work presents a solid step for the electrocatalytic generation of hydrogen through water splitting by harvesting low energy.
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JOURNAL OF MATERIALS SCIENCE
·
2020
·Vol. 55
·期 35
·16625-16640
·
IF 3.553
Zhang Zewu,Zhou Jiamin,Wei Hanlin,Dai Yifan,Li Shijia,Shi Haojun,Xu Gang
Abstract Efficient design and preparation of cost-effective and binder-free bifunctional electrocatalysts to accelerate the hydrogen and oxygen evolution reaction (HER and OER) are critical for overall water splitting. In this work, 3D hierarchical NiFe-LDH/FeCoS 2 /CFC electrodes were synthesized for the first time. The carboxyl groups derived from acid treating promote the homogeneously coated FeCoS 2 on CFC, giving rise to the strongly coupled FeCoS 2 /CFC hybrid. The NiFe-LDH exhibited the vertical growth feature on the FeCoS 2 /CFC composite, which can efficiently expose the active edges sites. Due to unique structure and synergistic effect between the components, the NiFe-LDH/FeCoS 2 /CFC exhibits significant electrocatalytic activity and stability under alkaline environments, with overpotentials of 190 and 308 mV to achieve 10 mA cm −2 for OER and HER, respectively, providing it as a promising electrocatalyst for water splitting reaction. In addition, we deeply studied the synergistic catalytic mechanism of NiFe-LDH/FeCoS 2 /CFC, explaining the reasons leading to the improved catalytic performance of HER and OER. Graphic abstract
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2020
·
IF 4.65
Yuanming Deng,Xi Zou,Zairan Liu,Jinzhi Wang,Zhong Wang,Jiaoning Tang
Here we present a simple method to prepare a highly efficient three components nanocomposites via thermal degradation of layered double metal hydroxides (LDHs)@polyvinyl alcohol (PVA) composites. Co 7 Fe 3 /CoFe 2 O 4 @C obtained from this method is applied to activate peroxymonosulfate (PMS) to degrade polluted organics and showed excellent performance. The best removal RhB efficiency of Co 7 Fe 3 /CoFe 2 O 4 @C (Co/Fe = 1:1) is near 100% within 10 min and the lowest ions elution (∼0.05 mg/L) under pH = 7, which is also better than the performance of the precursor Co–Fe LDH. Through further cycling experiments and degradation of p -nitrophenol, the stability and catalytic performance of the catalyst were verified. Finally, free radical scavenging experiments prove ·OH and SO 4 · - radicals participating in the reaction, which are the key factors for degradation. Based on the above, the derivation of the mechanism of Co 7 Fe 3 /CoFe 2 O 4 @C (Co/Fe = 1:1) catalyzing PMS to degrade polluted organics was proposed, and we consider this catalyst has great application prospect.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2020
·
IF 3.573
Qinglei Sun,Bo Chen
The serious pollution of water resources has brought great challenges to human existence; it is urgent to develop adsorbents for removing toxic dyes from wastewater. In this work, we synthesized hierarchically porous MgAl-layered double hydroxide (LDH)/carbon fiber (CF) composites with excellent adsorption of Congo red (CR) by combining the biotemplating and hydrothermal method. The effects of various Mg/Al molar ratios on the X-ray powder diffraction (XRD), scanning electron microscopy (SEM), Brunauer–Emmett–Teller (BET), and Fourier transform infrared (FT-IR) spectroscopy characterizations and the dye adsorption capacity of composites were investigated. Three-dimensionally stackable MgAl-LDH nanosheets with a Mg/Al molar ratio of 4 were attached uniformly on the surface of hollow carbon fibers calcined from cotton, generating higher crystallization and specific area. The maximum adsorption capacity of Mg4Al-LDH/CF was equal to 271.00 mg g–1 (linear Langmuir model, at 200 mg g–1 CR in 72 h), which was significantly higher than the adsorption capacity of MgAl-LDH synthesized without the use of a biotemplate (linear Langmuir model, 170.35 mg g–1 at 200 mg g–1 CR in 72 h). The adsorption reaction followed the linear pseudo-second-order kinetics as well as the linear Langmuir model. Anion exchange and electrostatic attraction were considered as the main adsorption mechanisms. Mg4Al-LDH/CF still maintained 85.33% of the maximum adsorption capacity after four adsorption–desorption cycles. The adsorbent synthesized by flexible and simple methods might be a competitive candidate to purify nondegradable substances from wastewater.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2020
·
IF 3.99
Tailong Cai,Xiaoyuan Shen,Erzhuo Huang,Yutao Yan,Xiaoping Shen,Fengqiang Wang,Zhe Wang,Qingfeng Sun
Wood is an important and ubiquitous material applied in building and decorative applications, but it is easily invaded by fire, water and microorganisms. In this study, a new Ag nanoparticles supported on MgAl-LDH decorated wood veneer is successfully developed via simple hydrothermal reaction and silver mirror reaction. This unique wood veneer shows excellent flame retardancy under a continuous open flame, and super water repellency with a large water contact angle of 156°. In addition, the wood veneer has admirable antimicrobial activity (e.g. Staphylococcus aureus and Escherichia coli ). This paper presents a novel route of synthesizing a well-designed wood based composite with enhanced flame retardancy, water repellency and antimicrobial activity, which greatly broadens the application range of wood.
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APPLIED CATALYSIS A-GENERAL
·
2020
·
IF 5.006
Sishi Zhang,Jie Xu,Hongmei Cheng,Cuicui Zang,Bin Sun,Heyan Jiang,Fengxia Bian
Atomic economy, non-toxicity, harmlessness and multidirectional selectivity advocated by green chemistry have increasingly become a hot and difficult research topic. Herein, we present a highly efficient, one-pot tandem and easy-to-operate method through which we could directly produce a broad range of multi-directional selective hydrogenated amines or N-alkyl aliphatic amines using aromatic nitro compounds as raw materials. Ru/LDH with characteristics of layered mesoporous structure, well dispersed small Ru nanoparticles and LDH stabilization to the Ru NPs was employed as the catalyst. It is remarkable that multi-directional superb chemoselectivity to aromatic amines, alicyclic amines as well as N-alkyl aliphatic amines could be achieved with excellent catalytic activity and recyclability by tuning reaction conditions over 5wt%Ru/LDH-2. Additionally, this catalytic system also exhibited attractive activity and multi-directional chemoselectivity in the hydrogenation of quinoline and its derivatives with solvents of different polarity. Chemoselectivity to 5,6,7,8-tetrahydroquinoline derivatives could reach as high as 95.6 %.
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DALTON TRANSACTIONS
·
2020
·Vol. 49
·期 29
·10203-10211
·
IF 4.174
Shaobin Li,Jing Pan,Fengbo Li,Li Zhang,Dongfeng Chai,Zhuanfang Zhang,Jianjiao Xin
A simple continuous hydrothermal method was used to synthesize a NiFe2O4@Ni–Mn LDH/NF composite. The layered structure provides a large void to transfer the electron effectively, and the composite materials exhibit remarkable electrochemical performance including excellent specific capacitance (1265 F g−1 at 1 A g−1) and remarkable cycling stability (the specific capacitance remains at 80.9% after 5000 cycles). In addition, the asymmetric supercapacitor exhibits a high energy density of 96.2 W h kg−1 at a power density of 700 W kg−1, and there is an extraordinarily good cycling stability with a capacity retention rate of 92.5% after 4000 cycles. The outcomes indicate that the NiFe2O4@Ni–Mn LDH/NF composite electrode has potential application as a high-performance supercapacitor.
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高影响因子
BIOELECTROCHEMISTRY
·
2021
·
IF 5.373
Mengmeng Zhang,Lisha Mei,Li Zhang,Xiao Wang,Xiaochen Liao,Xiuwen Qiao,Chenglin Hong
Electrochemical immunoassays are commonly used to detect biomarkers and Ti 3 C 2 MXene anchored CuAu-LDH two-dimensional hydroxide heterojunctions for dual-mode electrochemical immunosensors were fabricated in this work. Layered double hydroxides have a large surface area, high chemical stability, tunable metal composition and interchangeable anions, however, the insulating nature of LDH further limits its catalytic performance. For this reason, Ti 3 C 2 Mxenes were introduced to improve this problem. 2D layers of Ti 3 C 2 Mxenes with large specific surface area and excellent conductivity have been well proven and widely used. And the surface of Ti 3 C 2 Mxenes (due to the presence of abundant surface functional groups), will facilitate the anchoring of metal ions and the nucleation of LDH. In addition, its excellent electrical conductivity will facilitate the electron transfer between Cu 2+ and Cu + . The immunosensor not only showed a heavy square wave voltammetry (SWV) signal. It also exhibited high electrocatalytic activity for H 2 O 2 redox reactions and improves the sensitivity of the Ampere Current (i-t) detection. The CEA immunosensor developed in this study showed a wide linear response (0.0001–80 ng/mL) and the lowest detection limits (SWV: 33.6 fg/mL and i-t: 45.4 fg/mL S/N = 3). The results confirmed the excellent analytical capability of the immunosensor.
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APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Li Zhang,Xuerui Yang,Runsheng Zhou,Sen Lin,Lei Zhou
In this study, Ni/Co layered double hydroxide (Ni/Co-LDH) with uniform flake structure was synthesized successfully as an effective activator in the carbamazepine (CBZ) degradation by peroxymonosulfate (PMS). Our results indicated that Ni/Co-LDH possessed a high specific surface area (72.9942 m 2 /g) and exhibited great activation performance, in which 100% CBZ removal could be achieved within 300 s under neutral conditions with 5 mg/L Ni/Co-LDH and 0.3 mmol/L PMS. In addition, the crystal structure and morphology of the prepared Ni/Co-LDH kept unchanged during degradation cycles. X-ray photoelectron spectroscopy (XPS) analysis and free radical identification experiment speculated that the cycle of Ni 2+ /Ni 3+ and Co 2+ /Co 3+ on Ni/Co-LDH surface were responsible for efficient HO•/SO 4 •− generation from PMS. Based on identified products through high resolution mass spectrometry (HR-MS), it was proposed that the degradation pathway of CBZ was a heterozygous process involving deamidation, hydroxylation and electron transfer. The ECOSAR calculation results indicated the toxicity of some products was still at very toxic level, thus certain attention should be paid to the toxicity of intermediates in the process of treating pollutants in water.
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Materials
·
2018
·Vol. 11
·期 7
·1113
·
IF 2.467
Zhe Wang,Xiaoping Shen,Temeng Qian,Kang Xu,Qingfeng Sun,Chunde Jin
The hydrophilicity and flammability of fiberboards have limited their real-life applications. In this study, a facile strategy for preparing the multifunctional coatings with superhydrophobicity and flame retardancy on medium density fiberboards (MDFs) has been investigated. The superhydrophobic and flame-retardant coating on the MDF surface was obtained by depositing polydimethylsiloxane (PDMS) and 1H, 1H, 2H, 2H-perfluorodecyltrichlorosilane (FDTS)-modified Mg/Al layered double hydroxide (LDH) particles step by step. The as-prepared coating exhibited superhydrophobic properties with a water contact angle (WCA) of ~155° and good self-cleaning properties. Furthermore, the limiting oxygen index (LOI) value of the superhydrophobic MDFs increased by 60.4% as compared to that of the pristine MDFs, showing improved flame retardancy. The peak heat release rate (PHRR) and total heat release (THR) of MDFs decreased after coating with PDMS@FDTS-Mg/Al LDH, suggesting that the superhydrophobic coating decreased the fire growth speed and risk of fire hazard of MDFs. This coating with multiple functions opens a new avenue for the protection and functionalization of MDFs.Keywords:medium density fiberboard;Mg/Al LDH;FDTS;superhydrophobicity;flame retardancy
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BIOMATERIALS
·
2013
·
IF 7.604
Dian Li,Yu-Ting Zhang,Meng Yu,Jia Guo,Deeptangshu Chaudhary,Chang-Chun Wang
Hierarchical structured nanomaterials with diverse functionality, such as magnetic susceptibility , stimuli-responsiveness, environmental sensing and biocompatibility, are highly sought after for biomedicine and biodetection alike. In this study, we designed and fabricated a new kind of multifunctional core/shell nanospheres as biodegradable targeted drug carriers, the controlled drug release progress and therapeutic effect were monitored in-situ by the fluorescent state of the cells. Firstly, the core/shell nanospheres with biodegradability were synthesized using magnetic supraparticles (MSPs) as core and the layered double hydroxide (LDH) as shell via a hydrothermal route, the reaction parameters were well investigated to obtain the desired structure of the LDH shell. The anti-cancer drug doxorubicin was modified with carboxyl group (DOX-COOH) and loaded in the shell of MSPs/LDH nanospheres via an anion-exchange intercalation. To endow the nanospheres with tumor-targeting capability, IDA (iminodiacetic acid)-modified folate was successfully immobilized onto the surface of LDH shell using chelating interaction. These nanospheres behaved as multifunctional carriers for targeted delivery of anti-cancer drug, doxorubicin (DOX), within Hela cells and thus, these nano-drugs exhibited clear cytotoxicity and inhibition toward Hela cells as compared to normal cell-lines of HEK 293T cells. Interestingly, after the internalization of these nano-drugs, there was a sharp contrast in illumination between the tumorous Hela cells and the normal HEK 293T cells, the acidic cytoplasm of Hela cell stimulated DOX-COOH in LDH shell quickly degraded into positive-charged DOX, and then rapidly escaped from the positive-charged intercalation of LDH shell by strong repulsive interaction, the released DOX rapidly lit up the whole tumor cells in a short time, but only very weak light was found in HEK 293T cells.
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