CATALYSIS COMMUNICATIONS
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2022
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IF 3.51
De Gao,Feng Han,Geoffrey I.N. Waterhouse,Yan Li,Lili Zhang
A catalyst with high selectivity for the catalytic oxidation of 5-hydroxymethylfurfural (HMF) to 5-formyl-2-furanic acid (FFCA) in alkaline media was successfully developed by ultrasonic intercalation of a copper‑iron layered double hydroxide (CuFe-LDH) platelets with an iron phthalocyanine (FePc) complex. The effects of reaction temperature, reaction time, H 2 O 2 concentration, NaOH concentration and amount of catalyst on HMF conversion and FFCA selectivity were systematically investigated. Under the optimized testing condition the developed FePc-CuFe catalyst delivered a HMF conversion of 85% with a FFCA selectivity of 81.8%. Further, the catalyst showed excellent stability over 5 testing cycles.
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SURFACE & COATINGS TECHNOLOGY
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2022
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IF 4.865
Zheng Dou,You Zhang,Tatsiana Shulha,Ruige Cui,Maria Serdechnova,Haoyue Tian,Tengfei Yan,Carsten Blawert,Longxue Li,Mikhail L. Zheludkevich,Fei Chen
A strategy based on chelating agent addition was used to assist the in-situ growth of MgAl-layered double hydroxides (LDHs) films on magnesium alloy AZ31 in a relatively mild condition. The growth behavior of MgAl-LDH films was studied on the magnesium alloy AZ31 substrate as the sole source of Al 3+ and/or adding aluminum compounds as a supplementary source of respective ions. The composition, structure, corrosion resistance , and formation mechanism of LDH films were investigated and discussed. Results showed that the LDH-coated samples could effectively retard the corrosion of magnesium alloy. A thicker Mg (OH) 2 /MgAl-LDH composite film with larger flake size was formed without additional aluminum source. MgAl-LDH film fabricated with moderate additional Al 3+ concentrations showed better corrosion resistance and an interesting stable network structure on a flat surface both covered/consisting of very fine LDH flakes.
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SOLID STATE SCIENCES
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2022
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IF 3.752
Jyunhong Shen,Antong Shi,Mengfan Wu,Hongyu Zhang,Zhuwu Jiang
For the advanced treatment of micropollutants from wastewater, this study synthesized a ternary Ag/ZnO/ZnAl‒LDH composite photocatalyst with performance optimization based on the Taguchi approach. The optimal synthesis parameters were statistically determined as the Ag doping amount of 5 wt%, Zn 2+ and Al 3+ with a molar ratio of 3:1, Ag/ZnO and ZnAl‒LDH with composite ratio of 3:2, and PEG-200 dosage of 25 mL. The optimally synthesized Ag/ZnO/ZnAl‒LDH achieved the efficient degradation of bisphenol A (BPA) under visible light irradiation, and the reaction rate constant was about 4.8-, 2.2- and 12.0-fold higher than that of ZnO, Ag/ZnO and ZnAl‒LDH, respectively. As proved by various characterizations, the enhanced photocatalytic performance of Ag/ZnO/ZnAl‒LDH can be attributed to the improvements of optoelectronic properties, such as the widened visible light responsivity and facilitated charge transfer, thus resulting in a significant increase of hydroxyl radicals (·OH) formation. Fluorescence measurements and radical quenching experiments indicated that ·OH mainly contribute to the degradation of BPA, and the oxidation of H 2 O by holes was the dominant formation pathway. According to the above results, this study summarized and proposed the enhanced photocatalytic mechanism of Ag/ZnO/ZnAl‒LDH for ·OH production and BPA removal.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
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IF 8.128
Jingyi Zhu,Yixin Zhu,Wenjun Zhou
Oxygen vacancies (OVs) were introduced into Ni-based layered double hydroxides (LDHs) through Cu doping, and the catalytic performance of the resulting Ni x Cu-LDHs were investigated for peroxymonosulfate (PMS) activation and methyl 4-hydroxybenzoate (MeP) degradation. Compared with that of Ni-LDH, the catalytic performance of Ni x Cu-LDHs were significantly enhanced and increased with increasing OV content in the catalysts, indicating that Cu doping introduced OVs into Ni x Cu-LDHs and greatly improved their catalytic activity with PMS. Quenching experiments and EPR analyses confirmed that oxidation processes dominated by superoxide radicals (O 2 •− ) and singlet oxygen ( 1 O 2 ), rather than sulfate radicals (SO 4 •− ) or hydroxyl radicals (•OH) used by traditional LDH catalysts, were responsible for MeP degradation by Ni 15 Cu-LDHs. In addition, quenching experiments with different systems showed the fate of reduced SO 4 •− and •OH, and demonstrated that O 2 •− and 1 O 2 concentrations grew with increasing OV content, confirming that the presence of OVs affected the process of PMS activation. Notably, O 2 •− mainly originated from adsorbed oxygen or dissolved oxygen (DO) by acquiring electrons from OVs in Ni 15 Cu-LDHs, since OVs possess abundant localized electrons. Consequently, an OV-mediated oxidative mechanism was proposed for Ni 15 Cu-LDHs/PMS. This study provides new clues for enhancing the catalytic performance of LDH catalysts by introducing OVs via metal doping in PMS-based AOPs systems.
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PubMed
高影响因子
CRYSTENGCOMM
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2021
·Vol. 23
·期 11
·2262-2268
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IF 3.545
Jing He,Zhufeng Hu,Kuan Deng,Renjun Zhao,Xingbin Lv,Wen Tian,Yu Xin Zhang,Junyi Ji
A rational structural design of electrodes with high electron conductivity, sufficient material interfaces/defects and a regulated charge transfer pathway can be applied in broad practical electrochemical application fields. A triple-layered PPy@NiCo LDH/FeCo2O4 hybrid with a tri-metal hybrid nanowire and conductive PPy coating layer is fabricated via a one-step hydrothermal reaction and in situ polymerization. NiCo LDH/FeCo2O4 nanowire arrays with a layered crystalline structure are synthesized via an in situ dissolution-growth method, where the partially etched nickel foam substrate subsequently acts as the Ni source. The NiCo LDH/FeCo2O4 nanowire arrays together with the ultrathin PPy coating layer can form bi-continuous conductive networks, numerous crystalline edges and structural interfaces to increase the electron transfer rate and the active/adsorption sites, which can further promote the energy storage and electrocatalytic activity. The bi-functional PPy@NiFeCo/NF-4 electrode exhibits a high areal capacitance (9.24 F cm−2 at 5 mA cm−2) and excellent rate capability (90.5% retention from 5 to 30 mA cm−2) as a supercapacitor and achieves a small overpotential (244 mV at 50 mA cm−2) and Tafel slope (64.39 mV dec−1) as an electrocatalytic OER electrode.
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Journal of Energy Chemistry
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2020
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IF 7.216
Mei Li,Xiaohui Deng,Yue Liang,Kun Xiang,Dan Wu,Bin Zhao,Haipeng Yang,Jing-Li Luo,Xian-Zhu Fu
The inefficiency of water splitting is mainly due to the sluggish anodic water oxidation reaction. Replacing water oxidation with thermodynamically more favorable selective methanol oxidation reaction and developing robust bifunctional electrocatalysts are of great significance. Herein, a hierarchical heteronanostructure with Ni–Co layered double hydroxide (LDH) ultrathin nanosheets coated on cobalt phosphide nanosheets arrays (Co x P@NiCo-LDH) are fabricated and used for co-electrolysis of methanol/water to co-produce value-added formate and hydrogen with saving energy. Benefiting from the fast charge transfer introduced by phosphide nanoarrays, the synergy in nanosheets catalysts with hetero-interface, Co x P@NiCo-LDH/Ni foam (NF) exhibits superior electrocatalytic performance (10 mA cm −2 @ 1.24 V and −0.10 V for methanol selective oxidation and hydrogen evolution reaction , respectively). Furthermore, Co x P@NiCo-LDH/NF-based symmetric two-electrode electrolyzer drives a current density of 10 mA cm −2 with a low cell voltage of only 1.43 V and the Faradaic efficiency towards the generation of formate and H 2 are close to 100% in the tested range of current density (from 40 to 200 mA cm −2 ). This work highlights the positive effect of hetero-interaction in the design of more efficient eletrocatalysts and might guide the way towards facile upgrading of alcohols and energy-saving electrolytic H 2 co-generation.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2020
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IF 7.489
Ning Song,Shihuan Hong,Mengya Xiao,Yan Zuo,Enhui Jiang,Chunmei Li,Hongjun Dong
The application of NiCo-LDHs in the hydrogen evolution reaction (HER) is rarely reported because it is usually served as an effective electrocatalyst for oxygen evolution reaction (OER) owing to the essential chemical and electric structure features. It still is a challenge to realize the effective HER over NiCo-LDHs unless modified with noble metals . In this work, the noble-metal-free core–shell Co(OH) 2 @P-NiCo-LDH hybrid with dodecahedral hierarchical structure is prepared by the sacrificial template method along with subsequent phosphating process, which is available for the electrocatalytic HER. The fabricated Co(Ni) δ+ -P δ- bonding states on the surface of outer shell NiCo-LDH not only provide the abundant active centers but also reduce interfacial charge transfer resistance to enhance the HER activity. Meanwhile, the unique core–shell dodecahedral structure effectively avoids the agglomeration and restacking of NiCo-LDH nanosheets to improve the electrochemical stability. This work exploits a novel noble-metal-free modification strategy to expand the application of NiCo-LDH in HER.
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Molecular Catalysis
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2020
·
IF 3.687
Yang Zhong,Bo Zhou,Lijun Wang
Fe/FeO x embedded in LDH was prepared by reducing the pre-synthesized [Fe(C 2 O 4 ) 3 ] 3− anions intercalated LDH and used as a multi-functional catalyst for synthesis of C7-C9 compound via transfer hydrogenation between furfural (C5) and short-chain alcohols (C2-C4) and a subsequent aldol reaction of furfural with intermediate short-chain aldehydes in the absence of a homogeneous base with furfuryl alcohol as a byproduct. Screening reaction conditions, evaluation and improvement of the cyclic catalytic performance, and determination of catalytically active components were performed, and the results demonstrated that both high conversion and high selectivity to the C C bond forming product can be obtained under a non-oxidizing atmosphere of Ar or H 2 /Ar mixed gas, a reaction temperature of 140 °C and a reaction time of 4 h; the catalyst was easily deactivated during the cycle experiments, however, its catalytic stability can be effectively improved by depositing Ni with weak reducibility on the surface of Fe nanoparticles at the cost of reducing partial catalytic activity. Fe/FeO x together with LDH as a whole proved to be effective in catalyzing the transfer hydrogenation reaction and the support LDH imparted basic catalytic function to the composite realizing the aldol reaction in the absence of a homogeneous base.
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CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Sa Wang,Shuqing Yang,Zhuolin Cui,Xueyan Liu,Yu Yang,Tao Wang,Wenjuan Ma,Yubin Zhou,Ruizheng Liang,Dan Yan,Huizhi Chen
Precise activation of therapeutic molecules in tumor tissues is the key step to ensure targeted antitumor performance and reduce adverse effects towards normal tissues and organs. Although the copper(I)-catalyzed azide-alkyne cycloaddition (CuAAC), i.e., bioorthogonal chemistry, has been used for the rapid synthesis of anticancer drugs in cells, it remains a great challenge to realize precise in vivo drug synthesis in tumor sites for precise cancer treatment. In this work, we first report the in-situ activation of CuAl-layered double hydroxide (CuAl-LDH) nanosheets to realize Cu(I)-catalyzed bioorthogonal chemistry in vivo in tumor microenvironment (TME) for precise chemotherapy and chemodynamic therapy (CDT). The Cu(II) ions in the biocompatible CuAl-LDH nanosheets can be in-situ reduced to Cu(I) ions partially by the overexpressed glutathione in TME. The generated Cu(I) can serve as a catalyst to catalyze the CuAAC reaction between alkyne and azide in TME, thus realizing in vivo drug synthesis for precise chemotherapy. Meanwhile, the generated Cu(I) can catalyze the Fenton-like reaction to generate toxic hydroxyl radicals (⋅OH) from H 2 O 2 in TME for CDT. Therefore, CuAl-LDHs can be used for the targeted synergistic chemotherapy and CDT to achieve highly precise and efficient elimination of cancer cells in vitro and inhibition of tumors in vivo .
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CHEMICAL ENGINEERING JOURNAL
·
2026
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IF 12.5
Cui Qiao,Yunong Li,Yong Li,Yuhao Han,Li Dong,Zifeng Yang,Yifan Liu,Suojiang Zhang
MgFe-LDH/CNT-COOH composite with branch-leaf-like architecture is fabricated via in-situ co-precipitation. • MgFe-LDH/CNT-COOH shows better activity and stability compared with various solid base catalysts. • Interfacial Fe–O–C bonds boost Lewis acidity and acid-base synergy. • Interfacial electronic engineering creates acid-base synergy beyond conventional basicity-dominated paradigm. Layered double hydroxides (LDHs) are promising solid base catalysts for the transesterification of ethylene carbonate (EC) with methanol to produce dimethyl carbonate (DMC), but their catalytic efficiency is often limited by severe nanosheet aggregation and insufficient regulation of active sites. Herein, a branch-leaf-like hierarchical MgFe-LDH/CNT-COOH composite was constructed via an in-situ co-precipitation strategy. The optimized composite achieved a DMC yield of 75% with a turnover frequency (TOF) of 116.14 h −1 at 60 °C. Notably, despite its lower total basicity than pristine MgFe-LDH, the composite exhibited significantly enhanced catalytic activity, indicating that the overall basicity alone does not govern the catalytic performance. Synchrotron X-ray absorption spectroscopy and density functional theory calculations revealed that the enhanced activity is closely associated with the formation of interfacial Fe–O–C bonds between MgFe-LDH and CNT-COOH. The interfacial bonding induces electron withdrawal from Fe 3+ centers and shifts the Fe 3d-band center closer to the Fermi level, thereby strengthening Lewis acidity. The enhanced Lewis acid sites facilitate the activation of EC, while the coexisting basic sites promote methanol activation, resulting in efficient acid-base synergistic catalysis. This work demonstrates that interfacial electronic modulation in hierarchical LDH-based composites provides an effective strategy for constructing high-performance acid-base synergistic catalysts. Download: Download high-res image (261KB) Download: Download full-size image
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ACS Sustainable Chemistry & Engineering
·
2023
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IF 8.4
Ran Li,Deliang Zhang,Huamao Chen,Shaozhen Wang,Yunyun Ling,Caihong Fang
Developing high-performance and low-cost electrocatalysts for the oxygen evolution reaction (OER) and urea oxidation reaction (UOR) is essential for hydrogen production. Herein, we prepared Zn,S-incorporated Fe,Co layered double hydroxide (ZnCoFeS–LDH) nanosheets on nickel foam via a two-step hydrothermal reaction. The attractive two-dimensional (2D) nanosheet morphology with ultrathin thickness offers abundant active sites, promotes the adsorption and desorption of intermediates on the surface, and also facilitates mass transportation. The electronic structure of ZnCoFeS–LDH was modified, which thus improves their conductivity, offers high-valence iron ions (Fe3+), and therefore intrinsically enhances their electrocatalytic properties. In particular, the constructed crystalline/amorphous interfaces benefit electron transfer between different phases. As a proof of concept, we examined the electrocatalytic performances of ZnCoFeS–LDH nanostructures to both the OER and UOR. As a result, the ZnCoFeS–LDH nanosheets exhibit excellent catalytic OER activity, with low overpotentials of 202, 217, 238, and 261 mV to achieve current densities of 10, 20, 50, and 100 mA cm–2, respectively, which are remarkably enhanced in comparison with that of commercial RuO2. Furthermore, they also demonstrate outstanding durability after long-term (48 h) and cycling (5000 cycles) measurements. Moreover, the ZnCoFeS–LDH nanosheets also possess superior UOR activity. The potentials were measured to be as low as 1.313, 1.334, 1.366, and 1.398 V to reach current densities of 10, 20, 50, and 100 mA cm–2, respectively, with high long-term stability after 20 h.
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FOOD CHEMISTRY
·
2023
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IF 8.8
Xin Tang,Shan Zhao,Jiaying Wu,Zhiyuan He,Yu Zhang,Ke Huang,Zhirong Zou,Xiaoli Xiong
It is necessary to efficient detection hydrazine in food . Exploring highly sensitive, low-cost and fast response electrochemical hydrazine sensing methods has been a challenge in this field. In this paper, a conformal transformation method is used to prepare rose flower-like NiCo-LDH derivating from the bimetallic NiCo-MOFs, and the N 2 H 4 sensing platform with a large electrocatalytic area, high conductivity and good stability was constructed. Based on the synergy between Ni and Co and the remarkable catalytic activity of the rough 3D flower-like structure, the N 2 H 4 sensor has a linear response in the concentration range of 0.001–1 mmol/L and 1–7 mmol/L, with a sensitivity of 5342 μA L mmol −1 cm −2 and 2965 μA L mmol −1 cm −2 (S/N = 3), respectively, and low limit of detection of 0.043 μmol/L. This study opens a new door for the successful application of electrochemical sensors to detect N 2 H 4 in real food samples.
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