Nanomaterials
·
2025
·Vol. 15
·期 6
·432
·
IF 4.3
Xin Zhong,Xiaojun Liu,Meihuan Ji,Fubin Jiang
As the most promising techniques for refractory antibiotic degradation in wastewater management, sulfate radical-based advanced oxidation processes (SR-AOPs) have attracted considerable attention. However, systematic studies on potassium peroxymonosulfate (PMS) activation by MOF-derived metal oxides coated with LDH materials are still lacking. In this work, a series of catalysts consisting of CoCu-MOFs coated with CuAl/LDH were synthesized for PMS activation in the removal of sulfamethoxazole (SMX). As expected, CoCu-MOFs coated with CuAl/LDH catalyst showed high SMX removal and stability in PMS activation. In the CoCu/LDH/PMS reaction, the SMX removal was nearly 100% after 60 min, and the mineralization reached 53.7%. The catalyst showed excellent catalytic stability and low metal leaching concentrations (Co: 0.013 mg/L, Cu: 0.313 mg/L), as detected by ICP. Sulfate radicals and hydroxyl radicals were identified as the dominant reactive species in the CoCu/LDH/PMS system. Moreover, the presence of 1 O 2 in the process revealed the coupling of non-radical and radical processes. The XPS results showed that the layered structure of CoCu/LDH promoted the recycling of metal ions (high and low valence), which facilitated heterogeneous PMS activation. The effects of different reaction conditions and reuse cycles were also determined. The SMX oxidation pathways were proposed based on the intermediates identified by LC/MS. The high activity and stability of CoCu/LDH provide a new mechanistic understanding of PMS activation catalysts and their potential utilization in practical wastewater treatment.
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JOURNAL OF SOLID STATE CHEMISTRY
·
2024
·
IF 3.2
Wei Xia,Gui-Zhi Guo,Xue-Qian Wu,Ya-Meng Yin,Ya-Pan Wu,Shuang Li,Ruan Chi,Dong-Sheng Li
Direct methanol fuel cells (DMFCs) can permit the utilization of noble-metal-free electrocatalysts , which certainly reduces the cost and accelerates their practical implementation. With the exploration of efficient and economical methanol oxidation reaction (MOR) catalysts, Ni-based nanostructures have been recognized as the most promising MOR catalysts in alkaline media. Herein, we construct a novel heterojunction MOR electrocatalyst composed of Ni-based metal-organic framework (Ni-MOF) and NiFe-based layered double hydroxides (LDHs) through a coordination-induced self-assembly strategy. Owing to the synergic effect between Ni and Fe sites, coupled with the effect of hetero-interface, the resultant Ni-MOF/NiFe-LDH composite exhibits remarkable MOR activity in 0.1 M KOH electrolyte with the oxidation current density (32.66 mA cm −2 ) is 2.65 and 2.44 times higher than that of the primitive NiFe-LDH and Ni-MOF. The excellent stability of the Ni-MOF/NiFe-LDH electrocatalyst has also been confirmed by long-term chronoamperometry (CA) analysis. Our work paves a facile controllable way for fabricating MOF/LDH heterostructure targets on MOR and underlines its potential to boost energy conversion efficiency through the manipulation of synergic components.
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COMPOSITES PART B-ENGINEERING
·
2025
·
IF 14.2
Muyang Shi,Lu Wang,Dong Zhang
The suboptimal multifunctionality exhibited by structural supercapacitors (SSC) can be ascribed to a range of factors, encompassing the trade-off between electrical and mechanical performance of electrolyte, an inadequate interface contact between the electrode and electrolyte, as well as sluggish ion transport in the electrode and electrolyte. Herein, a new SSC architecture is introduced. First, the molybdate-ion-intercalated NiCo-LDH electrode is prepared by a convenient hydrothermal process. Benefiting from the unique 3D flower-like structure and MoO 4 2− doping effect, the as-prepared NiCo-LDH-MoO 4 2- -1 possesses high capacitance (1937.7 F g −1 ) and reversible charge-discharge stability. Subsequently, the PVA/PAA-cement composite is prepared by constructing a dual polymer-cement interwoven network. The rich intertwined network structure endows the composite with excellent mechanical and electrical properties, manifesting in a 189 % improvement in compressive strength and a 427 % augmentation in ionic conductivity compared to the pure cement. Meanwhile, an all-in-one SSC is assembled by an integrated polymerization-hydration synchronization strategy to improve interface contact. The resulting device presents superb energy density of 37.1 Wh kg −1 and long-life cycles. On the basis of these unique features, the device can be integrated into houses or road substrates for energy autarkic shelters and self-charging roads, which will significantly contribute to the development of new energy technologies and carbon neutrality fields.
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ELECTROCHIMICA ACTA
·
2024
·
IF 5.5
Shilong Wang,Chuqi Li,Ziyun Zhang,Lei Li,Wentao Ding,Sheng Han,Jibo Jiang
Engineering a heterogeneous structure with distinctive morphology and nanostructure is deemed to be an efficacious tactic for realising high energy density supercapacitors (SCs). Herein, the FeCo 2 S 4 @NiCo-LDH(FeCoS@NiCo-LDH)/NF nanocomposite heterostructure is successfully constructed through a facile two-step electrodeposition method. This heterostructure merges the merits of FeCoS with high electrical conductivity and NiCo-LDH with ultra-high specific surface area, which not only can deliver sufficient electroactive central sites, but also provide shorter routes for expedited ion diffusion, even more significantly, the heterogeneous interfaces that emerge in composites can moderate their electronic structure and augment electrical conductivity. Density functional theory (DFT) calculations indicate that the heterostructured FeCoS@NiCo-LDH/NF displays preferable electrochemical activeness and enhanced adsorption ability. Thanks to the abundance of heterogeneous interfaces and synergistic effects of the various active ingredients, FeCoS/NiCo-LDH electrodes exhibit an extraordinary specific capacity of 930 C g −1 at 1 A g −1 together with remarkable cycle longevity (10.9 % capacity decay after 10,000 cycles). In addition, a hybrid FeCoS@NiCo-LDH/NF//AC exhibits a high energy density of 52.81 Wh kg −1 at the 750 W kg −1 .
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JOURNAL OF ENVIRONMENTAL MANAGEMENT
·
2024
·
IF 8
Jiangfu Zheng,Changzheng Fan,Xiaoming Li,Qi Yang,Dongbo Wang,Abing Duan,Shuaijun Pan,Fengyuan You
The construction and precise synthesis of materials based on functional and structural orientations have emerged as a pivotal platform in the field of environmental management. In this paper, an efficient and stable catalyst (RuLDH) was constructed to achieve this goal. RuLDH comprises individual Ru atoms that are uniformly dispersed on ZnAl-LDH, achieved by room temperature stirring. Remarkably, RuLDH exhibits exceptional performance under visible light, effectively triggering the photocatalytic degradation of tetracycline hydrochloride (TC) via peroxymonosulfate (PMS) with a remarkable efficiency of 100%, all while avoiding the generation of highly toxic intermediates. In addition, RuLDH0.2 demonstrated its utility in fluorescence detection of TC, showcasing commendable analytical performance characterized by rapid response, low detection limit, and robust resistance to environmental interferences (with a detection limit of 1.0 mg/L). Notably, the RuLDH0.2/PMS/Vis system exhibited remarkable efficacy in treating actual pesticide wastewater, effectively exerting bactericidal and disinfectant effects. This study serves as a source of inspiration for the design of multifunctional single-atom catalysts, thereby pushing the boundaries of "integration of diagnosis and treatment" in environmental management and control.
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JOURNAL OF HAZARDOUS MATERIALS
·
2025
·
IF 11.3
Shuwen Peng,Yuran Li,Bin Wang,Yanbin Cui,Jinglei Tian,Hongqiang Liu,Tingyu Zhu
Removal of sulfur species from blast furnace gas is urgently needed due to the strict emission limits imposed on iron-steel industrial flue gas. Improving the sulfur capacity of H 2 S is a crucial challenge to reduce the operation cost. NiFe layered double hydroxide (LDH) adsorbents were synthesized using the hydrothermal method to strengthen the adsorption of H 2 S, achieving a high sulfur capacity of 133.6 mg/g at 50 °C. Characterization studies have revealed that the reaction pathway of H 2 S on the NiFe LDH surface involves adsorption, dissociation and oxidation. It has been clarified that the high sulfur capacity can be attributed to the abundant H 2 S dissociation sites and the excellent O 2 activation sites. The dissociation sites of H 2 S encompass metal sites, -OH and CO 3 2- . The interaction between O 2 and the bridge site of asymmetric metal atoms significantly enhances the dissociation of O 2 . Strengthening the dissociation of H 2 S and O 2 improves the sulfur capacity. The deactivation of adsorbents comes from the continuous consumption of oxygen species mainly composed of -OH and the deposition of sulfur species in the smaller mesopores ranging from 2 to 10 nm. This work provides useful insights into designing highly efficient iron-based adsorbents for the desulfurization of blast furnace gas.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Zhimin Li,Guanhui Chen,Shuqi Gou,Xiaofang Deng,Zhongai Hu,Xiaoquan Lu
The quasi-solid-state flexible supercapacitor has been successfully built by freezing-thawing method and in-situ polymerization. The high redox activity nickel-iron layered double hydroxide (NiFe-LDH) provides certain pseudocapacitance, interacts with high conductivity reduced graphene oxide (RGO), and avoids the activity structural collapse and agglomeration. Polyvinyl alcohol (PVA) serves as a flexible framework with uniform cross-linking between the components, facilitated by the presence of abundant hydrogen bonds. Polypyrrole (PPy) is further polymerized in-situ into PVA/RGO/NiFe-LDH to improve its electrochemical performance and flexibility. The PVA/RGO/NiFe-LDH 0.40 /PPy hydrogel electrodes exhibit a high area specific capacitance of 729 mF/cm 2 at 1 mA/cm 2 . The elongation at break of the electrodes is up to 749 %, which reflects excellent tensile properties. The quasi-solid-state flexible supercapacitor has been built using PVA/H 2 SO 4 as the gel electrolyte and PVA/RGO/NiFe-LDH 0.40 /PPy as the electrodes. The device exhibits a high energy density of 15.9 µWh/cm 2 at a power density of 0.19 mW/cm 2 and the capacitance retention of 96.7 % after 10,000 charge-discharge cycles.
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Nanoscale
·
2024
·Vol. 16
·期 7
·3650-3658
·
IF 5.8
Jun Tang,Jinzhao Huang,Sixuan Zhang,Zehui Liu,Jing Xiao
Although molybdenum disulfide (MoS2) has garnered significant interest as a potential catalyst for the oxygen evolution reaction (OER), its poor intrinsic activity and few marginal active spots restrict its electrocatalytic activity. Herein, we successfully constructed a catalyst via a simple hydrothermal method by forming a heterostructure of MoS2 with Cr-doped nickel–iron hydroxide (NiFe LDH) to synthesize a MoS2/NiFeCr LDH catalyst to significantly improve the OER catalytic performance. MoS2 plays a crucial function as an electron transport channel in the MoS2/NiFeCr LDH heterostructure, which increases the electron transport rate. Furthermore, a larger active surface area for NiFeCr LDH is provided by the ultrathin layered structure of MoS2, increasing the number of active sites and encouraging the OER. On the other hand, the introduction of Cr element increased the density of the catalytic center and provided additional Cr-OH active sites, which accelerated the oxygen decomposition reaction. These two factors act synergistically to improve the intrinsic structure of MoS2, increase the number of reactive sites, and dramatically enhance the OER catalytic performance. Excellent OER activity is demonstrated by the MoS2/NiFeCr LDH catalyst, which only needs an overpotential of 224 mV to obtain a current density of 10 mA cm−2 and a Tafel slope of 61 mV dec−1. The catalyst also demonstrated outstanding stability, with its activity practically holding steady after 48 h of testing. This work offers novel ideas for enhancing and designing MoS2-based OER catalysts, and it provides a crucial reference for research in the field of clean energy.
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ADVANCED MATERIALS
·
2024
·Vol. 36
·期 30
·2401694
·
IF 27.4
Yin Zhu,Yanxu Chen,Yafei Feng,Xiangmin Meng,Jing Xia,Genqiang Zhang
Hydrazine oxidation-assisted water splitting is a critical technology to tackle the high energy consumption in large-scale H 2 production. Ru-based electrocatalysts hold promise for synergetic hydrogen reduction (HER) and hydrazine oxidation (HzOR) catalysis but are hindered by excessive superficial adsorption of reactant intermediate. Herein, this work designs Ru cluster anchoring on NiFe-LDH (denoted as Ru c /NiFe-LDH), which effectively enhances the intermediate adsorption capacity of Ru by constructing Ru─O─Ni/Fe bridges. Notably, it achieves an industrial current density of 1 A cm −2 at an unprecedentedly low voltage of 0.43 V, saving 3.94 kWh m −3 H2 in energy, and exhibits remarkable stability over 120 h at a high current density of 5 A cm −2 . Advanced characterizations and theoretical calculation reveal that the presence of Ru─O─Ni/Fe bridges widens the d-band width (W d ) of the Ru cluster, leading to a lower d-band center and higher electron occupation on antibonding orbitals, thereby facilitating moderate adsorption energy and enhanced catalytic activity of Ru.
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IONICS
·
2025
·
IF 2.6
Jiang Zhuwu,Tu Zhehan,Xu Dongdong,Chen Jinfeng,Yang Jiahan,Zhang Fengying,Lin Weixin,Bai Xue,Zhang Hongyu
In the process of sterilization and disinfection, chemical reagents will react with natural organic matter and inorganic matter in water, and inevitably generate disinfection byproducts. These harmful substances are carcinogenic, teratogenic and mutagenic, and their content is low and difficult to detect. Therefore, in this study, we prepare Fe/CoFe-LDH electrodes by in-situ co-precipitation method, and their special structures and morphologies are used to achieve efficient removal of disinfection byproducts. On this basis, the prediction model of trichloroacetamide removal rate is constructed by using the backpropagation neural network, and the prediction model is used to predict the trichloroacetamide removal rate under different experimental parameters and the experiment is verified. The optimal process conditions are obtained, and the maximum trichloroacetamide removal rate is up to 81.62%. The feasibility of the data analysis and processing method based on machine learning in the prediction of disinfection by-products in drinking water is effectively proved.
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Journal of Materials Chemistry A
·
2024
·
IF 10.7
Hongtao Zhou,Xuefeng Sha,Fan Zeng,Xueli Wu,Minghao Yu,Zhidan Shi,Xingang Zhang,Xianyin Song,Changzhong Jiang
Nickel–cobalt layered double hydroxide (NiCo-LDH) is a promising electrode material for supercapacitors due to its high electrochemical activity. However, it easily restacks and aggregates due to its nanosheet structure, which limits the effective utilization of redox active sites. Herein, the NiCo-LDH nanosheets derived from ZIF-67 were in situ grown on the surface of a basic copper cobalt carbonate (CoCu) urchin-like skeleton and supported by nickel foam (CoCu@NiCo-LDH). The well-designed three-dimensional (3D) hierarchical nanostructure not only effectively prevents the aggregation of NiCo-LDH nanosheets, but also provides a rapid charge transport channel, which facilitates ion diffusion and electron transport, therefore enhancing the utilization of NiCo-LDH redox active sites to a greater extent. Besides, the synergistic interactions between NiCo-LDH nanosheets and CoCu nanoneedles further enrich the redox reactions and increase the electrical conductivity and reaction kinetics of the electrode at the same time. As a result, the CoCu@NiCo-LDH electrode exhibits outstanding electrochemical performance with an ultrahigh mass loading of 14 mg cm−2, including excellent specific capacitance (18.71 F cm−2 or 1346 F g−1 at 3 mA cm−2) and distinguished rate capability of 87.3% from 3 mA cm−2 to 50 mA cm−2. When the CoCu@NiCo-LDH electrode was assembled with active carbon (AC) to form an asymmetric supercapacitor (ASC), the CoCu@NiCo-LDH//AC ASCs display outstanding energy density (1.98 mW h cm−2) and power density (97.5 mW cm−2) with excellent cycling stability (86.0% initial capacitance after 5000 cycles), and could keep an LED light bulb working for 90 min after only charging for 60 s. This work provides an effective strategy for the design and application of layered double hydroxide based pseudocapacitors.
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APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Xuan Wei,Mingjie Li,Linlin Li,Wanzhong Feng,Hongyue Wu
Supercapacitors, as advanced electronic devices and energy storage systems for the next generation of electric vehicles, have garnered significant attention owing to their myriad of beneficial attributes. Compared to bimetallic layered double hydroxides (LDH) materials, trimetallic LDH exhibits superior electronic conductivity, faster ion diffusion, and minimal volume variation when employed as supercapacitor electrodes. In this work, the novel NiCoCu-LDH/black phosphorus quantum dots (BPQD) are directly anchored to carbon cloth (CC) using a simple precipitation method combined with hydrothermal technology, along with electrostatic adsorption. Due to abundant active sites, enhanced electron transfer, and stable microstructure, the pseudocapacitance of the prepared CC@NiCoCu-LDH/BPQD is about 1810.6F g −1 (1 A/g). In addition, the assembled asymmetric supercapacitor CC@NiCoCu-LDH/BPQD//activated carbon demonstrates an exceptionally high energy density (202.2Wh kg −1 @800 W kg −1 ) at a satisfactory operating voltage of 1.6 V, along with an extended cycle life, maintaining about 81.4 % capacitance after 10,000 cycles.
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