ACS Applied Materials & Interfaces
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2017
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IF 7.504
Yanna Wang,Liguang Dou,Hui Zhang
A series of novel nanosheet array-like catalysts Pdx/rGO@CoAl-LDH (x = 0.0098–1.9, refers to Pd loading in wt % on ICP, rGO: reduced graphene oxide, LDH: layered double hydroxide) were first prepared via a simple and green lattice atomic-confined in situ reduction of oxidative Pd precursors by the evenly atomic-dispersed reductive Co2+ sites on LDH layers of a nanohybrid rGO@CoAl-LDH with hexagonal LDH nanoplates (∼73 × 7 nm) interdigitated vertical to the surfaces of rGO layer in both sides, fabricated through a simple citric acid-assisted aqueous-phase coprecipitation method. The as-obtained Pd catalysts possess clean Pd nanoclusters (NCs) with tunable sizes in 1.3–1.8 nm on varied Pd loadings. All the Pdx/rGO@CoAl-LDH catalysts show excellent activities for the Heck reaction, and the Pd0.0098/rGO@CoAl-LDH with the ultrafine Pd NCs of 1.3 ± 0.2 nm yields a maximum turnover frequency of 160 000 h–1 over a heterogeneous catalyst so far. The excellent activities can be attributed to the ultrasmall Pd NCs with high dispersion and clean Pd surfaces, increased electron transfer capacity and surface area, and remarkable Pd–CoAl-LDH—rGO three-phase synergistic effect of the present unique nanosheet array-like Pd NCs catalysts. Moreover, the catalyst Pd0.33/rGO@CoAl-LDH shows a broad range of substrate applicability and can be reused more than five runs without obvious loss of activity, giving the present catalysts long-term stability. These findings make the rGO@CoAl-LDH hybrid prepared by a facile and scalable synthesis route a universal green platform to support other noble or nonprecious metal NCs via lattice atomic-confined in situ reduction strategy to construct more desired heterogeneous catalysts.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Jiangfu Zheng,Xiaoming Li,Qi Yang,Dongbo Wang,Abing Duan,Shuaijun Pan,Xuan Wu
Photocatalysts designed for all-weather applications, capable of efficient charge carrier separation, are set to transform the adoption of photocatalysis-driven advanced oxidation processes in wastewater management. In this investigation, an energy-storing ZnAl-LDH@SrAl 2 O 4 :Eu 2+ , Dy 3+ (SALDH) was synthesized successfully, optimized for the photocatalytic selective degradation of NTP and tetracycline hydrochloride (TC) under varying weather conditions, with 100 % degradation of both NTP and TC within 75 min. Remarkably, SALDH demonstrates energy storage capabilities that markedly reduce energy demands relative to traditional photocatalytic approaches. The primary reactive species identified were O 2 − , and the Fukui index, computed via density-functional theory (DFT), identified the specific interaction sites of O 2 − on NTP molecules. Utilizing the energy retention properties of SALDH, a novel, environmentally friendly device was engineered for processing organic pollutants in agricultural wastewater. This system harness the energy from solar radiation to induce the oxidation of pollutants. The experiments that were performed in the both artificially prepared lab-scale and actual agricultural WWT plants indicated the degradation efficiencies of 36 % and 37 %, respectively. As seen during the day, both SALDH and persulfate were capable of effectively decomposing organic contaminants; at night, the SA’s luminescence maintained the oxidative ability of ZnAl-LDH. Meanwhile, SALDH combines the corrosion resistance of ZnAl-LDH with good metal compatibility, enabling SALDH to effectively improve the photostability of long afterglow. This work contributes to the existing knowledge on the degradation of organic pollutants by efficient photocatalysts and points to possible implementations in water treatment processes.
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Kunpeng Song,Xue Bi,Dong Wang,Ye-Tang Pan,Meina Xie,Jiyu He,De-Yi Wang,Rongjie Yang
Preventing aggregation and inducing homogeneous dispersion of flame retardant nanofillers is critical to enhance the fire safety and mechanical properties of nanocomposites. Although chemical modifications are commonly used to improve the filler’s compatibility with the polymer chain, such methods are often cumbersome and limited. Herein, porous liquids (PLs) with flame retardant function were constructed in which porous defect-Co-LDH@ZIF-67 (d-LDH@ZIF) heterostructure particles were converted into liquid materials by electrostatic interaction with a large-volume solvent. This is also the first report of PLs in the field of flame retardant. Specifically, the d-LDH@ZIF heterostructure was designed by defect engineering and in situ growth strategy to compensate for the low catalytic activity and specific surface area of Co-LDH, and to serve as a rigid porous framework for PLs. Numerous cobalt/oxygen vacancies and lattice defects in the d-LDH@ZIF heterostructure have also been proven to confer higher flame retardancy relative to Co-LDH. d-LDH@ZIF porous liquids (PLs-d-L@Z) presents favorable liquid characteristics and achieves a monodisperse state in the polyurea matrix. The limiting oxygen index of polyurea composites blended with 20 wt% PLs-d-L@Z (3 wt% d-LDH@ZIF content) can be increased to 24.2 % and pass the V-0 rating in the UL-94 test. Moreover, the peak of heat release rate, total heat release, and total smoke production are reduced by around 40.4, 27.0, and 39.9 %, respectively, compared to neat polyurea. Emphatically, the PLs-modified polyurea composites exhibit significantly improved mechanical and impact resistance properties, as well as favorable chemical resistance. This strategy of liquefying solid flame retardant fillers will open an avenue to the design of functional nanomaterials for fire safety and other potential applications.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Hong Jia,Mengyang Wang,Mengyao Feng,Guangzhi Li,Longhua Li,Yu Liu
Constructing heterostructures with nanotube arrays not only provides rich ion electron pathways to promote rapid Faraday reactions, but also enhances interfacial electron transfer, supplying larger capacitance and rapid energy storage. Herein, NiCo-layered double hydroxide (LDH)/NiCo 2 S 4 nanotube arrays decorated with black phosphorus quantum dots (BPQD) is prepared through solvothermal method and electrostatic adsorption. In the unique structure, tubular structure of NiCo-LDH/NiCo 2 S 4 /BPQD nanoarrays on carbon cloth can expose sufficient redox reaction active sites and multiple ion diffusion channels to promote rapid faradic reactions. Density functional theory (DFT) theoretical calculations further confirm the enhancement of conductivity and OH – adsorption in ternary composite materials. The as-obtained NiCo-LDH/NiCo 2 S 4 /BPQD achieves an ultra-high capacitance of 2938.2F g −1 at 1.0 A g −1 . Finally, an asymmetric supercapacitor consists of activated carbon and NiCo-LDH/NiCo 2 S 4 /BPQD exhibits a satisfactory energy density of 133.7 Wh kg −1 at 800 W kg −1 . In addition, after 10,000 repetitions of charging/discharging, the capacitance still remains 76.5 %. Above results suggest that NiCo-LDH/NiCo 2 S 4 /BPQD electrode may facilitate the further development of hierarchical array structure electrodes in the energy storage field.
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JOURNAL OF CONTROLLED RELEASE
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2025
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IF 11.5
Meng Zhang,Yumei Wang,Jiayi Wang,Jiayi Zuo,Feng Jiang,Feng Cao
Neovascular ocular diseases are a leading cause of irreversible vision loss. Although intravitreal anti-VEGF therapy is the standard treatment, its invasive delivery and limited efficacy in some patients emphasize the need for non-invasive strategies targeting multiple angiogenic pathways. In this study, we developed a novel hybrid nanoplatform for the non-invasive co-delivery of axitinib (Axi) and telmisartan (Tel) to synergistically inhibit both VEGF and Ang-2 signaling pathways. Poorly soluble drugs were incorporated into layered double hydroxides (LDHs) via a micelle-assisted intercalation strategy and subsequently modified with hyaluronic acid (HA) conjugated to Gly-Val-Sar (GVS), a novel PepT1-targeted tripeptide. The Zn-containing LDH provided controlled drug release, and exhibited anti-inflammatory properties. HA modification prolonged ocular retention, and GVS enhanced transmembrane transport. The resulting Axi/Tel-D@LDH-HA-GVS nanocomposites demonstrated favorable physicochemical properties, efficient uptake by human conjunctival and retinal pigment epithelial cells, and potent inhibition of hypoxia-induced angiogenesis in vitro. In vivo, the formulations exhibited prolonged ocular retention, effective posterior tissue distribution, and good biosafety. In a diabetic retinopathy model, Axi/Tel-D@LDH-HA-GVS nanocomposites restored retinal structure and markedly reduced the expression of VEGF, Ang-2, TNF-α, and IL-6. Collectively, this study provides a promising non-invasive and synergistic strategy for targeted treatment of ocular neovascular diseases.
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高影响因子
APPLIED SURFACE SCIENCE
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2021
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IF 6.707
Tianyu Wang,Yong Yang,Qinghua Deng,Xiaoyue Zhang,Lijun Xiong,Zheng Tang,Panjie Li,Nan Yin,Aiwu Sun,Dan Chen,Jinyou Shen
Developing of a photocatalyst for multiple antibiotics degradation and revealing their different mechanism are of great importance for wastewater remediation. Herein, a 3D marigold-like CoAl-LDH/Ti 3 C 2 hybrid is developed via in situ growth of CoAl-LDH on Ti 3 C 2 nanosheets and on-spot self-assembly during the hydrothermal process. The existence of optimized Ti 3 C 2 steers the morphology evolution from 2D lotus leaf-like nanoplate to 3D marigold-like hierarchical architecture, which greatly boosts the adsorption capacity and photon capture of the catalyst by the increased specific surface area and the scattering cross section. Meanwhile, the well-defined 2D/2D interface between the components effectively promotes the electron transfer from CoAl-LDH to Ti 3 C 2 , and the photoinduced electron-hole pairs on CoAl-LDH can be greatly separated. The density functional theory (DFT) calculations further demonstrate the change of electronic structure for the composite photocatalyst. As a result, CoAl-LDH/Ti 3 C 2 hybrid presents 85%, 56% and 70% degradation efficiency towards tetracycline hydrochloride, chloramphenicol and terramycin, which are 3.1, 3 and 2.1 times of the pristine CoAl-LDH. Furthermore, the degradation path for chloramphenicol is explored and the reason for its different degradation efficiency is revealed. The design of 3D hierarchical scaffold cooperating with 2D/2D heterogeneous interface provides a new avenue to develop ideal catalysts for wastewater remediation.
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高影响因子
Desalination and Water Treatment
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2024
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IF 1
Huali Zhang,Jiaxin Zhang,Hanjun Wu,Yi Pan,Yan Xia,Zhiquan Pan,Dongshen Wang
In this work, heterogeneous catalysts of Cu(II)-ethylenediamine tetramethylene phosphonic acid (Cu(II)-EDTMPA) complex intercalated layered double hydroxides (EDTMPA-Cu-LDH) was synthesized by co-precipitation method for visible-light photocatalytic degradation of Rhodamine B (RhB). The synthesized catalysts were characterized by X-ray diffraction, Fourier-transform infrared spectroscopy, scanning electron microscopy, transmission electron microscopy, UV-Vis diffuse reflectance spectroscopy, and X-ray photoelectron spectroscopy. The results indicated that the EDTMPA-Cu-LDH showed a typical layered structure. After intercalation, layer spacing increased from 7.96 to 12.21 Å. The catalysts showed excellent catalytic activity for the degradation of RhB in visible light. The optimum conditions for RhB degradation were confirmed to be natural initial pH value 5.85, 10 mmol L –1 of RhB concentration, 7 mmol L –1 of H 2 O 2 concentration, and 0.3 g L –1 of catalyst dosage. The maximum degradation efficiency was 98.2% under the optimum conditions and excellent reusability and stability were obtained in the regeneration test. In the end, the reaction mechanism that might exist in the heterogeneous UV-Fenton system was proposed.
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PROGRESS IN ORGANIC COATINGS
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2023
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IF 6.6
Chunlin Chen,Bin Wang,Guoqing Xiao,Fei Zhong,Jian Zhou,Min Cao,Zhengwei Yang,Chunyan Chen,Rui Zou
In this study, phytic acid -doped polyaniline (PPA) was loaded on the surface of carbon spheres, resulting in a classical C-N-P flame retardant system, that has a beneficial function for the formation of residual carbon. Subsequently, using this phosphorus-nitride carbon sphere (CS/PPA) as a carrier, flower-like Ni-Al-layered double hydroxide (Ni-Al/LDH) were uniformly grown on its surface, thus obtaining a novel nano-fire retardant with a graded structure to heighten the fire-resistant properties of aqueous epoxy resin . Importantly, the intervention of Ni-Al/LDH nanosheets not only imparts a gas-phase fire retardant function to the coating, but also the presence of Ni and Al bimetals can effectively catalyze the formation of more residual carbon in the combustion process. The highest residual carbon (30.7 %) in thermal weight loss experiments of the CS/PPA@Ni-Al/LDH/EP composite coating confirmed this view. Tests on the thermal insulation behavior of coatings illustrated that the backside temperature (168.8 °C) for CS/PPA@Ni-Al/LDH/EP was significantly smaller than that of other coatings, and that this optimum thermal shielding is inextricably linked to the high residual carbon and the residual metal oxides . Furthermore, the CS/PPA@Ni-Al/LDH/EP specimen shown the greatest expansion height (25.1 mm), expansion ratio (19.61) as well as the smallest smoke density rating (39.1 %), proving that its expansion property and smoke suppression were effectively improved. Moreover, the microstructure for the expanded carbon layer demonstrated that the CS/PPA@Ni-Al/LDH filled EP possessed a more complete and dense residual carbon after burning. Moreover, the high degree of graphitization of the residual carbon for CS/PPA@Ni-Al/LDH/EP determined its high thermal stability. The lowest cracked gas phase products and CO release of the CS/PPA@Ni-Al/LDH/EP composite coating during TG-IR testing confirmed its lowest fire toxicity. The development of such a composite flame retardant with a graded structure could help to advance the progress of waterborne intumescent fire coatings.
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高影响因子
APPLIED CLAY SCIENCE
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2020
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IF 4.605
Yufei Yuan,Cuiyan Tong,Changli Lü
ABSTRACT The low ionic conductivity and poor dimensional stability severely influence the application of anion exchange membranes (AEMs). Therefore, how to balance the problem of excessive swelling of polymer matrix caused by increasing ion conductivity becomes an important challenge. Herein, 3-(dimethylamino)-1- propylamine (DMAPA) and polyethyleneimine (PEI) were grafted to the surface of layered double hydroxide (LDH) through mussel-inspired chemistry. The sheet-like functionalized LDH (DLDH and PLDH) as both filler and crosslinker was incorporated into the quaternized fluorenyl-containing polyethersulfone (QPFSU) matrix to get a series of new composite anion exchange membranes (AEMs). The as-prepared micro-crosslinked AEMs were found to form more hydrophilic conductive ion clusters owing to the generation of new quaternary ammonium groups during the crosslinking reaction. The micro-crosslinked AEMs have better dimensional stability while having higher OH − conductivity. Especially the ion conductivity of CQPFSU-1%-PLDH membrane can reach 86.8 mS cm −1 at 80 °C with excellent dimensional and chemical stability (SR is 9.6% at 80 °C, 21.8% decrease in OH − conductivity at 60 °C in 1.0 M NaOH for 200 h). Overall, the micro-crosslinking method for functionalized LDH modified AEMs achieves a balance between ion conductivity and dimensional stability of AEMs.
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JOURNAL OF SOLID STATE CHEMISTRY
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2024
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IF 3.2
Xiaoyu Chen,Xiaoshuai Yu,Chuncheng Yang,Guoyong Wang
The oxygen evolution reaction is more challenging than the hydrogen evolution reaction in overall water splitting, not only because the four-electron reaction is more complex but also because the oxidizing environment of the anode reaction is more destructive to the electrode material. Generally, such destruction results in the formation of an oxide film that hinders the transition of electrons and subsequently decelerates the succeeding reaction. This paper proposes a transition layer for self-supporting electrodes (NiFe LDH@NiCoP/NF) in which NiCoP grows between the NF and NiFe LDH. The implementation of NiCoP as a transition layer, showcasing excellent antioxidation capability and conductivity, effectively reduced overpotentials and consequently enhanced the catalytic performance. Benefiting from this transition layer, in a 1.0 M KOH, the NiFe LDH@NiCoP/NF catalyst exhibited outstanding OER and HER performance, requiring only 281 and 102 mV, respectively, to achieve 100 and 10 mA cm −2 , and also exhibited a cell voltage for overall water splitting of 1.56 V at 10 mA cm −2 .
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ACS Applied Materials & Interfaces
·
2019
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IF 8.456
Xiaolong Guo,Xiaolin Hu,Dan Wu,Chuan Jing,Wei Liu,Zongling Ren,Qiannan Zhao,Xiaoping Jiang,Chaohe Xu,Yuxin Zhang,Ning Hu
The rational design of excellent electrocatalysts is significant for triggering the slow kinetics of oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) in rechargeable metal–air batteries. Hereby, we report a bifunctional catalytic material with core–shell structure constructed by Co3O4 nanowire arrays as cores and ultrathin NiFe-layered double hydroxides (NiFe LDHs) as shells (Co3O4@NiFe LDHs). The introduction of Co3O4 nanowires could provide abundant active sites for NiFe LDH nanosheets. Most importantly, the deposition of NiFe LDHs on the surface of Co3O4 can modulate the surface chemical valences of Co, Ni, and Fe species via changing the electron donor and/or electron absorption effects, finally achieving the balance and optimization of ORR and OER properties. By this core–shell design, the maximum ORR current densities of Co3O4@NiFe LDHs increase to 3–7 mA cm–2, almost an order of magnitude increases compared to pure NiFe LDH (0.45 mA cm–2). Significantly, an OER overpotential as low as 226 mV (35 mA cm–2) is achieved in the designed core–shell catalyst, which is comparable to and/or even better than those of commercial Ir/C. Hence, the primary zinc–air battery employing Co3O4@NiFe LDH as an air electrode achieves a high specific capacity (667.5 mA h g–1) and first-class energy density (797.6 W h kg–1); the rechargeable battery can show superior reversibility, excellent stability, and voltage gaps of ∼0.8 V (∼60% of round-trip efficiency) in >1200 continuous cycles. Furthermore, the flexible quasi-solid-state zinc–air battery with bendable ability holds practical potential in portable and wearable electronic devices.
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高影响因子
CHEMOSPHERE
·
2021
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IF 7.086
Jiangfu Zheng,Wenbo Li,Rongdi Tang,Sheng Xiong,Daoxin Gong,Yaocheng Deng,Zhanpeng Zhou,Ling Li,Long Su,Lihua Yang
In this study, an investigation is conducted into the degradation of nitenpyram (NTP) using highly efficient APMMO/PDS/Vis system. As photocatalysts, silver phosphate (AP) and calcined Zn–Al layered double hydroxides (MMO) exhibit high efficiency in achieving charge separation. Besides, the injection of electrons into peroxydisulfate (PDS) from the APMMO can contribute to obtaining the species in the active state with higher efficiency. Based on the APMMO/PDS/Vis system, 50 mg/L of nitenpyram (NTP, 50 mL) can be completely removed in 60 min using 0.8 g/L photocatalyst and 0.2 g/L PDS under the optimum condition and visible light (780 nm > λ > 420 nm). Meanwhile, as demonstrated under visible light within 30 min, an ultrahigh degradation efficiency can be achieved by NTP based on APMMO1/PDS/Vis system. Besides, the electron paramagnetic resonance (EPR) technique and radical quenching experiments suggested 1 O 2 , h + , SO 4 − •, •O 2 − , and •OH are all contributory to the removal of pollutants. Given the outcomes achieved by LC/MS system and mass spectrometry, the primary degradation intermediates of NTP end up being converted into photodegradation products (such as 2-Chloropyridine, 6-Chloropurine Riboside and dl -Leucine). Additionally, there are three potential photodegradation pathways to NTP degradation have been deployed. Moreover, the NTP light degradation occurring in APMMO1/PDS/Vis system is competent under the three types of real water sample. Accordingly, the high-efficiency APMMO1/PDS/Vis system is fit for use in water pollution control for agricultural productions.
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高影响因子
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