ACS Catalysis
·
2023
·
IF 12.9
Mei Li,Zhenyang Zuo,Shengbo Zhang
Developing effective photocatalysts for CO2 reduction to high value-added chemicals or fuels is a promising strategy for alleviating serious environmental problems and energy crisis. Currently, the photocatalytic efficiency is still too slow to arouse industrial interest for most semiconductor photocatalysts due to their low CO2 uptake, limited visible light capture capacity, and serious recombination of electron–hole. Herein, we successfully synthesized a high-density ultrafine Au cluster (∼0.7 nm)-doped cobalt-layered double hydroxide nanocage (Au/Co-LDH) photocatalyst through an in situ redox strategy to explore the structure–activity relationship in the CO2 reduction system. A series of experimental characterizations showed that CO2 adsorption, visible light capture capacity, and charge transfer rate are significantly enhanced due to the highly dispersed and ultrafine Au cluster doping. Density functional theory calculations indicate that Au doping also promoted charge redistribution at the active site, increased the density of states near the Fermi energy level, stabilized the *COOH intermediate, and reduced the energy barrier of the rate-determining step. As a result, Au/Co-LDH delivers a CO evolution rate of 5610 μmol g–1 h–1 toward CO2 reduction under visible light (λ > 420 nm), which is 4 times and 22 times more active than the undoped one and Au nanoparticles, respectively. We believe that this work will provide an important implication for the development and optimization of photocatalysts for CO2 reduction.
研究领域:
材料科学
·
环境科学
·
化学工程
·
纳米技术
·
催化
✓ 已验证
DOI
高影响因子
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.
研究领域:
环境科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
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.
研究领域:
环境科学
·
化学工程
·
水处理技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ELECTROCHIMICA ACTA
·
2022
·
IF 7.336
Qifeng Lin,Zeyu Yuan,Dongyi Wang,Wei Wei,Xibin Wang,Wei Han,Lili Wang
The growing problem of limited lithium resource reserves has resulted in increased attention and a corresponding surge in sodium-ion battery (SIB) research. However, SIBs have disadvantages, such as a short cycle life and low energy density. The lack of high capacity and long-cycle stability anode materials are important factors hindering the development of SIBs. In this study, hollow carbon nanospheres were nitrogen-doped, and the zeolitic imidazolate framework-67 was used as a precursor to synthesize cobalt-based layered double hydroxide using the hydrothermal method followed by synthesizing an NHCNS@CoSe 2 @C complex using calcination and carbon coating. In this design concept, the hollow-cavity structure of the carbon nanospheres provided shorter electron diffusion paths and increased stability; the introduction of nitrogen increased the number of defect sites and charge density of the porous carbon materials, which, with the transition metal selenide, enhanced the conductivity of the final product. The resulting carbon-supported anode material, NHCNS@CoSe 2 @C, had an initial stable discharge capacity of 465.6 mAh g − 1 at a current density of 0.1 A g − 1 and maintained a high capacity of 373.8 mAh g − 1 after 100 cycles. Moreover, it exhibited a high rate performance of 285.6 mAh g − 1 at a current density of 5 A g − 1 .
研究领域:
材料科学
·
能源存储技术
✓ 已验证
产品关联
DOI
高影响因子
Journal of Energy Storage
·
2024
·
IF 8.9
P.S. Dighe,R.S. Redekar,N.L. Tarwal,P.B. Sarawade
Because of the high energy demand, hybrid supercapacitors (HSC) are one of the best options in energy storage systems. The energy demand can be fulfilled by achieving superior energy density . Recently, layered double hydroxides (LDHs) have been favoured as magnificent supercapacitive electrode materials due to their capability of storing high energy density using their tuneable layered structure. In this study, we have synthesized nickel‑cobalt layered double hydroxide on nickel foam (Ni-Co LDH/NF) by utilizing a low-cost hydrothermal technique to obtain high energy density. To monitor the effect of the morphological aspects on electrochemical performance, reaction time during synthesis was varied. The structural and compositional studies confirmed Ni-Co LDH deposition on the Ni-foam. The morphological analysis showed highly interconnected nanosheets which efficiently provided fast transport pathways for electrons and electrolyte ions. The Ni-Co LDH/NF film synthesized at 6 h delivered a distinguished rate capability with a specific capacitance of 1577 F/g at 1 mA/cm 2 . Notably, a fabricated aqueous asymmetric supercapacitor showed a good energy density of 38 Wh/kg. These results highlighted the remarkable advantages of the binder-less nanosheet structure of the Ni-Co LDH for potential use in the supercapacitor application.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
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.
研究领域:
材料科学
·
化学工程
·
火灾安全科学
✓ 已验证
产品关联
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2026
·
IF 5.4
Jiahuan Wang,Zuozhu Yin,Xiangyu Han,Yongcun Ma,Zhen Hong,Chan Xie,Zhiyang Jiang,Mingshan Xue
A superhydrophobic conductive fabric is fabricated via scalable spray-coating of Zn-Co LDH/MWCNTs/POTS. • The fabric achieves > 96% oil-water separation efficiency with excellent cyclic stability. • Integrated electrocatalytic function degrades organic pollutants within 2 h under low voltage. • Robust durability under abrasion, chemical, thermal, and vibration stresses is demonstrated. • COMSOL simulations reveal the wettability–pore synergy governing enhanced separation. The ingress of moisture into aircraft engine lubrication systems poses a serious threat to flight safety and component service life; consequently, there is an urgent need to develop novel multifunctional materials capable of oil-water separation and environmental remediation. In this study, a three-dimensional superhydrophobic conductive fabric with a structure resembling peacock feathers was fabricated for oil-water separation in the aerospace sector. The material was prepared by spraying a composite of zinc-cobalt layered double hydroxide (LDH), modified with perfluorooctyl triethoxysilane (POTS) and multi-walled carbon nanotubes (MWCNTs), onto a conductive fabric substrate. It exhibits superhydrophobicity (water contact angle as high as 161.2°), electrocatalytic degradation capability and oil-water separation capability. The conductive network of multi-walled carbon nanotubes enables electrocatalytic degradation at a low voltage of 20 V, whilst the superhydrophobic surface selectively allows rapid oil penetration, achieving oil-water separation efficiencies of 96–99.4% under thermal radiation conditions. The material maintains stable superhydrophobicity even after repeated cycles and exposure to mechanical abrasion, corrosive media and high-temperature ageing (220°C). COMSOL simulations elucidated the synergistic mechanism between selective wetting and thermal viscosity modulation. This study provides an integrated solution for next-generation aviation fuel systems that combines physical separation with electrocatalytic purification. Furthermore, the coating preparation process is simple and the raw materials readily available, offering significant potential for large-scale mass production. Download: Download high-res image (178KB) Download: Download full-size image A superhydrophobic conductive fabric (HCF) modified with Zn-Co LDH/MWCNTs composite was fabricated. Through micro-nano structure regulation and surface energy modification, it synergistically achieves efficient oil-water separation, low-voltage electrocatalytic degradation, and self-cleaning properties. Exhibiting excellent mechanical stability and chemical durability under harsh operating conditions of aero-engines, this material provides a multifunctional integrated solution for water pollution control and contaminant purification in aviation fuel systems.
✓ 已验证
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2021
·
IF 4.539
Xiangying Yin,Xiaoyu Ma,Yi He,Hongjie Li,Yi Fan,Teng He,Xiao Guo,Li Chen
In the face of frequent oil spills and dye emissions, membrane technology is an efficient method to treat wastewater. However, selectivity , membrane fouling and high operating pressure are tricky problems for practical membrane applications. Hence, it is desirable to design a novel membrane with high selectivity, high flux and superior antifouling properties for gravity-driven separation of complex oily wastewater. In this study, bioinspired by sea urchins with good self-cleaning properties, an urchin-like Ni/Co layered double hydroxide (LDH) surface was grown onto stainless steel mesh (SSM) via a facile hydrothermal method . Due to the unique hierarchical architecture and surface chemistry, Ni/Co@SSM displays a robust self-cleaning oil-repellent ability without hydration. Combining the unique superwettability and highly porous nanostructure , Ni/Co@SSM could be used to separate various oil/water mixtures and emulsions efficiently under only gravity-driven conditions. In addition, Ni/Co@SSM exhibits great catalytic degradation ability of dye solutions in a short time. Notably, Ni/Co@SSM displays excellent physical, chemical and thermal stability in acidic, alkaline and saline environments. Consequently, Ni/Co@SSM possesses broad application prospects with superior self-cleaning and outstanding catalytic degradation ability of aromatic dyes. It shows promising application value in practical complex oily wastewater treatment without complicated operations and chemicals.
研究领域:
材料科学
·
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Weibin Chen,Changshui Wang,Shibiao Su,Hai Wang,Dandan Cai
The quest for desirable two-dimensional (2D) materials and facile strategies to construct 2D layered composites with fascinating structures and compositions for high-performance electrocatalysis is still a major challenge. In the present research, novel nanocomposites of 2D zeolitic imidazolate framework-9 (ZIF-9) combined with Co-layered double hydroxide (Co LDH) were successfully synthetized through a controllable phase transition from ZIF-9(I). The 3D to 2D structural transformation of ZIF-9 was induced by deionized water, and the formation of 2D Co LDH was simultaneously realized during the one-step fabrication of ZIF-9(III)/Co LDH nanocomposites. Due to the high surface area, the presence of abundant metal sites, and the interactions between 2D ZIF-9(III) and 2D Co LDH, the as-optimized ZIF-9(III)/Co LDH nanocomposite exhibits great electrochemical activities for oxygen evolution reaction (OER) (η = 297 mV at 10 mA cm −2 ) in 1.0 M KOH solution. The electrochemical performance of the ZIF-9(III)/Co LDH nanocomposite was superior to those of the pure Co LDH, ZIF-9(III), and commercial RuO 2 . The present work demonstrates that the proposed strategy can effectively boost catalytic activities and also design new routes to synthesize advanced MOF nanohybrids for various applications.
研究领域:
材料科学
·
电化学
·
纳米技术
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Mengqing Hu,Di Zhao,Xinlong Yan,Yun Wang,Jin Zhang,Xiaoyan Hu,Ming Zhou,Porun Liu
Designing advanced bimetallic catalysts is essential to improving peroxymonosulfate (PMS) activation. Herein, a novel magnetic nickel/cobalt-layered double hydroxide decorated nitrogen-doped carbon (Ni/Co LDH@NC) catalyst we synthesized using carbonized ZIF-67 as a template for simultaneous removal of sulfamethoxazole (SMX) and Pb(Ⅱ) by PMS activation. The synthesized Ni/Co LDH@NC achieved complete degradation of SMX within 20 min and adsorbed Pb(Ⅱ) at 90.3 mg g −1 in 2 h. Notably, in simulated mixed wastewater, Ni/Co LDH@NC removed 100 % of SMX and simultaneously absorbed 84 % of Pb(Ⅱ) within 60 min. Density functional theory (DFT) studies revealed that synergistic Ni-Co sites and “bridging oxygen” vacancies enhanced electron transfer to PMS, facilitating O-O bond cleavage. The catalyst maintained high performance after four cycles, with over 85 % SMX degradation and 80 % Pb(Ⅱ) removal. This study highlights the potential of MOF-derived catalysts for efficient, simultaneous remediation of antibiotic and heavy metal pollutants, contributing to advanced wastewater treatment.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）