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.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Shixiang Xue,Tong Zhou,Pan Wu,Liang Zhao,Yanli Nan,Mingtao Qiao,Wanying Lei
Exploring high-efficient, earth-abundant and stable electrocatalyst for oxygen evolution reaction (OER) is of vital importance for large-scale implementation of energy converting and storing. Thus, we fabricated a free-standing hierarchical heterostructure electrode of Ni 0.85 Se@CoFe LDH/NF via a rational combination of hydrothermal, selenization and electrodeposition process, among which the ultrathin CoFe LDH nanosheets intimately assembled onto the vertical aligned Ni 0.85 Se nanosheets supported on Ni foam. The constructed core-shell nanosheet arrays hold the plentiful hetero-interfaces and intimate interactions through metal-oxygen bonds between two individuals, which guarantee the fast OER kinetic processes. Additionally, CoFe LDH with crystalline/amorphous hybrid structure favors providing more reaction sites. Remarkably, the optimal Ni 0.85 Se@CoFe LDH/NF binary composites possess outstanding OER activity with a low overpotential of ∼223 and 280 mV at 10 mA cm −2 and 100 mA cm −2 in alkaline solution as well as good durability. This research offers an alternative approach for improving electrocatalytic water splitting through constructing 3D hierarchical heterostructures.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Fengzhan Si,Yan Zhang,Yue Liang,Xiaomin Kang,Jianwen Liu,Xian-Zhu Fu,Jing-Li Luo
Water decomposition is the most promising system for developing renewable energy, but the sluggish kinetics of the oxygen evolution reaction (OER) is the key limiting factor. Recently, inorganic nanomaterials have been widely used as an effective catalyst for the stimulation of OER kinetics, for which the subsequent dispersion and the current collector are essential. We present a three-dimensional NiFe-layered double hydroxide (NiFe-LDH) synthesized by electrochemical corrosion , with increased electrochemical performance for electrocatalytic water splitting. Electrochemical measurements reveal that the NiFe-LDH has a lower Tafel slope of 46 mVˑdec −1 compared with the NiFe foam. The resulting electrode had a current density of 50 mAˑcm −2 and a remarkably low overpotential of 150 mV. Theoretical calculations and experimental observations showed and explained NiFe-LDH-90 electrode has high alkaline medium endurance, implying excellent OER electrocatalytic activity . The produced composite is expected to bring new insights into the design of foam electrocatalyst materials for OER.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Jiangfu Zheng,Changzheng Fan,Xiaoming Li,Qi Yang,Dongbo Wang,Abing Duan,Shuaijun Pan,Baowei Zhang,Jinglin Ding,Shengxiang Rong,Haoyu Yin
Development of efficient nanomaterials for photocatalytic degradation is very important in the removal of organic pollutants from water. The oxygen vacancy-rich g-C 3 N 4 / LDH composites (g-C 3 N 4 /LDH-OVs) with a layered structure was prepared for the efficient photocatalysis degradation and mineralization of tetracycline hydrochloride (TC) under visible light irradiation. Oxygen vacancies in the composites achieved through structural induction strategy not only provide abundant active sites but also improve the separation efficiency of the photo-generated carriers, thereby enhancing the degradation and mineralization of TC, as revealed both by theories and experiments. The optimized g-C 3 N 4 /LDH-OVs have achieved excellent photocatalytic activity (i.e., 95 % degradation and 28 % mineralization of TC after 60 min of visible light irradiation), which was 2.3 and 3.5 times higher than that of the pristine g-C 3 N 4 and LDH-OVs, respectively. Furthermore, experimental results based on bio-acute toxicity show that the g-C 3 N 4 /LDH-OVs/Vis system can effectively detoxify the transformation products. This study provides an insight into the development of LDH-based photocatalysts, so as to realize photocatalytic mineralization and simultaneous detoxification through the new strategy of oxygen vacancy defect engineering.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2022
·
IF 4.598
Huanling He,Shiwen Lv,Ying Kang,Jiaxin Yi,Yi Zhang,Yanqing Cong
Herein, for the first time, a self-supported electrode for simultaneous determination of hydroquinone (HQ) and catechol (CA) was synthesized by loading NiCoFe-layered double hydroxide nanoflowers on hydrophilic carbon cloth (NiCoFe-LDH NFs/CC) with a simple hydrothermal method. By combining the advantages of NiCoFe-LDH NFs with hydrophilic carbon cloth such as good conductivity, 3D porous network structure, high electrocatalytic activity, and fast electron transport, the proposed NiCoFe-LDH NFs/CC electrode dispalyed good electrochemical activity for detecting HQ and CA. The binder-free and free-standing electrode based on NiCoFe-LDH NFs/CC possessed good linear range (5–200 μM), low determination limit (0.15 μM and 0.11 μM), and strong selectivity. Furthermore, it also showed good electrochemical stability without obvious change in ten days. More importantly, as-prepared electrode could be used as an efficient electrochemical sensor to determine HQ and CA content in actual samples with good recovery rate, revealing its feasibility in potential application.
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Journal of Materials Chemistry C
·
2022
·Vol. 10
·期 27
·9989-10000
·
IF 8.067
Yixuan Guo,Damien Boyer,Federico Cisnetti,Anthony Barros,François Reveret,Yongjun Feng,Geneviève Chadeyron,Fabrice Leroux
Perylene diimide-based dyes substituted by four sulfonate groups at their bay position are known to be extremely sensitive to their mutual π–π intermolecular interaction. They do not emit fluorescence in solid state. When co-hosted in LDH with a surfactant in extremely small quantities, an absolute photoluminescence quantum yield (PL QYabs) of about 35% is reached upon blue excitation at 465 nm for a dye content as low as 0.1% of the total interleaved anions and yet revealing the presence of excimers. When this material is dispersed in silicone, the emission spectrum exhibits a blue shift compared to the hybrid assembly. A saturated red color with PL QYabs as high as 50% is obtained. When this red-emitting film is combined with a YAG/Ce silicone film and a blue LED chip emitting at 465 nm, warm white light (T = 3366 K) with a high color rendering index of 91.4 is produced. Finally, the phosphors hosted in LDH are photo-stable even when dispersed in a silicone matrix, with emission properties that do not suffer any decrease in intensity under combined thermal and photonic stresses, thus opening up real possibilities for applications in LED technology.
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JOURNAL OF POLYMER RESEARCH
·
2022
·Vol. 29
·期 3
·1-13
·
IF 3.061
Li Lingtong,Chen Shaopeng,Guo Xincheng,Qin Jun,Chen Xiaolang,Lu Zongcheng,Wu Hong
In a purpose to develop good dispersity and compatibility of layered double hydroxide (LDH) in polypropylene (PP) matrix, a novel DOPOi-LDH@GO hybrid nanomaterial was fabricated via three-step reactions including the synthesis of DOPO-itaconic acid (DOPOi), an electrostatic adsorption of LDH coating on the surfaces of graphene oxide (GO) (LDH@GO), and the preparation of DOPOi-LDH@GO by an anion exchange. The thermal stability and crystallization behaviors of PP/DOPOi-LDH@GO nanocomposites are greatly different from neat PP. The thermal stability of PP/DOPOi-LDH@GO nanocomposites are lower than that of neat PP. The addition of nanoparticles provides a non-homogeneous nucleus for PP crystals, producing a heterogeneous nucleation mechanism that increases the spherulite density and decreases the spherulite size. The DOPOi-LDH@GO hinders the crystallization of PP and crushes spherulite integrity. The combination of LDH with GO for agglomeration-tolerant and LDH-modified at the interlamination and surface provides a potential way to improve the efficient dispersion and enhanced interfacial adhesion in the PP matrix. Thus, PP/DOPOi-LDH@GO nanocomposites exhibit a wide range of application potentials.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2021
·
IF 5.316
Yinke Wang,Lujun Wang,Zixin Xiao,Shichao Liu,Jun Hu,Xinqi Long,Lixu Wu,Chun Sun,Kangbo Chen,Feipeng Jiao
A novel (BiO) 2 CO 3 /ZnFe-LDH photocatalyst was fabricated via a simple hydrothermal method for degradation of tetracycline aqueous solution. Due to the unique band structures of (BiO) 2 CO 3 and ZnFe-LDH, the combination of these two materials formed a Z-scheme heterojunction, which was conducive to the separation of photo-generated carriers. Through measuring the absorbance, it was found that the composite with 5% ZnFe-LDH has the optimal photocatalytic performance among all the samples. 98.09% of tetracycline (TC) was degraded after adsorption for 30 min and light irradiation for 90 min. In addition, the (BiO) 2 CO 3 /ZnFe-LDH composite displayed a remarkable reusability and stability in five successive runs. Based on the results of characterization and performance, a possible photocatalytic mechanism was proposed. This work would be helpful for the application of composites in the field of photocatalysis .
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Inorganic Chemistry Frontiers
·
2021
·Vol. 9
·期 1
·146-154
·
IF 6.569
Hanzhi Yu,Yaoyi Xie,Liming Deng,Hongjiao Huang,Junnan Song,Deshuang Yu,Linlin Li,Shengjie Peng
Developing hierarchical heterostructures as bifunctional electrocatalysts which promote renewable hydrogen production is a desirable but challenging technology in electrochemical water splitting. Herein, the interface engineering of the FeNi2Se4-FeNi LDH composite is achieved by the in situ growth of FeNi LDH nanosheets and the subsequent partial selenization treatment. Enhanced mass transfer and accelerated gas release are achieved in such a unique self-supported hierarchical heterostructure during overall water splitting. Moreover, the strong electronic interaction between FeNi2Se4 and FeNi LDH optimizes the electron redistribution of Fe and Ni sites, which significantly improves the interfacial reactivity of reactants and/or intermediates with the hybrid catalyst. Benefiting from increased active sites and enhanced intrinsic activity, the hybrid electrocatalyst requires only a potential of 205 mV for the oxygen evolution reaction (OER) and a potential of 106 mV for the hydrogen evolution reaction (HER) to realize 10 mA cm−2. Specifically, the optimized FeNi2Se4-FeNi LDH as a bifunctional electrode in overall water splitting delivers 10 mA cm−2 at a low cell voltage of 1.56 V driven by a solar cell. This strategy by rational design of heterostructures thus paves an efficient pathway to fabricate active and non-precious bifunctional electrocatalysts for overall water splitting.
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ADVANCED FUNCTIONAL MATERIALS
·
2023
·
IF 19
Ben Wu,Guofang Zhang,Jiawen Ji,Rong-Hua Luo,Junkang Chen,Feng-Liang Liu,Emerson Coy,Sergio E. Moya,Qi Li,Xiaoman Suo,Xinyue Chen,Yong-Tang Zheng,Yang Li,Guocheng Wang
In this study, a novel strategy is developed for the first time, referred to as high-concentration cobalt ion-assisted hydration (HCCAH) utilizing zeolitic imidazolate framework-67 (ZIF-67) as a precursor, to produce independent and flat α-cobalt hydroxide nanosheets (CHN). These nanosheets offer abundant contact sites for binding with virus surface proteins. The formation of CHN involves the in situ transformation from ZIF-67, due to the matching of the hydrolysis rate of ZIF-67 and in situ growth rate of cobalt hydroxide orchestrated by high concentration of cobalt ions. Notably, the CHN contains a higher proportion of trivalent cobalt, which is shown to enhance the binding with the Severe Acute Respiratory Syndrome Coronavirus 2 (SARS-CoV-2) Spike protein and induce protein structural denaturation, as demonstrated by molecular dynamics (MD) simulation. Antiviral experiments using pseudovirus and authentic viruses have confirmed the promising antiviral performance of CHN. Furthermore, both in vitro and in vivo experiments have demonstrated the excellent biocompatibility of CHN. This research opens up new possibilities for the application of cobalt hydroxide nanosheets and serves as a valuable reference for the design of antiviral nanomaterials.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Xiaolin Ma,Linxiang Zhou,Ting Chen,Panpan Sun,Xiaowei Lv,Haizhou Yu,Xiaohua Sun,T. Leo Liu
Seeking cathode materials with high areal capacity and excellent cycling tolerance is a key step to develop aqueous rechargeable zinc-based alkaline batteries with high energy density, power density and excellent stability. Here, the bilayered cathode composite (MCN-LDH@CP) of molybdate intercalated cobalt–nickel layered hydroxide nanosheets (MCN-LDH) grown on cobalt phosphate octahydrate microsheet (CP) was prepared by a two-step hydrothermal process. Molybdate intercalation significantly reduces the thickness of cobalt–nickel layered hydroxide, greatly increases its specific surface area, regulates its pore distribution, increases the crystal plane spacing, promotes the diffusion rate of hydroxide in it, and increases its specific capacity. Meanwhile, the bilayered MCN-LDH@CP electrode significantly improved the areal energy density (2.89 mWh/cm 2 ) and peak power density (111.22 mW/cm 2 ) and cycle stability (97.8 % after 7000 cycles) of the CoNi//Zn battery. The excellent stability is mainly due to the fact that the MCN-LDH overlay inhibits the loss of P element of CP and improves the structural stability of the sample. The quasi-solid-state MCN-LDH@CP//Zn battery can still charge a mobile phone even when hammered and pierced, showing excellent safety and reliability. This work opens a new avenue to develop CoNi//Zn batteries with high energy density, power density and excellent tolerance.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Tiantian Liu,Xiaomei Yu,Shuang Yu,Huijing Yang,Qimeng Sun,Chengduo Wang,Songjie Li,Jin You Zheng
Alkaline water electrolysis techniques have enormous potential for industrial-scale hydrogen generation, but a lack of effective and low-cost bifunctional electrocatalysts capable of steady high-current density operation has hampered progress. Layered double hydroxides (LDHs) have been considered promising OER electrocatalysts, but their poor electrical conductivity impedes hydrogen evolution reaction (HER) activity. Integrating LDHs with transition metal phosphides (TMPs) can potentially achieve bifunctional capability by overcoming individual limitations. Herein, CoP@NiFe LDH/Ni heterostructured catalyst was rapidly synthesized by a scalable two-step electrodeposition method. The integration of NiFe LDH with CoP enhanced its electrical conductivity. Meanwhile, electron transfer occurred from the metal atoms to the more electronegative phosphorus, facilitating phosphorus to act as a proton acceptor and expedite the HER process. Benefiting from the synergistic integration and optimized electronic structure, CoP@NiFe LDH/Ni exhibited excellent alkaline water-splitting performances with low overpotentials of 260 mV for HER and 351 mV for OER at 400 mA/cm 2 . The CoP@NiFe LDH/Ni two-electrode-based alkaline electrolyzer displayed a cell voltage of 2.13 V and stable operation for 100 h at a high current density of 1000 mA/cm 2 . This work elucidates a strategy to tackle critical challenges impeding the design and preparation of high-current-density tolerant bifunctional electrocatalysts.
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