JOURNAL OF MATERIALS SCIENCE
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2021
·Vol. 56
·期 9
·5717-5729
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IF 4.22
Lu Lili,Ma Yongjin,Dong Rui,Tan Pengfei,Chen Yi,Pan Jun
A series of Zn x Cd 1−x S solid solutions were synthesized through a simple one-step chemical bath co-precipitation route. The microstructure, morphology, composition and optical properties had been thoroughly investigated. The results showed that the as-obtained Zn x Cd 1−x S samples exhibited monodisperse spherical feature. These monodisperse Zn x Cd 1−x S spheres were composed of a large number of 5–10 nm crystal grains. The chemical composition of the Zn x Cd 1−x S solid solutions can be controlled by adjusting the ratio of Zn source to Cd source and the dosage of ammonia solution. Meanwhile, the energy band structure and photocatalytic properties can be optimized. The photocatalysis experiment results revealed that the as-synthesized Zn 0.30 Cd 0.70 S sample exhibited optimum water splitting performance. The satisfactory hydrogen evolution rate (HER) of Zn 0.30 Cd 0.70 S reached 27.004 mmol g −1 h −1 even without any cocatalysts, which was more than 48 times that of pure CdS (0.561 mmol g −1 h −1 ). This enhancing effect can owe to the balance between light absorption capacity and redox potential caused by the incorporation of Zn in the Zn x Cd 1−x S solid solutions.
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Nature Communications
·
2020
·Vol. 11
·期 1
·1-12
·
IF 12.121
Zhai Panlong,Zhang Yanxue,Wu Yunzhen,Gao Junfeng,Zhang Bo,Cao Shuyan,Zhang Yanting,Li Zhuwei,Sun Licheng,Hou Jungang
Rational design of the catalysts is impressive for sustainable energy conversion. However, there is a grand challenge to engineer active sites at the interface. Herein, hierarchical transition bimetal oxides/sulfides heterostructure arrays interacting two-dimensional MoO x /MoS 2 nanosheets attached to one-dimensional NiO x /Ni 3 S 2 nanorods were fabricated by oxidation/hydrogenation-induced surface reconfiguration strategy. The NiMoO x /NiMoS heterostructure array exhibits the overpotentials of 38 mV for hydrogen evolution and 186 mV for oxygen evolution at 10 mA cm −2 , even surviving at a large current density of 500 mA cm −2 with long-term stability. Due to optimized adsorption energies and accelerated water splitting kinetics by theory calculations, the assembled two-electrode cell delivers the industrially relevant current densities of 500 and 1000 mA cm −2 at record low cell voltages of 1.60 and 1.66 V with excellent durability. This research provides a promising avenue to enhance the electrocatalytic performance of the catalysts by engineering interfacial active sites toward large-scale water splitting.
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ANALYTICAL CHEMISTRY
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2020
·
IF 6.785
Meng Ding,Limin Yang,Jiahui Zeng,Xiaowen Yan,Qiuquan Wang
We report an approach that polymerizable handle-modified nanosized metal organic frameworks (MOFs) are used as independent monomers to be covalently organized by crosslinking molecules (CLMs) into an orderly MOF-assembled hybrid monolithic stationary phase, overcoming the respective problems of previously reported MOF-mixed or embedded stationary phases so far. It has a hierarchical micro-, meso-, and macropore structure throughout the monolithic matrix that is donated from MOF themselves, formed via CLM crosslinking in-between MOFs and expended by porogenic solvents, and a tunable surface chemistry derived inherently from MOFs, regulated by CLMs and initiated by the mobile phases as well. Such a pore structure and surface chemistry display multiplex interactions of sieving and electrostatic repulsion in addition to the polarity-based interactions that synergistically govern the partitioning way and degree of target molecules between the stationary and mobile phases, thus offering the ability to simultaneously separate small and large molecules during one chromatographic run on a nano-flow capillary high-performance liquid chromatography platform. A baseline mutual separation with the HETP and Rs of, for example, 9.2 μm butylbenzene and 4.56 (butylbenzene and pentylbenzene), 7.9 μm (phenylalanine) and 3.50 (tryptophan and phenylalanine), and 7.0 μm (myoglobin) and 1.91 (bovine serum albumin and myoglobin) was achieved when UiO-66/NH-methacrylate was exemplified as a model of MOFs and 1,6-hexanediol dimethacrylate and stearyl methacrylate together as CLMs. Not limited to the MOFs and CLMs demonstrated here, other available MOFs and CLMs or newly designed and synthesized ones are expected to be used for constructing one’s own desired monolithic stationary phases toward her/his particular purposes.
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ANALYTICA CHIMICA ACTA
·
2020
·
IF 5.977
Yulan Gao,Miaomiao Tian,Yaxue Jia,Xiaohong Wang,Li Yang
The combination therapy based on artemisinin is the most effective method to treat malaria. Sensitive, rapid and accurate detection of artemisinin is very important to monitor clinical pharmaceutical effect as well as the drug quality control. In this work, catalytic performance of polyoxometalates (POMs), vanadomolybdophosphoric heteropoly acid ( H 5 PMo 10 V 2 O 40 , PMoV 2 ) and tungstophosphoric heteropoly acid ( Na 5 PW 11 O 39 Cu, PW 11 Cu) , are investigated. It is indicated that the POMs exhibit peroxidase-like activity, which efficiently catalyze the artemisinin/thiamine reaction to produce fluorescent product thiochrome. With the usage of the POMs as the catalyst in combination with fluorescent probes , we propose a method for highly sensitive and rapid determination of artemisinin. When PMoV 2 and PW 11 Cu are used as catalysts, the linear ranges are 1.0 × 10 −6 -1.0 × 10 −1 mM and 5.0 × 10 −6 -9.0 × 10 −1 mM, and the detection limits are as low as 0.5 nM and 1 nM, respectively. The method is successfully applied to determine artemisinin in human plasma and Artemisia annua . L leaves with good accuracy.
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Polymers
·
2020
·Vol. 12
·期 9
·2134
·
IF 3.426
Li Zeng,Liping Zhang,Xingang Liu,Chuhong Zhang
Sodium-ion batteries (SIBs), as a supplement of lithium-ion batteries (LIBs), are attracting intensive research interest due to their low cost and abundance. Molybdenum disulfide (MoS2) is regarded as a suitable candidates for SIBs electrode materials, which suffer from prominent volume expansion and poor conductivity. In this study, three-dimensional porous graphene composites loaded with MoS2were prepared via a facile two-step method. The MoS2nanoflower particles were uniformly dispersed within the layered graphene matrix, and a three-dimensional porous graphene supported MoS2nanoflower battery (MoS2/3DG) was demonstrated to have superior performance to that of the pristine pure MoS2nanoflower battery. At a current density of 100 mA/g, the MoS2/3DG delivered a reversible capacity of 420 mAh/g. What is more, it yielded a reversible specific capacity of 310 mAh/g at 2 A/g, showing an excellent rate of 73.8%. The excellent performance of the novel MoS2/3DG composite are attributed to the promoted infiltration of electrolytes and the hindered volume expansion for the porous structure, good conductivity, and robust mechanical properties of graphene.Keywords:MoS2nanoflower;three-dimensional porous graphene;sodium-ion batteries;solvothermal
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2020
·
IF 3.99
Yanyun Zhu,Luting Yan,Mingyuan Xu,Yuting Li,Xiaodong Song,Lan Yin
Nitrogen-doped graphene quantum dots (N-GQDs) with prime fluorescence properties were synthesized through a simple one-pot hydrothermal method by using citric acid as carbon source and ammonia (A-GQDs) or urea (U-GQDs) as nitrogen source. Both A-GQDs and U-GQDs exhibited a graphene-like structure, but their average particle size is about ten times different. A-GQDs exhibited an evident excitation-dependent photoluminescence (PL) behavior. By contrast, the emission of U-GQDs can be divided into two regions with the development of excitation wavelength: a wavelength-independent emission peak at approximately 540 nm (green) with the excitation wavelength from 400 nm to 500 nm and an excitation-dependent emission peak with the excitation wavelength below 400 nm. Ammonia was introduced into citric acid polycondensator in the form of five membered ring and urea in the form of seven membered ring, respectively, which further affected the subsequent crystallization and surface functionalization. At this time, the structural instability of the nitrogen-containing doped ring itself, coupled with the progress of carbonization, mostly forms a stable nitrogen-containing ring structure, which is likely to be pyrrolic nitrogen or graphitized nitrogen. Therefore, the differences in particle size and nitrogen-containing doped rings partially between A-GQDs and U-GQDs lead to the differences in optical properties. Finally, U-GQDs with high quantum yield (QY) of 54 % were obtained at the molar ratio of 9:10 (citric acid/urea) by optimizing the reaction conditions.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2020
·
IF 7.489
Junnan Tao,Xiaohui Yu,Qinqin Liu,Guiwu Liu,Hua Tang
The requisite interfacial contact of heterojunction photocatalysts has a significant contribution in separation of interfacial charge carriers for photocatalytic hydrogen (H 2 ) evolution in a more efficient manner. Herein, an internal electric field (IEF)-induced S–scheme system comprised of two-dimensional (2D) CoAl layered double hydroxide (LDH) and 2D molybdenum disulfide (MoS 2 ) was constructed via a simple hydrothermal process. In the presence of visible-light irradiation, the 2D/2D MoS 2 /CoAl LDH hybrid demonstrates eightfold greater photocatalytic H 2 generation rate as compared with that of CoAl LDH. The mechanism was investigated in the light of the results of the X-ray photoelectron spectroscopy (XPS) and work-function calculated by density functional theory (DFT) simulation, and the improved activity was ascribed to that the rapid detachment of the electron-hole (e − -h + ) combinations and high redox ability, both are simultaneously realized in MoS 2 /CoAl LDH hybrid with a 2D/2D S–scheme charge transfer mechanism induced by the IEF across interface of the MoS 2 and CoAl LDH. Furthermore, favorable 2D/2D structure and better H* adsorption behavior of MoS 2 /CoAl LDH also promoted the improvement of water reduction performance. This work is a valuable guideline in developing of IEF-induced S–scheme photocatalysts with 2D/2D architecture for improved photocatalytic performance.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2020
·
IF 7.489
Fanying Meng,Yingying Qin,Jian Lu,Xinyu Lin,Minjia Meng,Gang Sun,Yongsheng Yan
In the practical process of photocatalytic H 2 evolution, optimizing the ability of light absorption and charge spatial separation is the top priority for improving the photocatalytic performance. In this study, we elaborately engineer neoteric g-C 3 N 4 nanotube@polydopamine(pDA)/NiCo-LDH (LPC) composite photocatalyst by combining hydrothermal and calcination method. In the LPC composite system, the one-dimensional (1D) g-C 3 N 4 nanotubes with larger specific surface area can afford more active sites and conduce to shorten the charge migration distance, as well as the high-speed mass transfer in the nanotube can accelerate the reaction course. The g-C 3 N 4 /NiCo-LDH type-II heterojunction can efficaciously stimulate the spatial separation of photo-produced charge. In addition, pDA as heterojunction metal-free interface mediums can provide multiple action (π-π* electron delocalization effect, adhesive action and photosensitization). The optimized LPC nanocomposite displays about 3.3-fold high photoactivity for H 2 evolution compared with the g-C 3 N 4 nanotube under solar light irradiation. In addition, the cycle experiment result shows that the LPC composite photocatalyst possesses superior stability and recyclability. The resultant g-C 3 N 4 @pDA/NiCo-LDH composite photocatalyst displays the potential practical application in the field of energy conversion.
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Nanoscale
·
2020
·Vol. 12
·期 43
·22330-22339
·
IF 6.895
Pengfei Liu,Yuanyuan Liu,Jing Li,Meiri Wang,Hongtao Cui
The microstructure of electrode materials and its synergism with current collectors have been a research focus in the area of Faraday supercapacitors (FSs), while the microstructure of current collectors has been neglected in most cases. To eliminate the electrochemical bottleneck of FSs, the comprehensive consideration on electrodes should simultaneously include both the microstructures of materials and current collectors, and their synergism. In this work, a dual nanostructure of NiCo2S4/nickel foam is built to achieve an electrode with structure-synergistical contribution from materials and current collectors. The as-built electrode presents an ultra-high rate capacity (1223.8 C g−1 at 2.5 A g−1; 53.40% capacity retention at an ultra-high current density of 148.5 A g−1) and excellent cycling stability (94.56% capacity retention after 10 000 charge–discharge cycles). The as-assembled asymmetrical supercapacitors show both high energy and power densities (76.7 W h kg−1 at 425.7 W kg−1; 41.9 W h kg−1 at 10 643.3 W kg−1). These results demonstrate that the dual nanostructure of the electrode is valuable for achieving high performance supercapacitors.
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CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Feng Wei,Xinyu Cui,Zhao Wang,Changchang Dong,Jiadong Li,Xiaojun Han
Antibacterial agents with enzyme-like properties and bacteria-binding ability have provided an alternative method to efficiently disinfect drug-resistance microorganism. Herein, a Fe 3 O 4 @MoS 2 -Ag nanozyme with defect-rich rough surface was constructed by a simple hydrothermal method and in-situ photodeposition of Ag nanoparticles. The nanozyme exhibited good antibacterial performance against E. coli (~69.4%) by the generated ROS and released Ag + , while the nanozyme could further achieve an excellent synergistic disinfection (~100%) by combining with the near-infrared photothermal property of Fe 3 O 4 @MoS 2 -Ag. The antibacterial mechanism study showed that the antibacterial process was determined by the collaborative work of peroxidase-like activity, photothermal effect and leakage of Ag + . The defect-rich rough surface of MoS 2 layers facilitated the capture of bacteria, which enhanced the accurate and rapid attack of OH and Ag + to the membrane of E. coli with the assistance of local hyperthermia. This method showed broad-spectrum antibacterial performance against Gram-negative bacteria, Gram-positive bacteria, drug-resistant bacteria and fungal bacteria. Meanwhile, the magnetism of Fe 3 O 4 was used to recycle the nanozyme. This work showed great potential of engineered nanozymes for efficient disinfection treatment.
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CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Jiali Tang,Jiling Zhao,Shixing Wang,Libo Zhang,Minghu Zhao,Zhen Huang,Yuting Hu
In this study, a novel metal organic framework (MOF) was prepared by pre-modification strategy and used as adsorbents to recover palladium ions in wastewater. The characterization indicates that the adsorbents have been successfully synthesized. The effects of various factors on the adsorption behavior of the adsorbents for Pd(II) was studied. Experimental research shows that the optimal pH of the adsorption process is 4.0. The adsorption kinetics and isotherms of Pd(II) on the adsorbents show that it conforms to pseudo-second-order and Langmuir models, respectively. Therefore, the adsorption reaction is a single layer adsorption on the uniform surface of the adsorbent, and chemical adsorption is the main rate-limiting step. According to thermodynamic analysis, the adsorption process is entropiezunahme, spontaneous and endothermic. The adsorption mechanism of Pd(II) on the adsorbents is mainly through the electrostatic action and chelation of Pd(II) with N and O atoms, and the reduction of Pd(II) to Pd(0) by N and O functional groups. The adsorbents can selectively uptake palladium ions from multi-ion wastewater, and after five adsorption–desorption cycles, the adsorption efficiency is still high. This new adsorbent has a wide application prospect in the field of palladium ion separation.
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RSC Advances
·
2020
·Vol. 10
·期 54
·32652-32661
·
IF 3.119
Yu Gao,Kun Qian,Baotong Xu,Fu Ding,Valerian Dragutan,Ileana Dragutan,Yaguang Sun,Zhenhe Xu
The generation of hydrogen-based energy and environmental remediation using sunlight is an emerging topic of great significance for meeting the ever-growing global need. However, the actual photocatalytic performance is still far below expectations because of the relatively slack charge-carrier separation and migration as well as insufficient spectral absorption in semiconductors. Therefore, the rational construction of heterojunctions is considered as an effective approach to solving the above issues. In this context, we have, for the first time, designed and synthesized a two-dimensional 2D-on-2D heterostructure, based on 2D Ag-doped ZnIn2S4 nanoplates deposited on 2D g-C3N4 nanosheets (denoted as g-C3N4/Ag:ZnIn2S4). This construct benefits from improved visible-light absorption by unveiling a greater number of catalytically active sites, effectively enhancing charge-carrier separation and relocation. Detailed analysis has proved that under visible-light irradiation, the optimized g-C3N4/20 wt% Ag:ZnIn2S4 nanocomposite has substantially upgraded photocatalytic activity in hydrogen formation by water splitting (hydrogen evolution rate of up to 597.47 μmol h−1 g−1) and in residual dyestuff degradation (methyl orange, MO; degradation rate constant of 0.1406 min−1). Noteworthily, these two exceptionally high values respectively represent 30.73 and 5.42 times enhancements vs. results obtained with bare g-C3N4. Another strong point of our g-C3N4/Ag:ZnIn2S4 is its impressive recyclability for 20 runs, with no relevant metal release in the aqueous solution following photocatalysis. This work introduces new, superior access to highly efficient photocatalysts founded on 2D/2D nanocomposites serving both the production of hydrogen as an energy carrier and environmental remediation.
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