Nanoscale
·
2018
·Vol. 10
·期 32
·15238-15248
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IF 7.233
Qijun Che,Ningning Bai,Qing Li,Xinhong Chen,Ya Tan,Xi Xu
An enormous challenge in the development of renewable hydrogen sources for electricity-driven water-splitting systems has been the limitation of the earth-abundant and robust highly-active cathode electrocatalysts. In this work, we developed a simple sulfur-anion doping strategy to obtain the S-doped NiCo composite (S-NiCo@50) on Ni foam (NF) via a one-step electrochemical deposition. It was found that doped sulfur plays a crucial role in reducing the overpotential of hydrogen evolution by providing abundant active sites as identified by the XPS spectrum. The formed metallic Ni and Co effectively promoted electron transportation. The synergistic effects between the amorphous CoxNiyS(x+y) substance and crystalline Ni and Co metal seemed to result in enhanced HER activity. In particular, the S-NiCo@50 electrode, featuring a hierarchical morphology, showed an ultralow overpotential of 28 and 125 mV at 10 and 100 mA cm−2, respectively, in 1.0 M NaOH with a large exchange current density (j0) of 4.8 mA cm−2 as well as high conductivity and stability; its catalytic properties are superior to most of the reported alkaline electrocatalysts and are on par with commercial Pt/C. Assembled with the counter electrode (Ni–Fe/NF), the overall water splitting was proved with a low 1.55 V at 10 mA cm−2. Moreover, we built the Ni24Co6S6 cluster as the S-NiCo@50 model and revealed its intrinsic activity by density functional theory (DFT) calculations. This study shows that S-doping and component control can be an exquisite strategy for realizing high-efficiency electrochemical water reduction.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2018
·
IF 4.229
Chenyi Wang,Yuanpeng Zhou,Chang Xu,Xiaoyan Zhao,Jian Li,Qiang Ren
In order to enhance the properties of polymer anion-exchange membranes (AEMs), a class of side-chain-type poly (arylene ether sulfone)s containing tri-imidazole cations in pendant phenoxyphenyl spacer (i.e., Im-PES-xx) were designed and prepared by polymer grafting reaction. Based on these imidazole functionalized polymers, a series of new AEMs were successfully prepared by their solution coating and ion exchange. The obtained membranes exhibited good alkaline stability with the retention of ion-exchange capacity in the range of 78.5%–83.3% after immersion in 4 M NaOH solution at 80 °C for 336 h. The membranes also had high hydroxide conductivity with the values of 34.1–70.5 mS cm −1 at 80 °C. Meanwhile, these membranes possessed good dimensional stability, and their swelling ratio was in the range of 2.5%–7.0% at 80 °C. The incorporation of the dense and local imidazole cations in the side chains for AEMs plays an important role for their properties.
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NEW JOURNAL OF CHEMISTRY
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2018
·Vol. 42
·期 4
·2857-2864
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IF 3.201
Chunxi Zhao,Yang Jiao,Lei Zhang,Yaling Yang
Herein, we report a fast and selective technique for the determination of diethylstilbestrol in milk sample using fluorescent sulfur and boron co-doped carbon dots (S,B co-doped CDs). The S,B co-doped CDs were synthesized by hydrothermal synthesis using poly(sodium-p-styrenesulfonate) and borax as precursors. The as-prepared S,B co-doped CDs possess good stability and fluorescence characteristics and exhibit a fluorescence quantum yield of 25.7%. The fluorescence intensity of the S,B co-doped CDs decreased in the presence of diethylstilbestrol, and a good linear relationship existed between the fluorescence quenching and different concentrations of diethylstilbestrol in the range of 0.1–200 μM with a detection limit of 0.06 μM. Finally, the S,B co-doped CDs were successfully applied in the detection of diethylstilbestrol in milk samples, yielding recoveries between 90.4% and 109.2%.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2018
·
IF 2.88
Zhenxing Qin,Wenhai Wang,Xiaozhi Zhan,Xiujuan Du,Qingmei Zhang,Rui Zhang,Kun Li,Jinhong Li,Weiping Xu
Luminescent carbon-based nanoparticles , named often as carbon dots (CDs), were synthesized from citric acid (CA) and guanidine thiocyanate (GITC) via an N and S co-doped hydrothermal procedure. In the present structure characterization, N and S elements could be sufficiently doped by means of the heteroatom or the functional groups bonded on the surface of CDs. The as-prepared CDs solution showed blue color fluorescence under ultraviolet excitation, yet the PL spectra exhibited a repetitive emission process from excitation-independent to excitation-dependent. In view of the triexponential feature of fluorescence lifetimes of CDs, one possibility was proposed to be co-existence of two types of CDs with different surface states. Additionally, the as-prepared CDs were used as a sensing probe for the detection of Ag + taking into consideration of the possible interactions between Ag + and various fluorophores attached to the CD surface. As expected, the changes of fluorescence intensities were linearly proportional to the different concentration ranges of Ag + , which suggests the complex nature of the quenching mechanism. And for the first time, the S C N group was found to accelerate the quenching of CDs towards Ag + , promising a new approach for efficient detection of Ag + for the application in industrial pollutants.
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Journal of Materials Chemistry A
·
2018
·Vol. 6
·期 38
·18649-18659
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IF 9.931
Zheming Liu,Aiwei Tang,Jun Liu,Dongxu Zhu,Xifeng Shi,Qinghua Kong,Zhijie Wang,Shengchun Qu,Feng Teng,Zhanguo Wang
Multinary copper-based chalcogenides have been exploited in photocatalytic hydrogen generation due to their exceptional visible light absorption properties and environmentally friendly character. Similar to other photocatalysts, to reinforce the charge separation and transfer is one of the most important pathways to enhance photocatalytic hydrogen evolution, which can be achieved by rationally designing the nanostructures and geometries of multinary copper-based chalcogenides. Herein, an improved photocatalytic hydrogen evolution is successfully realized in L-shaped Cu–Ga–Zn–S (CGZS) alloyed nanorods compared with the binary Cu31S16 and ternary CuGaS2 nanocrystals. The L-shaped wurtzite CGZS nanorods with a uniform spatial composition distribution are synthesized via a non-injection solution approach for the first time. The successive incorporation of zinc and gallium ions into Cu31S16 seeds leads to formation of Cu31S16–ZnS and Cu31S16–CGZS heteronanostructures and finally results in the formation of single phase CGZS nanorods. The intrinsic features of L-shaped wurtzite CGZS nanorods offer efficient spatial charge separation and electrical transport, which contribute synergistically to the improved photocatalytic activity. This study provides a new way to develop novel multinary copper-based chalcogenides with flexible nanostructures for efficient photocatalytic hydrogen production.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2019
·
IF 4.175
Worku Lakew Kebede,Dong-Hau Kuo,Misganaw Alemu Zeleke,Kedir Ebrahim Ahmed
Environmentally toxic methylene blue organic pollutants are of more concerns due to their antagonistic effects on human health, animals, and plants, thus needs serious attention for their removal. For elimination purpose, the Sb-doped Mo(O,S) 3 oxy-sulfide nanoplate catalyst with different Sb contents was synthesized at low temperature of 95 °C via a facile method. The structural, morphological, chemical composition, optical properties , and electrical conductivity of the catalyst were characterized with different techniques. The photocatalytic performance of Sb-Mo(O,S) 3 at various Sb contents was investigated for the degradation of methylene blue dye under visible light irradiation using hydrogen peroxide as an effective electron scavenger to further accelerate the reaction. It was observed that the incorporation of Sb enhanced the catalytic activity. Sb-Mo(O,S) 3 -10 was the most efficient catalyst with excellent activity to degrade 99.7% of the dye within 60 min irradiation time. The degradation kinetics follows a pseudo-first-order reaction with a rate constant 8.78 × 10 −2 min −1 , which is 3-fold higher than that for Sb- Mo(O,S) 3 -0 catalyst. Sb-Mo(O,S) 3 -10 showed slower recombination of photogenerated charge carriers and lower charge transfer resistance which proved to be capable for the removal of toxic methylene blue organic pollutant.
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ACS Applied Nano Materials
·
2018
·
IF 0
Kai Yang,Lei Zhong,Jiaxiang Qin,Junchen Liu,Min Xiao,Dongmei Han,Shan Ren,Luyi Sun,Shuanjin Wang,Yuezhong Meng
The high theoretical specific capacity of lithium–sulfur battery is regarded as a promising candidate for next-generation battery systems. However, “polysulfide shuttle” is known as a major issue of accelerating capacity fading and corroding the metal lithium anode, which impedes its commercial application. Here, a nitrogen–sulfur codoped two-dimensional carbon material is synthesized using a novel template method by pyrolyzing chemical adsorption of montmorillonite and methylene blue. The microstructure and morphologies of the synthesized two-dimensional carbon materials are fully characterized using SEM, TEM, XRD, and Raman techniques. The experiment results indicate that the carbon material shows a typical graphene structure. The micro/mesoporous and heteroatoms codoped structure of the synthesized carbon material exhibits excellent performance in electronic conductivity and polysulfides confinement. The functional separator laminated with the binder-free carbon material endows the battery outstanding electrochemical and rate performances. The excellent rate performance is discovered a capacity of 828 mAh g–1 at 4 C with good reversibility. The battery presents a high initial discharge specific capacity of 1049 mAh g–1 with good capacity retention of 690 mAh g–1 after 500 cycles at 1 C. Consequently, the separator laminated with the nitrogen–sulfur codoped graphene is promising for the construction of high performance Li–S batteries.
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CHEMICAL ENGINEERING JOURNAL
·
2018
·
IF 6.735
Liwei Chen,Xiaoxin Hu,Ying Yang,Canlan Jiang,Cheng Bian,Chao Liu,Miaoyue Zhang,Tianming Cai
The occurrence of s -triazine herbicides in soils and groundwaters has been reported globally and remediation of these contaminated sites are essentially imperative, especially at accidental spill sites. Present work investigated the feasibility of using Fe 2+ catalyzed persulfate (PS) to effectively degrade s -triazine herbicides (e.g., atrazine (ATZ), terbuthylazine (TEA) and ametryn (AMT)) in soils. The degradation kinetics, mechanisms and soil-types effects were systematically investigated. For arable soil A1, extent of degradation reached 80% for 100 mg kg −1 ATZ contaminated soil after 600 min (PS/Fe 2+ of 16.6 mM/16.6 mM) at 23 °C. Increasing PS and Fe 2+ dosages could enhance ATZ degradation. Acidic condition was favorable for the degradation of ATZ with Fe 2+ /PS process and the contribution of SO 4 − to the overall degradation of ATZ decreased as initial pH increased. The ethyl group and chloride substituent on molecular structure of ATZ affected its degradation comparing to other two s -triazine herbicides. ATZ degradations in two arable soils and one paddy soil indicated that different soils with various physical-chemical properties, such as soil organic matter, available and total Fe contents, may influence the ATZ degradation. Moreover, a total of five degradation products of ATZ were identified in soil A1 by Fe 2+ /PS process. Three degradation pathways including alkyl chain oxidation, dealkylation and dechlorination-hydroxylation reactions with the underlying oxidation mechanisms were tentatively proposed.
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CHEMICAL ENGINEERING JOURNAL
·
2017
·
IF 6.216
Xiao-Fei Wang,Gui-Gen Wang,Jia-Bing Li,Zheng Liu,Wen-Feng Zhao,Jie-Cai Han
In this article, a new application of using S, N co-doped graphene quantum dots (S, N-GQDs) as ideal color converters in solid-state white light-emitting diode (WLED) is reported. To this end, the S, N-GQDs with an average diameter of ∼4.46 nm are obtained by a hydrothermal approach using citric acid and thiourea as source materials. The PL spectra of S, N-GQDs show an excitation-independent behavior in the range of 300–380 nm. Under UV illumination, the S, N-GQDs display intense blue-light with the quantum yield of 51.2%. The PL mechanism is also investigated. Then, we fabricate freestanding luminescent composite films in a solution casting method by combining S, N-GQDs with YAG:Ce 3+ phosphors based on a polyvinyl alcohol (PVA) matrix. The luminescent films have superior foldability and photostability and excellent heat resistance, and retain their optical performances in the solid-state. To realize their potential, a high-powered remote WLED has been demonstrated. The results indicate that S, N-GQDs and YAG:Ce 3+ can be homogeneously dispersed in the PVA without aggregation so that uniform white-light emission can be obtained. These composite films containing S, N-GQDs are promising to be used in state-of-the-art UV-pumped remote WLED according to their wide wavelength emission and collapsible illumination device.
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Journal of Energy Chemistry
·
2024
·
IF 14
Yangyang Chen,Yu Liao,Ying Wu,Lei Li,Zhen Zhang,Sha Luo,Yiqiang Wu,Yan Qing
Lithium-sulfur batteries (LSBs) are considered promising candidates for next-generation battery technologies owing to their outstanding theoretical energy density and cost-effectiveness. However, the low conductivity and polysulfide shuttling effect of S cathodes severely hamper the practical performance of LSBs . Herein, in situ-generated single layer MXene nanosheet/hierarchical porous carbonized wood fiber (MX/PCWF) composites are prepared via a nonhazardous eutectic activation strategy coupled with pyrolysis-induced gas diffusion. The unique architecture, wherein single layer MXene nanosheets are constructed on carbonized wood fiber walls, ensures rapid polysulfide conversion and continuous electron transfer for redox reactions. The C–Ti–C bonds formed between MXene and PCWF can considerably expedite the conversion of polysulfides, effectively suppressing the shuttle effect. An impressive capacity of 1301.1 mA h g −1 at 0.5 C accompanied by remarkable stability is attained with the MX/PCWF host, as evidenced by the capacity maintenance of 722.6 mA h g −1 after 500 cycles. Notably, the MX/PCWF/S cathode can still deliver a high capacity of 886.8 mA h g −1 at a high S loading of 5.6 mg cm −2 . The construction of two-dimensional MXenes on natural wood fiber walls offers a competitive edge over S-based cathode materials and demonstrates a novel strategy for developing high-performance batteries.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
·
IF 8.1
Rourou Zhang,An Ding,Xuejun Cai,Peter Desmond,Xu He,Guibai Li,Heng Liang,Chuyang Y. Tang
The fluctuation of pathogen removal in ultrafiltration (UF) systems and its dependence on irreversible fouling necessitates frequent chemical cleaning/disinfection, raising concerns about leakage of conditioned pathogens. An additional barrier utilizing carbon materials with notable adsorption and antimicrobial properties offers a promising and practical solution. This study achieved complete retention of nano-sized viruses (∼6 log reduction value (LRV)) and micron-sized bacteria (∼7 LRV) by introducing ε-polylysine (EPL)-modified biochar (BC) into UF feeds. During the UF process, biochar with superior adsorption capacities and conformational flexibility, significantly enhanced the entrapments of natural organic matter (NOM), viruses, and bacteria. Specially, EPL exhibited conformational transitions that adapted to different NOM (macromolecule proteins and linear polysaccharides), greatly facilitating the formation of reversible biochar-NOM cake layers and the transfer of pathogens from the irreversible fouling layer to the biochar surface and reversible fouling layer. The random coil structures of EPL promoted electrostatic attraction for virus particles, while bend or sheet-like structures created barriers for both bacteria and viruses through a refined NOM-biochar network. The trapping of viruses was attributed to the combined effects of electrostatic attraction, bonding forces, and the complex cake layers. And size exclusion by the biochar-NOM complex fouling layer played a prominent role in the retention of bacteria. This breakthrough in addressing the trade-off between irreversible fouling and pathogen removal inspires promising applications of EPL-modified biochar for UF systems to consolidate barriers for water and process biosafety. Future efforts should focus on EPL′s conformational response to protein-like NOM with significant steric hindrance, which pose challenges for fouling alleviation and bacteria capture.
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Journal of Materials Chemistry A
·
2025
·
IF 9.5
Yuanyuan Yang,Tingting Luo,Min He,Jie Yu,Xiao Wu,Mingze An,Ting Lei,Qingqing Qin,Shuhao Qin
The non-homogeneous photocatalysis-self-Fenton technology represents a highly effective strategy for the degradation of pollutants. However, conventional catalysts are hindered by limitations such as restricted light absorption and challenges in separation. In this study, BaFe12O19 (BFO) was combined with iron-carbon dots modified resorcinol-formaldehyde (FRF) to construct an S-scheme heterojunction (BFR), which was subsequently incorporated into a cross-linked polyacrylic acid-base hydrogel (PAM) matrix to fabricate a floating composite gel catalyst. Under visible light irradiation, this catalyst achieved complete degradation of 20 mg/L chloroquine phosphate within 30 minutes, exhibiting a reaction rate constant 10 times greater than that of the BFR powder catalyst. The rate of in-situ generated H2O2 (30.05 mmol g−1 h−1) also increased by 11 times, that promoting the production of hydroxyl radicals (•OH). This significant improvement can be attributed to enhanced adsorption capacity of PAM hydrogel (124.2 mg g-1), superior near-infrared absorption, and photothermal effects of BFR heterojunction. The underlying mechanisms, including the formation of internal electric fields between FRF and BFO and the construction of the S-scheme heterojunction, were elucidated using in situ XPS and Kelvin probe force microscopy. Additionally, the analysis of reactive species, with potential degradation pathways for chloroquine phosphate (CQ), while toxicity assessments of the degradation products were conducted. This design of a floating photocatalyst provides an innovative approach to the development of efficient and recyclable photo-self-Fenton systems.
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