DALTON TRANSACTIONS
·
2020
·Vol. 49
·期 7
·2258-2263
·
IF 4.174
Jin Wang,Shuang Wang,Jinping Li
In this study, we report sulfur-doped three-dimensional graphene (S-3DG) as a metal-free electrocatalyst for N2 reduction reaction (NRR) under ambient conditions. Due to the high electron transport capacity and stable physicochemical properties of 3DG, it was utilized to improve the NRR catalytic performance dramatically. Hence, in 0.05 M H2SO4 the S-3DG achieved a remarkably large NH3 yield of 38.81 μgNH3 mgcat−1 h−1 and a high faradaic efficiency of 7.72% at −0.6 V versus a reversible hydrogen electrode (RHE), which is superior to most non-metal catalysts. Notably, it shows such outstanding selectivity that no hydrazine by-products were detected and the electrochemical stability passed a long-term durability test.
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ADVANCED POWDER TECHNOLOGY
·
2019
·
IF 3.25
Kedir Ebrahim Ahmed,Dong-Hau Kuo,Worku Lakew Kebede
Heterojunction construction with low band gap materials is an effective way of utilizing UV light active materials under visible light irradiation. Here, we report the synthesis of Bi 2 (O,S) 3 /Zn(O,S) heterostructure using simple solvothermal method without surfactant. The catalysts were investigated with different characterization techniques. All the composite catalysts showed high light absorption capacity in the whole visible light spectrum. The catalytic activity of the catalysts was evaluated by Cr(VI) reduction. While pure Zn(O,S) catalyst showed no significant Cr(VI) reduction, higher photocatalytic activity than individual components were exhibited after heterojunction construction with Bi 2 (O,S) 3 . 20-BiZnOS catalyst with Bi/Zn molar percentage of 20% showed the best photocatalytic activity among the composites with 99.5% Cr(VI) reduction within 12 min under visible light irradiation. Heterojunction formation between Bi 2 (O,S) 3 and Zn(O,S) nanoparticle, and selective adsorption of Cr(VI) and desorption of Cr(III) on the surface of 20-BiZnOS composite catalyst were ascribed to the enhanced photocatalytic activity of the composite catalyst.
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HIGH PERFORMANCE POLYMERS
·
2014
·
IF 1.09
Jiangtao Liu,Guofei Chen,Xingzhong Fang
A series of isomeric poly(thioether ether imide)s (PTEIs) containing both thioether and ether linkages were prepared by aromatic nucleophilic substitution reaction of isomeric bis(chlorophthalimide)s (BCPIs) with bis(4-mercaptophenyl) ether (BMPE). The inherent viscosities of synthesized polymers were found in the range of 0.41–0.86 dL g−1 in N-methyl-2-pyrrolidone at 30°C. The glass transition temperature (Tg) of the isomeric PTEIs were 210–242°C and increased by increasing the content of 3-substituted phthalimide unit in the polymer backbone. The 5% weight loss temperature values reached up to 525–539°C under nitrogen and 523–534°C in air atmospheres, respectively, which indicated this kind of polyimide possessed excellent thermal stability. Flexible films could be cast from the polymer solution. The PTEI films exhibited moderate mechanical properties with tensile strengths of 106–127 MPa, elongations at break of 8.6–11.5%, and tensile moduli of 2.2–2.8 GPa, respectively. Dynamic mechanical thermal analysis results illustrated that the storage moduli (E′) of PTEI (a–e) almost completely maintained at about 2.3 GPa before reaching the corresponding Tg. It is noted that the minimum melt viscosity of isomeric PTEIs (a′–e′) decreased by increasing the content of unsymmetrical 3,4′-substituted phthalimide unit in the polymer main chain.
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FORENSIC SCIENCE INTERNATIONAL
·
2014
·
IF 2.115
Ting Wang,Baohua Shen,Yan Shi,Ping Xiang,Zhiguo Yu
Methamphetamine (MA) and amphetamine (AM) are widely abused drugs. Differentiation of MA and/or AM abuse from therapeutic ingestion of MA and/or AM or one of their precursor drugs is therefore of relevance in clinical and forensic toxicology. The aim of the study was to develop a simple, rapid, and accurate method for the chiral separation and determination of R / S -MA and R / S -AM in urine using liquid chromatography electrospray ionization tandem mass spectrometry operating in the positive ion multiple-reaction monitoring (MRM) mode. 20 μL of urine was diluted 500 times and 20 μL was injected. The chromatographic system consisted of a Chirobiotic™ V2 column (2.1 mm × 250 mm, 5 μm), and the mobile phase was methanol containing 0.1% (v/v) glacial acetic acid and 0.02% (v/v) ammonium hydroxide. The method was fully validated through assessments of its linearity (0.05–50.00 mg/L, r 2 > 0.994 for all analytes), and LOQ (0.05 mg/L for all analytes). No matrix effect was observed. The method was successfully applied to 86 urine samples from suspected MA abusers. Only the S -isomers of MA and AM were detected in 72 samples. The concentrations of R -MA ranged from below the LOQ to 13.76 mg/L in 14 urine samples with both enantiomers of MA and/or AM. Pure S -MA is the most common found analyte in urine and principally used by abusers.
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Journal of Materials Chemistry A
·
2022
·Vol. 10
·期 47
·25279-25294
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IF 14.511
Linlin Sun,Xiaoshuo Liu,Xiaohan Jiang,Yibing Feng,Xunlei Ding,Nan Jiang,Jigang Wang
Inadequate accessible active sites and inhibited electron separation efficiency are always burning issues. This work successfully solves the above problems by constructing a novel S-scheme heterojunction with S–C bonds bridging composed of hierarchical g-C3N4 (3DA-CN) coupled with sulfur vacancies (Sv) ZnIn2S4 (Sv-ZIS/CN). The special structure provides more active sites for the photocatalytic reaction and maintains multiple light transmission channels, resulting in the improvement of the capture and conversion of solar energy. The interfacial electric field and S–C bonds as well as their effects benefiting the regulation of the efficiency of electrons transfer for efficient photocatalytic reactions are deeply investigated and comprehended. The tetracycline degradation efficiency of Sv-ZIS/CN reaches 96.36% and has the highest k value (0.03361 min−1), which is 7.55, 5.47 and 3.04 times that of 3DA-CN, Sv-ZIS and ZIS-S/CN (prepared by a mechanical approach), respectively. Meanwhile, H2O2 production experiments also verified that the photocatalytic activity of Sv-ZIS/CN was significantly improved compared with ZIS-S/CN. The mechanisms of tetracycline degradation and H2O2 production are discussed in depth. This work provides an unparalleled and impressive strategy to construct significantly efficient photocatalysts.
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ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Guiting Chen,Gaoheng Qian,Shuwang Yi,Zhicai He,Hong-Bin Wu,Wei Yang,Bin Zhang,Yong Cao
The development of effectively universal interfacial materials for both conventional and inverted polymer solar cells (PSCs) plays a very crucial role in achieving highly photovoltaic performance and feasible device engineering. In this study, two novel alcohol-soluble conjugated polymers (PBSON-P and PBSON-FEO) with bis(benzothiophene-S,S-dioxide)-fused aromatics (FBTO) as the core unit and amino as functional groups are synthesized. They are utilized as universal cathode interfacial layers for both conventional and inverted PSCs simultaneously. Ascribing to the enlarged conjugated planarity and higher electron affinity for an FBTO unit, both PBSON-P and PBSON-FEO exhibit versatile electron-transporting abilities. They show wide band gaps that are important for light absorption in inverted PSCs, at which point PBSON-P and PBSON-FEO are more progressive than some of the reported small band gap cathode interfacial materials. Importantly, PBSON-P and PBSON-FEO display deep highest occupied molecular orbital energy levels, which can block holes at the cathode and thus increase the fill factor. As a result, both conventional and inverted PSCs using PBSON-P and PBSON-FEO as cathode interlayers realize high photovoltaic performance. Therefore, this series of novel polymers are amphibious cathode interfacial materials for high-performance conventional and inverted PSCs.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2022
·
IF 10.753
Yuxin Liu,Tianye Wang,Ningning Song,Quanying Wang,Yuqing Wu,Ying Zhang,Hongwen Yu
An efficient, simple, and inexpensive N, S-co-doped hydrochar (SNHC) was synthesized from waste straw by a one-pot hydrothermal process without calcination for the removal of Cr(VI). SNHC demonstrated excellent adsorption performance for Cr(VI) and high stability, achieving a high capacity of 171.33 mg/g (293 K, pH 2) and a capacity retention of 82.73 % after five cycles. The adsorption behavior was determined as a multilayer adsorption process based on chemisorption according to the simulation the results of Freundlich adsorption isotherms and pseudo-second-order models. The characterization of SNHC revealed that graphite N and thiophene S formed by the material were the effective active sites, functioning as electron donors to contribute a significant amount of electrons to reduce Cr(VI) to Cr(III). Therefore, next to electrostatic adsorption and complexation, the synergistic reduction of Cr(VI) by graphite N and thiophene S was the main mechanism for Cr(VI) removal. Additionally, density functional theory calculations indicated a low adsorption energy of thiophene S, which increased the attractive interaction between SNHC and Cr(VI) and played the most important role in reducing Cr(VI). The mechanism of the effect of graphite N and thiophene S on Cr(VI) removal not only offered a comprehensive perspective on the role of N, S co-doped mediation in hydrochar but also provided the basic theory for its practical application.
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CHINESE JOURNAL OF CATALYSIS
·
2020
·
IF 6.146
Minglun Cheng,Xiongfei Zhang,Yong Zhu,Mei Wang
Photocatalytic reduction of CO 2 to CO is a promising approach for storing solar energy in chemicals and mitigating the greenhouse effect of CO 2 . Our recent studies revealed that [( μ -bdt)Fe 2 (CO) 6 ] ( 1 , bdt = benzene-1,2-dithiolato), a [FeFe]-hydrogenase model with a rigid and conjugate S-to-S bridge, was catalytically active for the selective photochemical reduction of CO 2 to CO, while its analogous complex [( μ -edt)Fe 2 (CO) 6 ] (2, edt = ethane-1,2-dithiolato) was inactive. In this study, it was found that the turnover number of 1 for CO evolution reached 710 for the 1 /[Ru(bpy) 3 ] 2+ /BIH (BIH = 1,3-dimethyl-2-phenyl-2,3-dihydro-1H-benzo[ d ]-imidazole) system under optimal conditions over 4.5 h of visible-light irradiation, with a turnover frequency of 7.12 min −1 in the first hour, a high selectivity of 97% for CO, and an internal quantum yield of 2.8%. Interestingly, the catalytic selectivity of 1 can be adjusted and even completely switched in a facile manner between the photochemical reductions of CO 2 to CO and of protons to H 2 simply by adding different amounts of triethanolamine to the catalytic system. The electron transfer in the photocatalytic system was studied by steady-state fluorescence and transient absorption spectroscopy, and a plausible mechanism for the photocatalytic reaction was proposed.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2020
·
IF 5.774
Fekadu Tadesse Bekena,Dong-Hau Kuo,Worku Lakew Kebede
Wastewater treatment becomes an important part to improve environmental quality and protect water resources. Thus, developing a new photocatalyst is a key solution for environmental issues. Herein, universal, highly efficient, and novel Bi 2 (O,S) 3 /Mo(O,S) 2 nanocomposite photocatalyst was fabricated by a facile method and the crystal structure, morphology, composition, and optical properties of the as-prepared catalysts were characterized in details. The photocatalytic performance of the catalysts was evaluated by the photodegradation of methyl orange (MO), rhodamine B (RhB), methylene blue (MB), and neutral red (NR), the results showed that 20% Bi-MoOS nanocomposite had excellent photodegradation activity towards all dyes. 96.0% of MO, 96.6% of RhB, 98.8% of MB and 91.3% of NR dyes were removed after 180 min, 40 min, 20 min, and 25 min visible light irradiation, respectively. The photodegradation of these dyes was further confirmed with HPLC. The excellent photocatalytic activity of the nanocomposites was due to the efficient separation and transport of photogenerated charge carriers induced by the fabricated binary heterostructures. The photodegradation fitted well the pseudo-first-order kinetics. The active species capture experiment study showed that, OH, O 2 − and h + all took parts in the degradation of dyes. The stability of the catalyst and reaction mechanism also explained in this work.
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Frontiers in Chemistry
·
2023
·
IF 5.5
Liping Zhao,Ye Zhao,Lihe Zhao,Gang Liu
A nitrogen–sulfur dual-doped black fungus porous carbon (NS-FPC) matrix was prepared with natural black fungus as the carbon source and cysteine as the nitrogen–sulfur source. A black fungus-based solution was obtained by hydrothermal treatment. After further carbonization activation and combination with sulfur processing, the NS-FPC/S positive electrode materials were prepared. The uniform recombination of biomass carbon provides an efficient conductive framework for sulfur. The porous structure is conducive to the transport of electrolytes. Heteroatom doping can provide a more active site. The structure and composition analyses of the materials were carried out using X-ray diffraction (XRD). The electronic binding energy and bonding state were analyzed by X-ray photoelectron spectroscopy (XPS). The morphology was observed by scanning electron microscopy and transmission electron microscopy. The specific surface area and pore size distribution were analyzed using an N 2 adsorption–desorption experiment. Sulfur loading was determined through thermogravimetric analysis. The electrochemical performance of NS-FPC/S in Li–S batteries was systematically investigated. The result shows that the NS-FPC/S electrode maintains more than 1,000 mAh g -1 reversible capacity after 100 cycles at 0.2 C current density, with a capacity retention of 85%. The cycle and rate performance are both considerably superior to those of traditional activated carbon materials.
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POLYMER DEGRADATION AND STABILITY
·
2023
·
IF 5.9
Shasha Tang,Haidan Lin,Kai Dong,Jun Zhang,Chengji Zhao
The waste and desertion of petroleum-based epoxy resins have attracted increasing concerns on the damage and pollution to the environment because they are difficult to reprocess and reuse after curing. Once broken or injured, the recovery or degradation of composites is a tough challenge owing to their permanently cross-linked networks. In this paper, a novel guaiacol-based epoxy resin (BGF-EP) was prepared from renewable resources instead of conventional petroleum-based bisphenol A, curing with 4-aminophenyl disulfide (AFD). The epoxy vitrimer BGF-EP-AFD had appreciable thermal stability ( T g :143 °C, T d5% :295 °C), sufficient mechanical properties (tensile strength:55.54 MPa, elongation at break:12.23%) and stress relax from 300 min at 130 °C to 27.5 s at 200 °C. And the vitrimer could be reprocessed into a complete film. More excitingly, an efficient strategy was proposed to dissolve the cured resin and recycle its carbon fiber reinforced composites in a closed loop in an appropriate mixing solution (50%DMF/50%β-ME) at room temperature. The recovered carbon fibers are not altered and remain intact for the next utilization as confirmed by SEM. This work contributes the development of guaiacol-based renewable functional materials and provides a feasible and economical way to recycle and reprocess the carbon fiber reinforced epoxy composites.
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Journal of Materials Chemistry A
·
2017
·Vol. 5
·期 20
·9873-9881
·
IF 8.867
Mingyu Tong,Shengwen Liu,Xian Zhang,Tianxing Wu,Haimin Zhang,Guozhong Wang,Yunxia Zhang,Xiaoguang Zhu,Huijun Zhao
Due to their controllable morphologies, tunable porous structures, diverse compositions and easy fabrication, metal–organic frameworks (MOFs) are an ideal class of precursor material to develop high performance carbon-based materials for energy applications. In this work, two-dimensional (2D) Co/Ni MOFs nanosheets with a molar ratio of Co2+ to Ni2+ of 1 : 1 were first synthesized at room temperature using thiophene-2,5-dicarboxylate (Tdc) and 4,4′-bipyridine (4,4′-Bpy) as organic linkers. As a precursor material, the as-synthesized 2D Co/Ni MOFs nanosheets were further pyrolized at 550 °C in N2 atmosphere to incorporate 2D CoNi alloy nanoparticles into S, N-doped carbon nanosheets (CoNi@SNC) with a surface area of 224 m2 g−1, a porous structure, and good conductivity. Interestingly, it was found that the 2D Co/Ni MOFs nanosheets can be directly used as electrode materials for supercapacitors, delivering a specific capacitance of 312 F g−1 at 1 A g−1, whereas CoNi@SNC derived from its MOFs precursor as an electrode material for supercapacitors exhibits a much higher specific capacitance (1970, 1897 and 1730 F g−1 at 1, 2, 5 A g−1, respectively) with long cycling life (retaining 95.1% of the value at 10 A g−1 after 3000 cycles) and excellent rate capability at a high charge/discharge current. Further, an asymmetric supercapacitor device was constructed with CoNi@SNC as the positive electrode and active carbon as the negative electrode, exhibiting an energy density of 55.7 W h kg−1 at a power density of 0.8 kW kg−1 with lifetime stability up to 4000 charge–discharge cycles (capacitance retention of ∼90.6%). The results demonstrate that electrochemical activation-generated CoNi oxides/oxyhydroxides on the surface of the CoNi alloy nanoparticles in alkaline electrolyte during electrochemical measurements are the electrochemical active species of the CoNi@SNC-constructed supercapacitor. Additionally, the high performance of the CoNi@SNC-constructed supercapacitor can be collectively attributed to its relatively high surface area, which is favourable for the exposure of electrochemical active sites; its porous structure, which promotes redox-related mass transport; and the combination of CoNi alloy nanoparticles with graphitic carbon, which functions as an electron collector to improve electron transfer.
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