WATER RESEARCH
·
2023
·
IF 12.8
Jiaming Guo,Dong Wang,Yinghao Shi,Honghong Lyu,Jingchun Tang
The corrosion and surface passivation of sulfidized zero-valent iron (S-ZVI) by common groundwater ions and contaminants are considered to be the most challenging aspects in the application of S-ZVI for remediation of chlorinated contaminants. This study investigated the impacts of corrosive chloride (Cl − ) and passivation of hexavalent chromium (Cr(VI)) on the long-term reactivity, selectivity, corrosion behavior, and physicochemical properties during the 60-day aging process of S-ZVI. Although the co-existing of Cl − promoted the initial reactivity of S-ZVI, the rapid consumption of Fe° content shortened the reactive lifetime owing to the insufficient electron capacity. Severe passivation by Cr(VI) (30 mg L −1 ) preserved the Fe° content but significantly interfered with the reductive sulfur species, resulting in an increase in electron transfer resistance. In comparison, minor passivated S-ZVI (5.0 mg L −1 Cr(VI)) inhibited the hydrogen evolution while concurrently mitigating the further oxidation of the reductive iron and sulfur species, which significantly enhanced the long-term reactivity and selectivity of S-ZVI. Furthermore, the enhancement effect of minor passivation could be detected in the aging processes of one-step, two-step, and mechanochemically synthesized S-ZVI particles with different S/Fe ratios and precursors, which further verified the advantages of minor passivation. This observation is inspirable for the development of innovative strategies for environmental remediation by S-ZVI-based materials.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Materials Horizons
·
2023
·Vol. 11
·期 3
·768-780
·
IF 13.3
Guiyang Yu,Ke Gong,Xiang Li,Luyang Guo,Xiyou Li,Debao Wang
The achievement of dual-functional photocatalytic technology requires a photocatalyst with accelerated charge flow and purposeful active-site arrangement. In this study, we developed an oriented embedding strategy to induce ReS2 growth at the S vacancy in twin-crystal Zn0.5Cd0.5S solid solution (Sv-ZCS), obtaining an atomic-level heterostructure (ReS2/Sv-ZCS). The electronic structure calculations demonstrate that the charge density of the Zn atom around the S vacancy is higher than for other Zn atoms and the introduced S vacancy establishes a high-speed channel for electron transport via formed Zn–S–Re bonds at the interface between ReS2 and Sv-ZCS. Photogenerated electrons and holes gathered on Re atoms and Sv-ZCS, respectively, which achieves spatial charge separation and separated arrangement for redox sites. As a result, the optimized ReS2/Sv-ZCS heterostructure possesses high efficiency of electron injection (2.6-fold) and charge separation (8.44-fold), as well as excellent conductivity capability (20.16-fold). The photocatalytic performance of the ReS2/Sv-ZCS composite exhibits highly improved dual-functional activity with simultaneous H2 evolution and selective oxidation of benzyl alcohol. The reaction rate of benzaldehyde and H2 evolution reaches 125 mmol gcat−1 h−1 and 159 mmol gcat−1 h−1, which is the highest efficiency achieved so far for simultaneous coproduction of H2 fuel and organic chemicals on ReS2-based composites. This work enriches the application of ReS2-modified composites in a dual-functional photoredox system and also gives insight into the role of defects in electronic structure modification and activity improvement.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHINESE JOURNAL OF POLYMER SCIENCE
·
2021
·Vol. 39
·期 11
·1459-1469
·
IF 3.603
Liu Yuan-Biao,Shi Gao-Peng,Wu Guo-Zhang
Introducing small molecule-bridged hydrogen bonds (HBs) between polymer chains has been reported to effectively reduce the interchain cooperativity despite of strengthening the intermolecular interaction. Here, a systematic investigation on tuning the Johari-Goldstein β ( β JG ) relaxation by adding various low-molecular-weight phenols in poly( n -alkyl methacrylate)s is carried out to further clarify the anomalous dynamics. Given these small molecules capable of coupling the motion with pendent groups of host polymers due to forming at least two HBs per molecule, poly( n -alkyl methacrylate) mixtures exhibit rich dynamic changes in the β JG -properties and α, β JG separations. An increased loading of phenols with a small size and strong inter-HB strength (Δ υ i ) clearly benefits for significant retardation and suppression of the β JG -relaxation, narrows the α, β JG separation and converges the β JG -peak with the α -peak, which demonstrates the alleviation of inter-chain topological constraints. However, small molecules with a relatively big size and weak Δ υ i are found to amplify the magnitude of the α, β JG separation of poly(butyl methacrylate), even though experimental results of changes in α -dispersion and dynamic fragility confirm a reduction of the coupling factor n in all of these hybrids. The counterintuitive phenomenon suggests that the crossover time t c in the Coupling Model is no longer a universal quantity if the inter-chain interaction of polymers is strengthened by HBs. These compelling findings shed vital insights into the HB-induced anomalous dynamics, and provide essential guidance for tailoring the β JG behavior and designing glassy polymeric materials.
✓ 已验证
产品关联
DOI
高影响因子
Molecular Catalysis
·
2023
·
IF 4.6
Linghui Kong,Bo Fan,Yu-Cai He
( S )-2-Chloro-1-(3,4-difluorophenyl)-ethanol [( S )-CFPL] is a key chiral intermediate in the manufacture of Ticagrelor. In this study, deep eutectic solvent (DES) was used as the co-solvent, and several reaction parameters were investigated and characterized. It was observed that supplementary of DES could promote the asymmetric reduction of 2‑chloro-1-(3,4-difluorophenyl) ethanone (CFPO) to ( S )-CFPL through the biological reduction by recombinant E. coli containing a NADH-dependent reductase CmCR. The high pKa value of carboxylic acid in DES and low viscosity of DES were beneficial to increase cell membrane permeability and enhancement of biocatalytic efficiency. By supplementary of DES ChCl:LA (7.5 vol%) into the bioreaction system, the efficient bioreduction reaction of 100 mM CFPO was achieved via the biocatalysis with whole-cell at 30 °C and pH 7.0, affording ( S )-CFPL in 95.9 % yield and optical purity > 99 %. The process was environmentally friendly with high biocatalytic productivity and had potential practicability in the mass production of ( S )-CFPL.
✓ 已验证
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2023
·
IF 10.9
Hainan Wei,Fanming Meng,Han Zhang,Wenqing Yu,Jialong Li,Sheng Yao
Constructing new photocatalysts for the photocatalytic reduction of CO 2 and efficient degradation of Levofloxacin is of great importance to renewable energy. Here, S-scheme Bi 2 MoO 6- x /MoS 2 heterojunction nanospheres containing abundant surface defects (oxygen vacancies) were designed and successfully synthesized to enhance CO 2 photoreduction activity in the absence of other sacrificial agents, co-catalysts or photosensitisers. At the same time, it can efficiently degrade organic pollutants (Levofloxacin). This heterogeneous structure with surface defects provides an abundance of reactive sites, accelerates charge separation and improves oxidation capacity. The improved Bi 2 MoO 6- x /MoS 2 heterogeneous nanospheres show excellent performance under simulated solar light, with the selectivity and yield of 92.45% and 29.01 µmol h −1 , respectively, for the generation of CO. Under visible light, the degradation efficiency of levofloxacin hydrochloride (LVX) reached 96.3% within 25 min and remained as high as 95% after three cycles. This work provides a new idea for the design of new S-scheme photocatalysts and an important reference for the preparation of photocatalysts for the efficient photocatalytic reduction of CO 2 and the efficient degradation of organic pollutants at the same time.
✓ 已验证
产品关联
DOI
高影响因子
DIAMOND AND RELATED MATERIALS
·
2023
·
IF 4.1
Baijian Feng,Zihao Chen,Na Li,Yongguang Bi,Fansheng Kong,Zhong Wang,Shaofan Tan
In this work, for the first time, biomass-derived carbon dots (AMP-CDs) with strong water solubility, antioxidant activity and good biocompatibility were synthesized by a one-step microwave method using Allium macrostemon Bunge polysaccharides (AMP) as the main carbon source, L-cysteine as the nitrogen and sulfur source, and phosphoric acid as the phosphorus source. The results showed that sphere-like AMP-CDs with an average particle size of about 2.34 ± 0.49 nm were successfully prepared, with good resistance to salt and photobleaching, and maintained high fluorescence intensity under normal pH conditions in human body. AMP-CDs were highly resistant to 2,2-diphenyl-1-pycrylhydrazyl (DPPH), 2,2′-Azinobis- (3-ethylbenzthiazoline-6-sulphonate) (ABTS) and hydroxyl radical (·OH) with significantly higher scavenging ability than AMP , with IC 50 (μg/mL) of 10.240, 7.265, and 574.730, respectively. In addition, AMP-CDs can be selectively used for the sensitive detection of Cr 6+ with the limit of detection was 5.25 μM, and satisfactory results were obtained for the Cr 6+ recovery experiments of actual environmental samples. In vitro cytotoxicity and hemolytic activity assays showed that AMP-CDs have good biocompatibility and can smoothly enter cells for clear imaging. Therefore, AMP-CDs are likely expected to be applied as a potential antioxidant and metal ion detection probe in the field of drug and food, environmental and biological scenario samples for metal ion detection analysis.
✓ 已验证
产品关联
DOI
高影响因子
Materials Today Physics
·
2023
·
IF 11.5
Wen-Fa Chen,Xiao-Ming Jiang,Bin-Wen Liu,Guo-Cong Guo
Infrared (IR) nonlinear optical (NLO) material with a concurrently wide band gap and significant NLO coefficient in a single crystal is an incompatible but addressable challenge. Hence, for the first time, the AgGaS 2 structure evolved into an Ag-based sulfide system integrating dual s -block elements, guiding the discovery of two NLO crystals named AMgAgGa 6 S 11 (A = K, 1 ; Rb, 2 ). Structurally, title phases possess a novel NLO functional motif [AgGa 6 S 17 ] assembled by two C 2 -type supertetrahedra through a shared [AgS 4 ] tetrahedron, in which the electropositive cations A + and Mg 2+ are embedded. Thus, compounds 1 and 2 display emulative band gaps (3.15 and 3.25 eV, exceeding that of 2.65 eV in AgGaS 2 ) toward optimizing the laser-induced damage thresholds (3.1 and 3.2 × AgGaS 2 @1064 nm). Remarkably, the noncentrosymmetric phases 1 and 2 exhibit moderate second-harmonic generation (SHG) responses (0.6 and 0.7 × AgGaS 2 @1910 nm), the greater-than-commercial half of the AgGaS 2 . To the best of our current knowledge, an experimental birefringence of 1 and 2 (0.029 and 0.027, @546 nm) is first observed in quinary ordered chalcogenides , indicating that samples 1 and 2 meet phase-matching conditions at the incident laser of 1910 nm. All these observations demonstrate that crystals 1 and 2 can become prospective NLO materials. This research will pave the way for discovering excellent IR NLO crystals with wide band gaps and impressive NLO coefficients by incorporating multiple strong electropositive elements into chalcogenides .
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Polymer Materials
·
2023
·
IF 5
Yumiao Su,Wenmu Li
Proton exchange membranes prepared from poly(aryl sulfone)s still need to overcome the drawbacks of chemical stability in acidic environments and low electrical conductivity due to water loss at high temperatures. Herein, we synthesized densely sulfonated poly(aryl sulfone) proton exchange membranes containing a 1H-imidazo[4,5-F][1,10]-phenanthroline moiety on the side chain with a metal ion coordination function. The coordination of 1H-imidazo[4,5-F][1,10]-phenanthroline groups to metal ions can effectively prevent the formation of •OH radicals from homolytic cleavage of H2O2 catalyzed by metal ions. Since the conditions for the continuous formation of •OH radicals are fundamentally eliminated, the antioxidant stability of the membrane material is greatly improved. Mesoscale microscopic simulations showed that 1H-imidazo[4,5-F][1,10]-phenanthroline has the effect of inducing phase separation, endowing the proton exchange membrane with a larger hydrophilic structural domain and possibly constructing a better connected channel for proton transport. Notably, these membranes can efficiently capture the Fe2+ and Fe3+ ions to form stable [Fe(phen)3]2+ and [Fe(phen)3]3+ interconnection points, respectively, which could not only enforce the water retention and the mechanical properties of the membranes but also serve as a catalyzed point to prevent H2O2 from undergoing homolytic cleavage and forming •OH radicals.
✓ 已验证
产品关联
DOI
高影响因子
International Journal of Electrochemical Science
·
2023
·
IF 1.5
ZhiZhong Xie,Guanghui Chen,Zhien Liu,Xinxin Zhu,Dan Liu,Rong Li,Deyu Qu,Junsheng Li
Serious shuttle effect and sluggish reaction kinetics are the two major barriers that limit the cathode cycling stability in lithium-sulfur batteries. In this study, we deviate from the prevalent approach compositing sulfur with various carbonaceous materials by introducing electrocatalysis concept in lithium-sulfur chemistries. Two-dimensional graphene has been used as model system to support electrocatalyst Pt. Uniform dispersion of Pt nanoparticles on graphene layers not only demonstrate to preferential adsorption of soluble polysulfide species, but also catalyze efficiently transformation to long-chain polysulfides in the subsequent redox process. The result rGO-Pt/S composite shows a 29.5% enhancement in capacity over pristine rGO/S electrode. More impressively, rGO-Pt/S electrode exhibits good cycling stability at a high rate of 2 C corresponding to a tiny capacity fading rate of 0.01% per cycle over 300 discharge/charge cycles. Thus, this work provides a facile strategy for improving the performance of Li-S batteries toward practical application.
✓ 已验证
产品关联
DOI
高影响因子
MOLECULES
·
2023
·Vol. 28
·期 5
·2221
·
IF 4.6
Lingxue Meng,Yige Wang,Wenwei Liu,Chunlei Fan,Haoxiong Nan,Jiang Wang,Jia Yu
Playing a significant role in electrochemical energy conversion and storage systems, heteroatom-doped transition metal oxides are key materials for oxygen-involving reactions. Herein, mesoporous surface-sulfurized Fe–Co3O4nanosheets integrated with N/S co-doped graphene (Fe–Co3O4–S/NSG) were designed as composite bifunctional electrocatalysts for the oxygen evolution reaction (OER) and the oxygen reduction reaction (ORR). Compared with the Co3O4–S/NSG catalyst, it exhibited superior activity in the alkaline electrolytes by delivering an OER overpotential of 289 mV at 10 mA cm−2and an ORR half-wave potential of 0.77 V vs. RHE. Additionally, Fe–Co3O4–S/NSG kept stable at 4.2 mA cm−2for 12 h without significant attenuation to render robust durability. This work not only demonstrates the satisfactory effect of the transition-metal cationic modification represented by iron doping on the electrocatalytic performance of Co3O4, but it also provides a new insight on the design of OER/ORR bifunctional electrocatalysts for efficient energy conversion.Keywords:iron-cobalt bimetallic oxides;surface vulcanisation;N/S co-doped graphene;oxygen evolution reaction;oxygen reduction reaction;bifunctional electrocatalyst
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF SOILS AND SEDIMENTS
·
2019
·Vol. 19
·期 12
·4042-4051
·
IF 2.669
Zhang Zhaoxue,Zhang Nan,Li Haipu,Lu Yi,Wang Qiang,Yang Zhaoguang
Purpose This study aimed to reveal spatial distribution of As, Cd, Cr, Cu, Mn, Ni, Pb, Sb, V, and Zn in paddy soils in the Zijiang River basin and to evaluate its pollution status and potential ecological risks, and thus to provide basic information for rational utilization of paddy soils in the study area. Materials and methods The heavy metal(loid) concentrations in one hundred and thirty-five paddy soil samples (these samples were collected from the top 0–20 cm layer) were measured by inductively coupled plasma-optical emission spectrometry. The spatial distribution characteristics of the heavy metal(loid)s were depicted by the Ordinary Kriging interpolation analysis. The contamination degree and potential ecological risks of the heavy metal(loid)s in paddy soils were assessed by Nemerow’s comprehensive index, geoaccumulation index, potential ecological risk factor, and potential ecological risk index. The potential sources of the heavy metal(loid)s were deduced by Pearson’s correlation analysis, hierarchical cluster analysis, and principal component analysis. Results and discussion The mean concentrations of the heavy metal(loid)s decreased in the order of Mn > V ≈ Zn > Cr > Ni ≈ Pb > Cu ≈ Sb > As > Cd. Except for Cd and Sb, the mean concentrations of As, Cr, Cu, Mn, Ni, Pb, V, and Zn were close to the background reference values. The concentration of Cd in 94.8% of samples exceeded the soil quality standard value (grade II, 5.5 < pH < 6.5, GB 15618–1995). According to the assessments of pollution and potential ecological risks for the heavy metal(loid)s, 45.2% and 46.7% of samples were severely polluted and moderately polluted, respectively. The potential sources analysis indicated that Cd, Sb, and Zn mainly originated from agricultural, mining, and smelting activities; As, Cu, and Pb mainly originated from agricultural activities, while coal combustion by-products was another major source of these heavy metal(loid)s in paddy soils near the thermal power plant in the southwest corner of the study area; Cr, V, Mn, and Ni mainly originated from natural source. Conclusions Cadmium and Sb are the main contaminants in paddy soils in the study area, and there are hot-spot pollution areas.
✓ 已验证
产品关联
DOI
高影响因子
Polymers
·
2019
·Vol. 11
·期 8
·1297
·
IF 3.164
Yang Zhao,Xue Li,Zhongyang Wang,Xiaofeng Xie,Wei Qian
Novel proton exchange membranes (PEMs) based on graft copoly(arylene ether sulfone)s with enhanced phase-separated morphology were prepared using atom transfer radical polymerization (ATRP). A series of PEMs with different graft lengths and sulfonation degrees were prepared. The phase-separated morphologies were confirmed by transmission electron microscopy. Among the membranes prepared and evaluated, PAESPS18S2 exhibited considerably high proton conductivity (0.151 S/cm, 85 °C), benefitting from the graft polymer architecture and phase-separated morphology. The membranes also possessed excellent thermal and chemical stabilities. Highly conductive and stable copoly(arylene ether sulfone)-based membranes would be promising candidates as polymer electrolytes for fuel cell applications.Keywords:Poly(arylene ether sulfone)s;atom transfer radical polymerization (ATRP);proton exchange membrane (PEM);phase-separated morphology;fuel cell
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）