TALANTA
·
2022
·
IF 6.556
Yujie Shen,Mingcong Rong,Xiaodan Qu,Bolin Zhao,Jinhui Zou,Zhenbang Liu,Yu Bao,Ying He,Siyi Li,Xiaojin Wang,Meiyun Chen,Kaiying Chen,Yuwei Zhang,Li Niu
Detection of heavy metal ions (HMIs) in water is an important topic in the field of analytical chemistry and environmental science. Fluorescence spectroscopy is one of the most promising strategies due to its simple instrument, low investment, rapid and convenient operation. However, current fluorescence probes for detecting HMIs are typically selective for certain ions. Herein we reported the development of a novel strategy that determined the total content of HMIs in water by fluorescence spectroscopy. A novel fluorescent nitrogen, sulfur co-doped carbon quantum dots (N, S-CQDs) was prepared via graphene oxide-assisted synthesis method. The results showed that, with the fluorescence quenching strategy, N, S-CQDs exhibited a wide linear response to a series of water-soluble metal ions . The fluorescence of N, S-CQDs is stable in a wide range of pH 4–11. The detection mechanism was proved that the integration, caused by coordination interaction between S element in N, S-CQDs and the d-orbital of associated metal ions, was the main reason for fluorescence quenching . In practice, the N, S-CQDs were applied to determine total content of HMIs in water successfully. Interestingly, further experiment proved that the N, S-CQDs could effectively remove HMIs in water after centrifuging and filtering thoroughly. It was shown that the fluorescence of N, S-CQDs was obviously quenched by the multiple-ions-involved water and scavenging effect of N, S-CQDs on HMIs with centrifugal in which the concentration of individuals meets the Chinese National Standard. This indicates that the N, S-CQDs are of a wide application prospect in water quality analysis.
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高影响因子
ACS Applied Polymer Materials
·
2022
·
IF 4.855
Qichen Yin,Bowen Xu,Yao Qin,Jingbo Zhao,Jue Cheng,Junying Zhang
Diglycerol and dimer acid (DA) are used as precursors for the solvent- and catalyst-free synthesis of fully biobased non-isocyanate polyurethanes to replace toxic isocyanates and petroleum-based reactants. Linear polyhydroxy(amide-urethane)s (L-NIPHAUs) were synthesized via the melt aminolysis copolymerization between diglycerol dicarbonate (DGDC) and diamino-telechelicoligoamides (DAPAhs) from DA and hexamethylenediamine (HDA). By changing the DA/HDA molar ratios, the structures of DAPAhs and L-NIPHAUs were regulated in a simple and straightforward manner. Atomic force microscopy (AFM) and dynamic mechanical analysis (DMA) of the L-NIPHAUs reveal that the huge polarity difference between the hard segments (HSs) and soft segments (SSs) leads to nanophase separation. The N-amidohexylene-diglycerolbis(hydroxyurethane)-N′-amidohexylene and N-amido-hexylene-N′-amido segments form double HSs, while the bulky nonpolar DA residues serve as SSs. L-NIPHAUs also exhibit semicrystalline structures with good thermal stability evidenced by wide-angle X-ray scattering (WAXS), differential scanning calorimetry (DSC), and thermogravimetry analysis (TGA). They possess Tm ranging from 94 to 110 °C and tunable mechanical properties with a tensile strength of 7.3–12.1 MPa and strain at break of 311–858%. Introducing DA segments increases the hydrophobicity of L-NIPHAUs and the water contact angle and decreases the surface energy. L-NIPHAUs also show excellent solvent resistance in organic solvents, thanks to their intramolecular hydroxyurethane hydrogen bonding, three-dimensional inherent intermolecular hydrogen bonding networks, and the modification of bulky nonpolar DA SSs.
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CHINESE JOURNAL OF CATALYSIS
·
2022
·
IF 12.92
Yangrui Xu,Xiaodie Zhu,Huan Yan,Panpan Wang,Minshan Song,Changchang Ma,Ziran Chen,Jinyu Chu,Xinlin Liu,Ziyang Lu
The recyclable and stable ZnFe 2 O 4 small particle decorated one-dimensional perylene diimide (PDI) S-scheme heterojunction (1D PDI/ZnFe 2 O 4 ) is prepared by the hydrochloric acid-mediated (HCl-mediated) strategy, interestingly, the morphology of the 1D PDI/ZnFe 2 O 4 can also be effectively regulated by HCl-mediated process, the existence of HCl can regulate PDI into a uniform rod structure, while the co-existence of HCl and PDI can limit ZnFe 2 O 4 to become the uniform small particles. More importantly, based on the 1D rod structure of PDI and the small size effect of ZnFe 2 O 4 , carriers can migrate to the surface more easily, which can improve the photocatalytic activity. Meanwhile, due to the appropriate energy level structure, the S-scheme heterojunction structure is formed between PDI and ZnFe 2 O 4 , which eliminates meaningless photo-generated charge carriers through recombination and introduces strong redox to further enhance the photodegradation effect, thereby, 1D PDI/ZnFe 2 O 4 exhibits excellent photocatalytic ability, under the visible light irradiation, the degradation rate of tetracycline (TC) with 1D PDI/ZnFe 2 O 4 (66.67%) is 9.18 times that with PDI (7.26%) and 9.73 times that with ZnFe 2 O 4 (6.85%). This work proposes new ideas for the assembly of magnetic organic-inorganic S-scheme heterojunction photocatalysts.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Zengyue Chen,Yunfeng Li,Fei Tian,Xin Chen,Zhansheng Wu
In this work, a green reaction route for the preparation of BiVO 4 /g-C 3 N 4 composite is constructed using the acetic acid and reusable ethylene glycol system combined with the microwave method. The rice grain-like BiVO 4 is successfully deposited on the surface of hollow tubular g-C 3 N 4 to form a S-scheme heterojunction within 25 min. The performance of the prepared photocatalysts is evaluated by removing glyphosate, methyl orange and tetracycline hydrochloride from simulated agricultural and urban runoff. The degradation evaluation results show that acetic acid in this route could play a better induction role compared to the conventional inducer nitric acid, while the ethylene glycol in this route can be recycled. The recovery of ethylene glycol could reach more than 85%, and the performance of the produced photocatalyst will not be decreased after the recovery of ethylene glycol reaches 20 times. The BV/CN 60 -R 20 sample has the highest photocatalytic activity for glyphosate removal under simulated sunlight irradiation, which is 14.5 times and 9.7 times higher than that of pure BiVO 4 and g-C 3 N 4 , respectively. In summary, the establishment of the ethylene glycol and acetic acid system not only provides a new perspective for the replacement of strong acids in the preparation of BiVO 4 -based photocatalyst but also provides a reference for the construction of other harmless and recyclable systems.
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ANALYTICA CHIMICA ACTA
·
2022
·
IF 6.911
Kaisheng Hong,Youfang Huang,Lingxin Zheng,Xinyi Zheng,Xiaojia Huang
Efficient capture is an essential procedure in the highly sensitive monitoring of phenylurea herbicides (PUHs) in various environmental waters. Herein, a new poly (ionic liquid)s functionalized magnetic adsorbent (PFMA) was conveniently fabricated by means of “one-pot” strategy. The preparation procedure was quite simple by mixing 1-allyl-3-methylimidazoliumbis[(trifluoromethy)sulfonyl]imide, ethylene glycol dimethacrylate , Fe 3+ , Fe 2+ , mixed solution of dimethyl sulfoxide/H 2 O and azobisisobutyronitrile in one pot, and the total reaction time was just 3.0 h which was far shorter than that needed in previous approaches. A series of characterized techniques were employed to observe and inspect the morphology, structure and magnetic properties of prepared PFMA. Results revealed that the adsorbent contained abundant functional groups and superior magnetic property. Combing with magnetic solid-phase extraction (MSPE) format, the resultant PFMA displayed high capture capability towards studied PUHs through multiple interactions, and the enrichment factors were in the range of 126–227. Under the selected extraction parameters, the introduced PFMA/MSPE was combined with HPLC equipped with diode array detector (HPLC/DAD) to measure investigated PUHs at trace levels in various environmental waters. Wide linear range (0.010–200 μg/L), low limit of detection (0.0025–0.015 μg/L) and good precision (RSDs<10%) were achieved. The reliability and practicality of established approach was demonstrated by quantifying trace studied PUHs in various waters. Satisfactory fortified recoveries (80.2–119%) and repeatability were achieved. The results well evidence that the prepared PFMA is a good alternative for capture PUHs, and the introduced approach has wide prospect in the analyzing trace levels of PUHs in water and other complex samples.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Lingjie Zhang,Zhisheng Ke,Wenzhe Wang,Huiling Liu,Yuting Mao,Mingxue Xiang,Ping Zhang
In this study, an innovative sulfur-doped graphene-like carbon-supported layered double oxide (G/S-LDO) was developed for removing toxic heavy metal ions (HMIs; Pb(II), Cd(II), and Co(II)) that are frequently found in wastewater. In single-solute systems, the maximum adsorption capacities were 720.01 (Pb(II)), 473.11 (Cd(II)), and 170.91 (Co(II)) mg/g, which were significantly higher than that of pure LDO and other materials reported in the literature. Even in mixed systems, the outstanding adsorption performance of G/S-LDO toward HMIs was observed with high distribution coefficient values ( K d , > 100 L/g). We found that the excellent performance of G/S-LDO depended both on LDO and sulfur-doped graphene-like carbon (G/S) in a complicated manner. In detail, the released OH – from LDO as precipitate agent contributed to HMIs removal. Further, G/S enhanced the 35.42% Pb(II) adsorption, 58.19% for Cd(II) and 48.69% for Co(II) via the complexation and the cation-π interaction from graphene, and coordination and precipitation effect resulting from the doped S. Consistent with experimental results, density functional theory (DFT) calculations unveiled the essence of the enhancement by G/S, and showed that the orbital hybridization between S p and the HMIs p and d states electrons played an important role on HMIs removal. Finally, the recyclability and leaching experimental results suggested the high stability and reusability of G/S-LDO. This work provides new insights into the interactions of HMIs with G/S-based materials, which may facilitate the development of prospective HMIs capturing agents in future studies.
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ACS Applied Nano Materials
·
2022
·
IF 6.14
Wanying Lin,Biao Zhang,Jun Jiang,Enzuo Liu,Junwei Sha,Liying Ma
The design of transition metal dichalcogenides that satisfies the essential requirements of the hydrogen evolution reaction (HER) in alkaline solutions remains a challenge. The study gives a description of sulfur atoms into both anionic and cationic sites of WTe2, which is deliberately designed and has been rarely reported. Herein, we report 3D self-supported anionic and cationic S-substituted WTe2 nanosheet arrays constructed on a carbon cloth by a three-step synthesis method at elevated temperatures. Experimental and theoretical analysis are both executed to investigate S-WTe2/CC nanocomposites for efficient alkaline HER, and the results attest to its excellent electrocatalytic performance. The optimized S-WTe2/CC exhibits an enhanced HER activity with an overpotential of 195 mV at the current density of 10 mA cm–2, which is 2.3 and 1.7 times lower than that of WO3/CC (451 mV) and WTe2/CC (327 mV), respectively. According to density functional theory calculations, such improvement of alkaline HER is attributed to the optimized p-band electron configuration of Te atoms, higher H* intermediate adsorption, and lower H2O dissociation energy barrier by anionic and cationic co-substitution of S, which accelerate the Volmer–Heyrovsky process. The present study paves a way to the modification strategy of WTe2 electrocatalysts.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Qingwei Gao,Jing Ding,Guanshu Zhao,Qingliang Zhao,Lili Li,Xiaoshan Zhao,Lingjun Bu,Shiqing Zhou,Shan Qiu
Sulfate radical-based advanced oxidation processes had been widely applied in the water treatment. In this study, a novel solar-assisted electrooxidation process (SEOP) to activate peroxymonosulfate (PMS) or peroxydisulfate (PDS) was conducted for the degradation of bisphenol S (BPS). The SEOP with persulfate (PS) demonstrated its synergistic effect for BPS degradation, compared with the electrooxidation/PS and the solar process. The hydroxyl radical, sulfate radical ( SO 4 · - ), and singlet oxygen were regarded as primary active species in BPS degradation in SEOP with PS. The transition structure complex ( persulfate* ) on the anode promoted the efficiency of BPS degradation via the non-radical mechanism. The activation of PMS and PDS in SEOP was dominated through radical and non-radical mechanism, respectively. To effectively supplement experimental work with quantum chemical calculation, density function theory (DFT) showed that the active sites mainly focused on the phenol ring of BPS. The energy barrier calculation indicated that BPS was more susceptible to be attacked by SO 4 · - through electron transfer. BPS was mainly degraded by ring-opening, substitution, addition, C–C bond breaking, and decarboxylation reactions. Furthermore, the effective decrease in bio-toxicity of BPS intermediates in SEOP with PS was predicted. Experiments under various current densities, initial concentration of PS, electrolyte, and humic acid suggested the feasibility of SEOP with PS. BPS was degraded with lower energy consumption (0.18 kWh·m −3 ·order − 1 ) in SEOP with PMS than that in SEOP with PDS (0.30 kWh·m −3 ·order − 1 ) and without PS (0.38 kWh·m −3 order − 1 ), respectively. The SEOP with PS poses the feasible, convenient, and economic potential for the degradation of refractory pollutants.
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CHEMOSPHERE
·
2022
·
IF 8.943
Zhihong Li,Danquan Lan,Zuji Li,Jiangli Sun,Shuo Chen,Jinhang Yang,Jingwen Wei,Zebing Yu,Shuangfei Wang,Yanping Hou
Development of efficient photocatalysts for efficient recalcitrant organic pollutants degradation is of great significance. Herein, the step-doped disulfide vacancies S-scheme Cu 3 SnS 4 /L-BiOBr (CTS/L-BiOBr) heterojunction photocatalyst was prepared for ciprofloxacin (CIP) degradation. X-ray photoelectron spectroscopy (XPS) analysis, ultraviolet photo-electron spectroscopy (UPS) analysis, band structure and dominant radicals’ identification together verified that the transfer of photogenerated carriers conformed to the S-scheme mechanism. Benefited from the interfacial electric field (IEF) of the S-scheme heterojunction and incorporation of L-cysteine with introducing S-vacancies and surface functional groups (-NH 2 , -COO - ), photogenerated charges generation and separation of the CTS/L-BiOBr (10) were greatly improved. With ·OH and h + as dominant reactive species, CIP removal reached 93% using CTS/L-BiOBr (10) within 180 min of visible light irradiation, which was 3.5 times and 2.6 times of pristine Cu 3 SnS 4 and L-BiOBr, respectively. Moreover, possible CIP degradation pathways were proposed and the degradation intermediates ecotoxicity were evaluated. This study could provide reference for designing efficient S-scheme photocatalysts for recalcitrant wastewater treatment .
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JOURNAL OF CATALYSIS
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2022
·
IF 8.047
Songbo Wang,Pengjie Liu,Chengzhen Meng,Yidan Wang,Lei Zhang,Lun Pan,Zhen Yin,Na Tang,Ji-Jun Zou
Photoelectrochemical (PEC) water splitting is a promising approach to solve the current energy and environmental crises. Herein, we developed a “one stone, two birds” strategy to construct Au@Pt decorated ZnO/CdS heterojunctions (ZCAP) with Au-S bond and surface plasmon resonance (SPR) effect for promoted PEC water splitting. The optimized ZCAP structure exhibited the highest photocurrent density of 4.23 mA/cm 2 at 1.23 V vs. RHE and hydrogen evolution rate of 72.3 μmol·cm −2 ·h −1 , which is magnitude higher than pure ZnO. In-depth investigations indicate that SPR effect can afford hot electrons, whereas Au-S bonds over interface act as transmission bridge for facilitated electron transfer, the synergy of them achieves efficient charge separation and light utilization. Meanwhile, surface Pt nanoparticles serve as active sites for rapid charge transfer and promoted surface reaction. This article illustrates that the synergy of SPR and electron transfer bridge is an efficient strategy for promoted PEC performance.
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Batteries-Basel
·
2022
·Vol. 8
·期 10
·161
·
IF 5.938
Han Wang,Sidra Jamil,Wenwen Tang,Jing Zhao,Hui Liu,Shujuan Bao,Yijun Liu,Maowen Xu
Due to the high theoretical capacity of 1675 mAh g−1of sulfur, lithium-sulfur (Li-S) batteries can reach a high energy density of 2600 Wh kg−1, which has shown fascinating potential in recent decades. Herein, we report the spiderweb-like nanocage (Co/Mel) as a novel sulfur host with a melamine-sacrificed pyrolysis method. The incorporation of embedded cobalt nanoparticles (Co NPs) in the tips of carbon nanotubes (CNTs) can catalyze polysulfide transformation kinetics. In addition, the nanocages form a conductive three-dimensional spiderweb-like network that facilitates electrolytic penetration and electronic/ionic transportation. Moreover, the porous internal nano-cavities not only improve sulfur loading levels but also provide buffer space for volume expansion during charging and discharging. As a result, the hollow Co/Mel polyhedra with a high content of sulfur (75.5 wt%) displays outstanding electrochemical performance with an initial discharge-specific capacity of 1425.2 mAh g−1at 0.1 C and a low decay rate of only 0.028% after 1000 cycles at 1 C.Keywords:lithium-sulfur batteries;pyrolytic synthesis;zeolite imidazolate framework;spiderweb-like nanocages;catalytic conversion
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EUROPEAN POLYMER JOURNAL
·
2022
·
IF 5.546
Ge Zhu,Haoji Lao,Feng Feng,Minyan Wang,Xingzhong Fang,Guofei Chen
Two series of poly(amide imide)s (PAIs) based on two novel isomeric amide-containing diamine monomers and different commercial aromatic dianhydrides were synthesized via thermal imidization. These PAIs exhibited excellent T g s ranging from 368 to 431 °C, low coefficients of thermal expansion (CTE) of 6.7–47.2 ppm/K, and good 5% weight loss temperatures ( T d5% s) in N 2 of 494–540 °C, which was attributed to the introduction of rigid backbone and strong intermolecular hydrogen bonding resulted from amide bond. In particular, PAI-1a and PAI-1b displayed well-balanced performance with T g s in the range of 419–431 °C, CTE in the range of 6.7–9.0 ppm/K, and mechanical properties with tensile strengths of 116–125 MPa, tensile moduli of 8.4–8.7 GPa, which could be probably used in flexible displays. In addition, the effects of two isomeric monomers on the properties of films were compared, and it was found that PAI-(1 – 3)a showed higher T g, T d5% and CTE, but lower tensile strength and transparency than PAI-(1 – 3)b .
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危险品化学品经营许可证（带存储）