Biomaterials Science
·
2023
·Vol. 11
·期 10
·3589-3602
·
IF 6.6
Bo Huang,Wei Guan,Chaofeng Wang,Shuilin Wu,Zhenduo Cui,Yufeng Zheng,Zhaoyang Li,Shengli Zhu,Hui Jiang,Paul K. Chu,Xiangmei Liu
Charge transfer and separation play a critical role in the photocatalytic efficiency of photoresponsive materials and their subsequent applications. Herein, for the first time, we constructed a homo-heterostructured S–Cu–FC/CuS modified carboxymethyl cellulose (CMC) hydrogel doped with graphene oxide (GO) (S–Cu–FC/CuS/GO@CMC) through an in situ ionic complexation reaction, which exhibited enhanced photocatalytic performance under 808 nm near-infrared (NIR) light irradiation. On the one hand, photo-excited charges can rapidly transfer across the homo-heterojunction interface with copper atoms in S–Cu–FC/CuS as both donors and acceptors. On the other hand, the interface between GO and S–Cu–FC/CuS also favors the fast transfer of photogenerated charges. Hence, with the assistance of a photothermal effect, the enhanced photocatalytic performance of S–Cu–FC/CuS/GO endowed the hydrogel with robust sterilization ability for killing 99.5% S. aureus and 100.0% E. coli under 10 min NIR light irradiation. An in vivo test disclosed that this hydrogel could also accelerate the healing of bacteria-infected wounds.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Changhao Bian,Yanyan Wang,Yuyan Yi,Shengyu Shao,Pengfei Sun,Yingping Xiao,Wen Wang,Xiaoping Dong
For the past few years, graphitic carbon nitride (g-C 3 N 4 ) has been widely used to eliminate environmental pollutants, but limited active site on surface and low separation/migration ability suppress its practical uses. Herein, we adopted a supramolecular self-assembly route followed with S doping to synthesize S-doped g-C 3 N 4 with a hollow microsphere composition (SCNHM), where the shell was demonstrated to compose of ultrathin nanosheets. The unique structural characteristics endow the SCNHM with high specific surface area (∼81 m 2 g −1 ) to provide abundant reaction sites and enhanced light-harvesting due to the light-scattering effect of hollow structure. Moreover, the S dopant meliorated the electronic structure to narrow the bandgap and promoted the charge separation/transfer capability. With this synergistic effect, the SCNHM presented greatly improved photocatalytic activity for degrading tetracycline hydrochloride (TC) compared to the CN, SCN and CNHM samples. This photocatalyst could eliminate high-concentration TC (50 mg L −1 ) in 18 min, and the 30 min removal efficiencies of 100 mg L −1 and 200 mg L −1 reached 92 % and 60 %, which is much better than the reported photocatalysts in literatures (usually ≤ 20 mg L −1 ). Additionally, the good photocatalytic durability was confirmed and the degradation pathway of TC was proposed. Furthermore, the SCNHM was proved to meanwhile possess superior performance for inactivating the typical Gram-positive bacterium of Staphylococcus aureus ( S. aureus ) and the typical Gram-negative bacterium of Escherichia coli ( E. coli ). Finally, based on determination of band alignment and detection of active species, a plausible photocatalytic mechanism was proposed.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Jing Chen,Chunyang Bao,Mengshi Chen,Yan Wang,Xiaoling Xu,Tao Yang,Cenyao Shang,Qiang Zhang
The design of highly rapid and efficient cross-linked polymer materials is essential for developing adsorption of pollutant methods based on cyclodextrin to replace currently used slow trapping activated carbons. It is rarely possible to achieve rapid and complete adsorption at high concentrations, even though available adsorbents have developed high adsorption capacity. Herein, a beta-cyclodextrin cross-linked poly(ionic liquid) adsorbents (CD-PILs), was facilely fabricated through one-pot radical polymerization for fast, high-capacity and selective removal of pollutants from water, including organic dyes, pharmaceutical and personal care products, heavy metal ions as well as microbial contamination. It could be completely removed from water within a short period ranging from seconds to minutes at a wide range of high-load anionic dyes (1 mM). Theoretical maximum adsorption capacity of CD-PILs for CR, MO, DS, SD, K 2 Cr 2 O 7 , and CA is 2058.2, 1338.6, 903.7, 1661.4, 878.2, and 343.6 mg/g, respectively. The adsorption rate of ionic CD-PILs superior than those of most of reported synthetic adsorbent materials with the highest adsorption capacity so far, especially for heavy metals. Moreover, after being regenerated five times, the water-remediation performance of CD-PILs remained almost the same as fresh ones, demonstrating the great potential of CD-PILs in industrial water remediation.
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Nanomaterials
·
2023
·Vol. 13
·期 5
·830
·
IF 5.3
Yang Yu,Fengjuan Chen,Xuekun Jin,Junyong Min,Haiming Duan,Jin Li,Zhaofeng Wu,Biaobing Cao
Recently, the use of semiconductor-based photocatalytic technology as an effective way to mitigate the environmental crisis attracted considerable interest. Here, the S-scheme BiOBr/CdS heterojunction with abundant oxygen vacancies (Vo-BiOBr/CdS) was prepared by the solvothermal method using ethylene glycol as a solvent. The photocatalytic activity of the heterojunction was investigated by degrading rhodamine B (RhB) and methylene blue (MB) under 5 W light-emitting diode (LED) light. Notably, the degradation rate of RhB and MB reached 97% and 93% in 60 min, respectively, which were better than that of BiOBr, CdS, and BiOBr/CdS. It was due to the construction of the heterojunction and the introduction of Vo, which facilitated the spatial separation of carriers and enhanced the visible-light harvest. The radical trapping experiment suggested that superoxide radicals (·O2−) acted as the main active species. Based on valence balance spectra, Mott-Schottky(M-S) spectra, and DFT theoretical calculations, the photocatalytic mechanism of the S-scheme heterojunction was proposed. This research provides a novel strategy for designing efficient photocatalysts by constructing S-scheme heterojunctions and introducing oxygen vacancies for solving environmental pollution.Keywords:BiOBr;CdS;oxygen vacancy;S-scheme;photocatalysis
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APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Fang Chen,JiaYu Liao,Xuan Lu,YuZhi Xu,XiaoHuan Jiang,Mengkui Tian
Exploring efficient and stable water-splitting photocatalysts is critical for realizing conversion solar energy into hydrogen energy. Herein, a unique 2D/2D S-scheme Cd 0.5 Zn 0.5 S/CuInS 2 heterojunction with sulfur vacancies was rationally designed by chemically converting inorganic–organic hybrid ZnS(en) 0.5 into inorganic Cd 0.5 Zn 0.5 S nanosheets and fabricating with CuInS 2 at 350 °C under an N 2 atmosphere. The final Cd 0.5 Zn 0.5 S/CuInS 2 photocatalyst was composed of thin nanosheets with a substantial interfacial contact area, which enhanced light absorption and allowed directional charge transfer and separation. Under visible light irradiation, the photocatalytic H 2 evolution activities of Cd 0.5 Zn 0.5 S nanosheets is 0.79 mmol·g −1 ·h −1 , which is greater than other solid solution materials obtained by varying Cd and Zn ratios. The 2D/2D nanosheets with 8% CuInS 2 exhibit excellent hydrogen evolution activity with yields of 7.73 mmol·g −1 ·h −1 , which are 9.8 and 138 times higher than Cd 0.5 Zn 0.5 S and CuInS 2 . In addition, Cd 0.5 Zn 0.5 S/CuInS 2 photocatalyst demonstrates outstanding stability and activity over the course of 24-hour period. Moreover, the transfer pathway of photogenerated charges were explored by the energy band bending, which proved that an S-scheme heterojunction is synthesized successfully.This work offers a useful methodology for analyzing S-scheme heterojunction with abundant sulfur vacancies, and improving the solar hydrogen evolution performance of Cd 0.5 Zn 0.5 S photocatalyst.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Junjie Fu,Afei Zhang,Dongxing Kou,Zewen Xiao,Wenhui Zhou,Zhengji Zhou,Shengjie Yuan,Yafang Qi,Zhi Zheng,Sixin Wu
One important issue limiting the development of Cu 2 ZnSn(S,Se) 4 (CZTSSe) solar cells is the severe recombination loss at CZTSSe/Mo(S,Se) 2 /Mo back contact, primarily arising from the non-matched potential barrier and inferior electric contact between absorber and weak n -type Mo(S,Se) 2 interfacial layer. It is expected that a p-type Mo(S,Se) 2 can effectively improve the hole extraction and enhance the device performance. In this work, we propose a plausible direction to build up an electrically benign back surface field by in-situ doping Mo(S,Se) 2 with group VB elements (TM = V, Nb and Ta). It is turned out that the generated V Mo , Nb Mo , or Ta Mo shallow acceptors could convert Mo(S,Se) 2 from weak n -type to p-type conductivity and increase its work function ( W F ) and hole concentration. With the contact of p-type absorber ( W F,absorber < W F,Mo(S,Se)₂ ), a benign ohmic contact with favorable downward band bending is formed, thereby accelerating the holes extraction and minimizing interface recombination loss. With significant gains in open-circuit voltage ( V oc ) and fill factor (FF), the Mo(S,Se) 2 :Ta device finally increases the efficiency from 10.82 % to 12.72 %. This convenient in-situ Mo(S,Se) 2 doping strategy is different from previous complicated or unstable cases and should serve as a basis for high-quality back contact engineering in kesterite photovoltaics.
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POLYMER
·
2019
·
IF 3.771
Zhengfang Zhu,Peng Cui,Yu Lu,Jianrong Wu,Jing Zeng,Weiye Ma,Xinsheng Zhao,Yuanqin Zhu
To develop a facile route towards anion conductive polymers containing multi-cation side chains, novel anion conductive poly (2,6-dimethylphenylene oxide)s (DQPPO-x-I) was prepared from a clickable di-quaternized side-chain precursor, via Cu(I)-catalyzed azide-alkyne click chemistry. The new precursor was synthesized from commercially available 2-{[2-(dimethylamino)ethyl]methylamino}ethanol and 3-bromopropyne via nucleophilic substitution and Menshutkin reaction . The chemical structures of the precursor and DQPPO-x-I polymers were characterized by 1 H NMR and FT-IR. Small angle X-ray scattering and transmission electron microscopy revealed that the obvious micro-phase separation was formed in the DQPPO-x-I membranes. The optimized DQPPO-19-OH membrane with ion exchange capacity of 2.13 meq./g exhibited the highest hydroxide conductivity of 31.6 mS/cm at 80 °C, tensile strength of 64 MPa, and thermal stability (onset decomposition temperature up to 187 °C).
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DALTON TRANSACTIONS
·
2019
·Vol. 48
·期 6
·2077-2085
·
IF 4.052
Jie He,Shanshan Sun,Zhao Zhou,Qipeng Yuan,Yanhui Liu,Hao Liang
A novel magnetic responsive Ni-based metal–organic framework material was developed to efficiently separate and immobilize thermal enzymes with high catalytic performance. Ni-based metal–organic framework nanorods (Fe3O4/Ni-BTC) with high magnetic responsiveness are prepared conveniently by a one-pot hydrothermal process. With the characterization, it was confirmed that Ni-based metal–organic framework nanocomposites were synthesized as nanorods mounted with magnetic Fe3O4 nanoparticles on the surface. Although Fe3O4/Ni-BTC showed a preference for histidine-tagged enhanced green fluorescent protein (His-eGFP), we found that a variety of forces played roles in enzyme immobilization, including affinity between Ni2+ and histidine tags, electrostatic attraction, hydrogen bonding and hydrophobic forces. After understanding the mechanism of the as-prepared nanocomposites, a new immobilization strategy for thermostable S-adenosylmethionine synthetase (SAMS) was further evaluated. As a result, SAMS from cell lysate achieved about 95% activity recovery in the biosynthesis of S-adenosylmethionine (SAM) under high temperature conditions (70 °C) with a simple mixing step. At the same time, the immobilized enzyme was more stable against temperature variation (by nearly 8-fold in an 80 °C water bath after 2 h) and extreme pH (by nearly 1.3-fold at pH 3) and exhibited excellent reusability after immobilization. This work indicates that magnetic responsive Ni-based nanorods are highly promising for thermostable enzyme immobilization with high efficiency and stability.
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Polymers
·
2018
·Vol. 10
·期 11
·1287
·
IF 2.935
Wenmeng Zhang,Shaoyun Chen,Dongyang Chen,Zhuoliang Ye
Sterically hindered (S)-1,1′-binaphthyl-2,2′-diol had been successfully copolymerized with 4,4′-sulfonyldiphenol and 4,4′-difluorobenzophenone to yield fibrous poly(arylene ether ketone)s (PAEKs) containing various amounts of binaphthyl unit, which was then selectively and efficiently sulfonated using ClSO3H to yield sulfonated poly(arylene ether ketone)s (SPAEKs) with ion exchange capacities (IECs) ranging from 1.40 to 1.89 mmol·g−1. The chemical structures of the polymers were confirmed by 2D1H–1H COSY NMR and FT-IR. The thermal properties, water uptake, swelling ratio, proton conductivity, oxidative stability and mechanical properties of SPAEKs were investigated in detail. It was found that the conjugated but non-coplanar structure of binaphthyl unit endorsed excellent solubility and film-forming capability to SPAEKs. The SPAEK-50 with an IEC of 1.89 mmol·g−1exhibited a proton conductivity of 102 mS·cm−1at 30 °C, much higher than that of the state-of-the-art Nafion N212 membrane and those of many previously reported aromatic analogs, which may be attributed to the likely large intrinsic free volume of SPAEKs created by the highly twisted chain structures and the desirable microscopic morphology. Along with the remarkable water affinity, thermal stabilities and mechanical properties, the SPAEKs were demonstrated to be promising proton exchange membrane (PEM) candidates for potential membrane separations.Keywords:proton exchange membranes;condensation polymerization;post-sulfonation;binaphthyl;film-forming capability
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NEW JOURNAL OF CHEMISTRY
·
2018
·Vol. 42
·期 24
·20180-20189
·
IF 3.201
Jinping Song,Qi Ma,Sufang Zhang,Huijun Liu,Yong Guo,Feng Feng
In this paper, we reported a facile approach for the preparation of sulfur and nitrogen co-doped carbon nanoparticles (S,N-CNPs) with strong blue luminescence, which exhibited multiple applications including metal ion detection, logic gate fabrication and bioimaging. S,N-CNPs were synthesized by one-step hydrothermal treatment of formamidine sulfinic acid (FAS) and ethylene glycol. The as-synthesized S,N-CNPs possess a high quantum yield (Φ = 69.04%) and display excellent photostability and storage stability. By modulating the pH environment, S,N-CNPs were successfully applied as fluorescent probes for the detection of three kinds of heavy metal ions (Hg2+, Ag+ and Ni2+). The fabricated fluorescence sensors display ultrahigh sensitivity and a wider signal response range. More importantly, ethylenediamine (or ammonium thioglycolate and glycine) could efficiently release Hg2+ (or Ag+ and Ni2+) from the S,N-CNP surface, leading to the recovery of the fluorescence. According to this phenomenon, interesting implication (IMP) logic gates were constructed. In addition, the S,N-CNPs exhibited low toxicity, good biocompatibility and easy cellular uptake behavior. Consequently, the obtained S,N-CNPs will have potential applications in multiple fields of environmental monitoring, logic gate operation, and cell bioimaging.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2019
·
IF 6.393
Cheng Li,Yu Chen,Lijun Yang,Congrou Zhang,Bin Wang,Yong Wang
“Turn-on” fluorescent materials in the absence of metal and organic solvent are highly desirable as bioprobes to selectively and sensitively detect pyrophosphate (PPi) anion. In this work, we embedded tetraphenylethene (TPE) inside the relatively rigid hyperbranched poly(amido amine) (HPA) to afford highly water soluble TPE-HPA materials, where the TPE fluorescence was pre-quenched in water by the hyperbranched structure of HPA without participation of any metal or organic solvents. The obtained TPE-HPA could be directly used as fluorescence “turn-on” bioprobe under physiological conditions to selectively detect PPi. There was a good linearity between the photoluminescence enhancement and the PPi concentration in the range of 0–1.0 μM with a limit of detection (LOD) of 6.5 nM. Compared with the other reported AIE probes for PPi detection, TPE-HPA with the optimal TPE content showed the best comprehensive performance, that is metal-free, organic-solvent free and nanomolar level LOD. The extreme selectivity and sensitivity towards PPi allowed TPE-HPA to accurately detect the PPi concentration in human urine.
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NEW JOURNAL OF CHEMISTRY
·
2019
·Vol. 43
·期 6
·2790-2796
·
IF 3.069
Xiuxiu Zhao,Xin Lin,Jianhua Wang,Xuwei Chen
Nitrogen and sulfur co-doped graphene oxide nanosheets (N,S-GO) were prepared via a facile one-step solvent-free approach using citric acid as a precursor and cysteine as a dopant. First, the graphene nucleus was formed via intermolecular dehydration of citric acid; N and S were then incorporated into the graphene structure by attacking the margin of the graphene nucleus. Crosslinking among the graphene nucleus via intermolecular condensation led to the final N,S-GO. The latter exhibited favorable photoluminescence behaviors, such as a high fluorescent quantum yield of 56.0%, excellent photoluminescence stability within the pH range 5–12, and high tolerance to external ionic strength ≤1.0 mol L−1 NaCl. The fluorescence energy transfer between AgNPs and N,S-GO could induce efficient quenching of N,S-GO fluorescence, and the presence of biothiols in the system restored fluorescence effectively, so a fluorescence “off–on” procedure was developed for quantitative detection of biothiols. Under optimal conditions, the limit of detection for cysteine (Cys), homocysteine (Hcy) and glutathione (GSH) was 11.8, 4.9, and 7.3 nmol L−1, respectively. This sensing platform exhibited good selectivity toward biothiols in the presence of other amino acids. The practicability of this sensing platform was well demonstrated by determining biothiol content in human plasma samples, which revealed spiking recoveries of 97.10–101.50% with Cys.
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