Chemical Science
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2023
·Vol. 15
·期 2
·726-735
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IF 8.4
Rong Zhang,Jiajing Lan,Fei Wang,Shumei Chen,Jian Zhang
In this study, we synthesized multi-nuclear indium oxide clusters (InOCs) using 1,1′-ferrocene dicarboxylic acid (H2FcDCA) as the chelating and surface protection ligand. The obtained clusters include the cubane-type heptanuclear InOCs ([In7]) and the sandwich-type thirteen-nuclear InOCs ([In13]). Notably, [In13] represents the highest nuclear number reported within the InOC family. In addition, the presence of labile coordination sites in these clusters allowed for structural modification and self-assembly. A series of [In7] clusters with adjustable band gaps have been obtained and the self-assembly of [In7] clusters resulted in the formation of an Fe-doped dimer, [Fe2In12], and an imidazole-bridged tetramer, [In28]. Similarly, in the case of [In13] clusters, the coordinated water molecules could be replaced by imidazole, methylimidazole, and even a bridged carboxylic acid, allowing the construction of one-dimensional extended structures. Additionally, part of the H2FcDCA could be substituted by pyrazole. This flexibility in replacing solvent molecules offered diverse possibilities for tailoring the properties and structures of the InOCs to suit specific applications.
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Materials Today Bio
·
2023
·
IF 8.2
Anning Chen,Zhengao Wang,Hailun Chen,Bo Pang,He Cai,Ziheng Chen,Chengyun Ning,Dong Ma,Jie Tang,Hongzheng Zhang
The cochlear implant (CI), an advanced electronic device replacing the entire cochlear function, is the ultimate treatment for over 466 million people with disabling hearing loss. Infection after cochlear implantation is a common and worrisome complication despite the routine administration of the antibiotic. The bacterial biofilms formed on the surface of CI are the main cause of antibiotic failure. To solve this problem, we developed a copper-containing zwitterionic coating consisting of anti-adherent poly sulfobetaine methacrylate (PSB) and steadfast polydopamine (PDA). CuSO 4 /H 2 O 2. was added to accelerate this co-deposition reaction and enhance the anti-bacterial property. The preparation method was simple, rapid, and suitable for clinical use. In our in vitro and in vivo studies, the PSB/PDA(Cu) coating showed high biocompatibility, and conferred CI implants excellent anti-inflammatory, strong anti-bacterial effects, and great anti-biofilm properties to representative Gram-positive and Gram-negative bacteria. These findings implied that the PSB/PDA(Cu) coating was a unique anti-bacterial strategy for enhancing CI performance.
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INORGANIC CHEMISTRY COMMUNICATIONS
·
2023
·
IF 3.8
Wei Zhang,Hu Wang,Chao Ding,Yizhu Lei,Chaochuang Yin,Renshu Wang,Qiming Yang,Tingting Wu,Mei Zhang
Three mononuclear Cu(II) complexes, [Cu(C 16 H 12 NO 3 F)(H 2 O)] ( C1 ), [Cu(C 16 H 12 NO 3 F)(C 10 H 9 N 3 )]·H 2 O·0.5CH 3 OH ( C2 ) and [Cu(C 16 H 12 NO 3 F)(C 3 H 4 N 2 )] ( C3 ) with a fluorinated Schiff base ligand (C 16 H 12 NO 3 F = 5-fluorosalicylaldehyde-L-phenylalanine) and different secondary ligands (C 10 H 9 N 3 = 2,2′-dipyridylamine; C 3 H 4 N 2 = imidazole) were synthesized and structurally characterized. Theoretical calculation of the three complexes was carried out by density functional theory (DFT) Becke's three-parameter hybrid (B3LYP) method using the Gaussian 09 package. The calculation results are in accordance with experimental results. In addition, the inhibitory activities of C1 - C3 were tested in vitro against jack bean urease. At the same time, molecular docking was investigated to determine the probable binding mode. The experimental values and docking simulation exhibited that C1 showed strong inhibitory activity (IC 50 = 0.68 ± 0.09 μM) compared with the positive reference acetohydroxamic acid (IC 50 = 27.73 ± 2.93 μM). Moreover, a 100-ns molecular dynamics (MD) simulation was performed to evaluate the stability of urease (PDB ID: 3LA4) and the binding stability of the 3LA4 /C1 and 3LA4/ C3 using the Desmond 2021 from Schrödinger. Their structure-inhibitory activity relationship was further discussed from the perspective of molecular docking, theoretical calculation and molecular dynamics simulation.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Qianqian Chen,Meng Zhou,Jun Yuan,Jiaqian Cai,Hongxia Xie,Mengxiang Zhu,Libing Cai,Peng Wei,Chunyu Chang
To alleviate the dilemma of plastic recycling, the development of sustainable bioplastics that are compatible with the environment throughout the whole material life cycle has received widespread attention. We report a vacuum-assisted filtration method for preparation of high-strength bioplastic films made from hydrophobic cellulose nanofibers that were obtained by esterification of natural cellulose with dodecenylsuccinic anhydride in recyclable deep eutectic solvent (triethylmethylammonium chloride/imidazole). The tensile strengths of the resultant hydrophobic films were 150.8 MPa and 94.8 MPa under dry and humid conditions, respectively. Importantly, these films could be programmed into various shapes, such as “U” shaped bracket, helix, and ring via a hydrosetting method and the strong hydrogen bonding interactions between cellulose nanofibers contributed to shape fixation. Benefiting from their hydroplastic properties, various shapes of bioplastic films could be reversibly engineered by kirigami, origami, and embossing. Meanwhile, the disposal of waste films followed the recycling route to regain hydrophobic cellulose nanofibers. This work provided a facile approach for the preparation of high-strength and recyclable hydroplastic cellulose nanofiber films.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
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IF 4.2
Hujian Wu,Qi Wang,Xiaoxin Zhang,Tao Wang
Alkyl anthraquinones play a crucial role as chemical raw materials in the production of hydrogen peroxide as well as intermediates for the synthesis of drugs and dyes. This study focuses on investigating the oxidation reaction of 2,6-di-tert-butylanthracene with hydrogen peroxide, employing Bronsted acidic ionic liquids as catalysts. The optimization of both the anion and cation components within the Brønsted acidic ionic iquids was carried out, revealing that bis(3-propanesulfonic acid-1-imidazole)propylidene bisulfate ([2(Im-PS)-C3][2HSO4]) exhibited the most effective catalytic performance. Furthermore, the Brønsted acidic ionic liquids demonstrated cyclic catalytic activity during the oxidation reaction. Successful preparation of 2,6-di-tert-butylanthraquinone was achieved with a remarkable yield of up to 92%. The recyclability of the ionic liquid suggests that this study will contribute to technical improvements in the original method while concurrently reducing the cost associated with the synthesis of alkyl anthraquinones via the oxidation method.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Xi Chen,Yunfeng Chen,Songrong Li,Cheng Xue,Dongfang Liu,Wenli Huang
Phthalic acid esters (PAEs) pose serious health risks to humans and are difficult to remove by conventional sewage treatment processes. Herein, Fe 2 Mo 3 O 8 /MoO 2 /Mo 2 N composite (FMON) derived from bimetallic organic framework was used to activate peroxymonosulfate (PMS) for dibutyl phthalate (DBP) degradation. FMON exhibited an excellent catalytic effect with DBP removal efficiency of 92.4 % within 60 min. Mo 2 N showed a superior ability in promoting Fe 3+ /Fe 2+ redox cycle. The reduction efficiencies of Fe 3+ by Mo 2 N/MoO 2 composite and MoO 2 were 67 %–94 % and 11 %–23 %, respectively, in the homogeneous comparative experiment. Moreover, the ratio of Fe 2+ /Fe 3+ in FMON increased significantly after the catalytic reaction. Fe element doping also enhanced the reuse stability and reduced the metal ion leaching of the catalyst. The degradation of DBP was mediated by a variety of reactive species, of which SO 4 − , OH and O 2 − were dominant. Fe element, Mo element and O vacancies were confirmed to exert significant contributions as active sites in the catalytic process. Three degradation pathways of DBP were obtained by DFT calculation and HPLC-MS analysis. And the toxicity of DBP degradation products was significantly reduced based on the assessment result of Toxicity Estimation Software Tool (T.E.S.T.). This study explored a novel Fe/Mo bimetallic catalyst with friendly Fe 3+ /Fe 2+ cycling for environmental catalysis and provided new ideas for the treatment of PAEs wastewater.
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ACS Sustainable Chemistry & Engineering
·
2023
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IF 8.4
Zhipeng Wang,Junkai Wang,Shaorun Zhu,Tingting Ma,Mei Zhang,Min Guo
Chemical passivation serves as a highly effective strategy for mitigating defects to obtain efficient and stable perovskite solar cells. However, concerns about the stability and environmental-friendliness of molecular modulators have emerged with regard to the passivation effect. In this article, we introduce a judicious hydrogen bond network (HBN) composed of imidazole (ImA) and salicylic acid (SA) to address this issue. The ImA-SA HBN features multiple functional groups (amino and carboxyl) that simultaneously passivate various defects, including I– vacancies and uncoordinated Pb2+ ions located at grain boundaries and surfaces of the perovskite films. Remarkably, the ImA-SA HBN effectively bridges perovskite grains and interfaces between the perovskite films and hole transport materials, which enhances the transport of photogenerated carriers. Moreover, cyclic ImA-SA, characterized by steric hindrance, inhibits ion migration derived from grain boundaries of the perovskite films. Consequently, the efficiency of the champion device processed in fully ambient air exceeded 21% and did not decline obviously after 3380 h of storage in the air environment (20 ± 5 °C, 30 ± 5% RH, and without encapsulation). This work offers a promising approach to diminishing the defects in perovskite grain boundaries and surfaces, enhancing optoelectronic properties and facilitating the creation of efficient and stable perovskite solar cells processed in fully ambient air.
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Gels
·
2023
·Vol. 9
·期 9
·725
·
IF 4.6
Lisong Hu,Shishuai Gao,Lihui Zhao,Lili Dai,Daihui Zhang,Chunpeng Wang,Xuezhi Fang,Fuxiang Chu
Hydrogels containing renewable resources, such as hemicellulose, have received a lot of attention owing to their softness and electrical conductivity which could be applied in soft devices and wearable equipment. However, traditional hemicellulose-based hydrogels generally exhibit poor electrical conductivity and suffer from freezing at lower temperatures owing to the presence of a lot of water. In this study, we dissolved hemicellulose by employing deep eutectic solvents (DESs), which were prepared by mixing choline chloride and imidazole. In addition, hemicellulose-based DES hydrogels were fabricated via photo-initiated reactions of acrylamide and hemicellulose withN,N′-Methylenebisacrylamide as a crosslinking agent. The produced hydrogels demonstrated high electrical conductivity and anti-freezing properties. The conductivity of the hydrogels was 2.13 S/m at room temperature and 1.97 S/m at −29 °C. The hydrogel’s freezing point was measured by differential scanning calorimetry (DSC) to be −47.78 °C. Furthermore, the hemicellulose-based DES hydrogels can function as a dependable and sensitive strain sensor for monitoring a variety of human activities.Keywords:hemicellulose;deep eutectic solvents (DESs);anti-freezing;conductivity;hydrogels
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Wenting Li,Hanjie Zhang,Sijie Huang,Jingyi Xu,Liping Liu,Junshan Li,Jianfang Jing,Yongfa Zhu
The efficient activation of peroxydisulfate (PDS) for wastewater treatment remains a great challenge. Photocatalysis, which generates highly-reactive electrons and holes, shows great potential in activating PDS for effective degradation and deep mineralization. Herein, an electron-enriched PDI-SiO 2 photocatalyst was synthesized by covalently linking 3,4,9,10-perylene tetracarboxylic dianhydride (PTCDA) onto silicon dioxide (SiO 2 ) to form π-π stacked supramolecular PDI layers for efficient PDS activation. The highly dispersed PDI generates electron-enriched PDI· - under visible light, promoting the rapid activation of PDS for bisphenol A (BPA) degradation. The PDI-SiO 2 activated PDS system realized a high BPA degradation rate of 0.100 min −1 and a remarkable mineralization rate of 81%. Moreover, the charge separation efficiency is significantly improved since the electrons of PDI· - are captured by PDS, boosting oxidative degradation and improving the mineralization efficiency. This work developed a novel PDS activation strategy by constructing electron-enriched photocatalyst, and revealed the mechanism of photocatalytic activation and deep mineralization.
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JOURNAL OF CHROMATOGRAPHY A
·
2023
·
IF 4.1
Ya-Qi Zhao,Shi-Song Yu,Meng-Ying Chen,Yuan Wang,Yu-Jun Shi,Xin-Yu Wang,Jia-Meng Zhao,Lin-Yi Dong,Zhen-Yu Zhao,Xian-Hua Wang
Developing high-performance magnetic particles for the effective separation and purification of target proteins has become an important topic in the area of biomedical research. In this work, a simple and novel strategy was proposed for fabricating magnetic Fe3O4@agarose-iminodiacetic acid-Ni microspheres (MAIN), which can efficiently and selectively isolate histidine-tagged/rich proteins (His-proteins). Based on the thermoreversible sol-gel transition of agarose , basic magnetic agarose microspheres were prepared through the inverse emulsion method, in which the emulsion contained agarose and amine-modified Fe 3 O 4 nanoparticles. The size of the emulsion was controlled by the emulsification of a high-speed shear machine, which improved the specific surface area of MAIN. Subsequently, the amine-modified Fe 3 O 4 nanoparticles were covalently crosslinked with agarose through epichlorohydrin, which could avoid leakage of the magnetic source during use and increase the stability of MAIN. The microsized MAIN exhibited a clearly visible spherical core-shell structure with a diameter range from 3.4 μm to 9.8 μm, and excellent suspension ability in aqueous solution. The maximum adsorption capacity of MAIN for histidine-rich bovine hemoglobin was 1069.2 mg g −1 at 35 °C, which was higher than those of commercialized and most reported magnetic agarose microspheres/nanoparticles. The MAIN showed excellent adsorption ability and selectivity toward His-proteins in a mixture of histidine-rich bovine serum albumin (BSA) and histidine-poor lysozyme (LYZ). When the amount of LYZ was 5-fold higher than that of BSA, the recovery of BSA reached 75.0%. To prove its practicability, MAIN was successfully employed for the enrichment of histidine-tagged RSV-F0 from the cell culture medium supernatant. According to the optimized conditions, MAIN could enrich approximately 0.1 mg of RSV-F0 from 1 mL of complex biological sample. Therefore, we believe that the novel MAIN could be applicable for efficient separation and purification of His-proteins from complex biological systems.
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JOURNAL OF THE AMERICAN CERAMIC SOCIETY
·
2023
·
IF 3.9
Xuejiao Wang,Guangguang Pi,Jianye Yang,Kai Wu,Yanshuo Li,Wei Fang
Developing a highly active and stable electrode with a controllable size is greatly demanded to satisfy the large-scale application of electrochemical hydrogen production via water splitting. To overcome this challenge, a novel binder-free membrane electrode comprising Pd anchored on ZIF-62 glass supported on a porous TiC substrate has been developed to catalyze the hydrogen evolution reaction (HER) in both acidic and alkaline conditions. The optimal Pd@ZIF-62/TiC membrane electrode only requires a stable overpotential of ∼90 mV to reach a current density of 30 mA cm −2 within 20 h of operation. The outstanding HER performance of such electrode can be ascribed to its unique porous membrane structure, which accelerates the mass transfer kinetics of electrolyte ions and in situ generated hydrogen bubbles. As the Pd decorated molten ZIF-62 glass penetrated heavily into the TiC support pores, a very strong adhesion between Pd@ZIF-62 electrocatalytic layer and TiC substrate could be formed, which lowers the interfacial resistance between the catalyst and its substrate as well as promotes the charge transfer kinetics of HER electrode.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
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IF 7.312
Yingying You,Haiguang Yuan,Yixiao Wu,Yiyang Ma,Chenchen Meng,Xuesong Zhao
Using solar energy to reduce bromate in drinking water is promising. Unfortunately, most effective photocatalysts for bromate conversion are metal-based semiconductors. Here, for the first time, metal-free hybrid composites made of red phosphorus and perylene diimide (RP/PDI) were successfully designed and constructed, and their excellent catalytic performance for removing bromate under visible light was demonstrated. Characterizations such as XRD, FTIR, Raman, SEM and XPS confirmed the successful preparation of the hybrid catalyst, and the impact of water matrices suggests that it can be used for the actual treatment of bromate. The bromate reduction rate of the prepared RP/PDI-2 was 4.2 times and 7.0 times faster than pure RP and PDI, respectively. As evidenced by EIS and EPR results, this improvement is mainly due to the formation of p-n heterojunctions , which enhanced the separation of charge carriers and inhibited the production of active species ( O 2 − and OH) with strong oxidative capabilities. Considered holistically, the current study provides not only a metal-free photocatalyst with good photoreduction performance, but also some guidance for the rational design of hybrid photocatalyst in the treatment of aqueous bromate.
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