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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH · 2023 ·Vol. 30 ·期 18 ·53355-53369 · IF 5.8

Catalytic oxidation activation of peroxymonosulfate over Fe-Co bimetallic oxides for flurbiprofen degradation

Ding Chunsheng,Lei Jia,Cai Zhiyue,Gao Mengying,Zou Zhaozheng,Li Yuanfeng,Deng Jing

In this research, FeCo 2 O 4 nanomaterial was successfully synthesized by a typical sol–gel method and conducted as an effective agent for peroxymonosulfate (PMS) activation to eliminate antibiotics flurbiprofen (FLU), a strong nonsteroidal drug. FeCo 2 O 4 nanomaterial was characterized by XRD, TEM, SEM, and XPS. Various characterization results proved that FeCo 2 O 4 held stable spinel structure. The interfering factors including initial pH, PMS concentration, catalyst dosage, inorganic anions, and humic acid on FLU removal were also discussed. The conclusion was that the removal efficiency of FLU reached 98.2% within 120 min after adding FeCo 2 O 4 (0.4 g L −1 ) and PMS (3 mM). The optimal pH for FLU degradation was the initial pH of 6.5; too acidic or alkaline was not conductive to the degradation. The existence of HA and Cl − restrained the degradation of FLU, and HCO 3 − promoted the removal, while the influence of NO 3 − and SO 4 2− could not be considered. The radical scavenging experiment confirmed that • OH, O 2 •− , and SO 4 •− participated in FLU removal and SO 4 •− functioned a leading role. FeCo 2 O 4 showed high efficiency for PMS activation in pH range of 3.0 to 10.0. After the fourth cycle operation, the FLU removal rate exceeded 76.9%, and the Co leaching rate was low during the catalytic reaction. This study shows that FeCo 2 O 4 nanomaterial is an efficient and environment-friendly catalyst, which can be applied for PMS activation to remove organic pollutants in water.

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JOURNAL OF POLYMER SCIENCE · 2023 ·Vol. 61 ·期 12 ·1171-1182 · IF 3.4

Three dimensional printable multi-arms poly(CL-co-TOSUO) for resilient biodegradable elastomer

Yue Meng,Hong Zhai,Ziting Zhou,Xiaoying Wang,Jiandong Han,WenJuan Feng,Yuxin Huang,Yuan Wang,Ying Bai,Jing Zhou,Daping Quan

The development of artificial organs and implants demands new materials with both processability and functionality. A series of star like poly(CL- co -TOSUO) copolymers with different molecular weights are synthesized via ring-opening polymerization. The polymers are modified with norbornene end groups for rapid photo-crosslinking. Due to the random insertion of 1,4,8-trioxaspiro-[4,6]-9-undecanone and well-constructed permanent chemical network, the photo-crosslinked elastomers are more flexible and resilient than conventional poly(ε-caprolactone), with 84% resilience above the melting point. Their thermal and mechanical properties can be fine-tuned by varying the molecular weights of the precursors. The polymer can be fabricated into complex shapes by digital light processing 3D printing. Combined with good cytocompatibility and degradability, the highly flexible elastomers show great potential for tissue engineering. Graphical

CAS / MDL: 842-07-9 301-10-0
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JOURNAL OF MEMBRANE SCIENCE · 2023 · IF 9.5

An efficient co-solvent tailoring interfacial polymerization for nanofiltration: enhanced selectivity and mechanism

Yanrui Wang,Hailin Chang,Shu Jiang,Jialong Chen,Jinlong Wang,Heng Liang,Guibai Li,Xiaobin Tang

The interfacial polymerization (IP) plays a fundamental role in the fabrication of polyamide (PA) nanofiltration (NF) membranes with high ion selectivity and water permeability, which has enormous value for the increasing permeate quality and production in desalination. Herein, this study adopted a weak-polar organic solvent of ethyl formate (EF) to effectively regulate the IP process between piperazine (PIP) and trimesoyl chloride (TMC). The engineered PA separate layer conferred a uniform and ultrafine pore size (∼0.195 nm), exhibited a precise solute separation, and maintained a desirable permeability (18.4 ± 0.9 L m −2  h −1 bar −1 ). Molecular dynamics (MD) simulation indicated that EF involvement would significantly reduce the interfacial tension to motivate a fast and abundant diffusion of amine monomers from the aqueous phase into organic phase during the IP reaction, contributing to engineering a PA film with higher crosslinking degree. The optimized PA NF membranes conferred a more efficient rejection for divalent anions and cations (e.g., 99.5% for Na 2 SO 4 and 98.8% for MgCl 2 ). Remarkably, the membrane endowed a fairly high mono/divalent ion selectivity at sub-angstrom size, such as 145 for Cl − /SO 4 2− and 61 for Na + /Mg 2+ . The outstanding NF performance successfully broke the "trade-off" bound of perm-selectivity and was superior to the most "state-of-the-art" NF membranes. Overall, the co-solvent based IP strategy was beneficial to developing high-performance NF membranes without any significant changes to the existing fabrication process, and its facile and cost-effective merits were full of significance to the membrane manufacture.

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International Journal of Nanomedicine · 2023 · IF 8

Efficient Delivery of Antibodies Intracellularly by Co-Assembly with Hexahistidine-Metal Assemblies (HmA)

Shaoyin Wei,Sijie Zhou,Wenjuan Huang,Xingjie Zan,Wujun Geng

Purpose There has been a substantial global market for antibodies, which are based on extracellular targets. Binding intracellular targets by antibodies will bring new chances in antibody therapeutics and a huge market increase. We aim to evaluate the efficiency of a novel delivery system of His6-metal assembly (HmA) in delivering intracellular antibodies and biofunctions of delivered antibodies.Methods In this study, the physicochemical properties of HmA@Antibodies generated through co-assembling with antibodies and HmA were well characterized by dynamic light scatter. The cytotoxicity of HmA@Antibodies was investigated by Cell Counting Kit-8 (CCK-8). The endocytic kinetics and lysosome escape process of HmA@Antibodies were studied by flow cytometry and fluorescent staining imaging, respectively. Compared to the commercialized positive control, the intracellular delivery efficiency by HmA@Antibodies and biofunctions of delivered antibodies were evaluated by fluorescent imaging and CCK-8.Results Various antibodies (IgG, anti-β-tubulin and anti-NPC) could co-assemble with HmA under a gentle condition, producing nano-sized (~150 nm) and positively charged (~+30 eV) HmA@Antibodies particles with narrow size distribution (PDI ~ 0.15). HmA displayed very low cytotoxicity to divers cells (DCs, HeLa, HCECs, and HRPE) even after 96 h for the feeding concentration ≤100 μg mL−1, and fast escape from endosomes. In the case of delivery IgG, the delivery efficiency into alive cells of HmA was better than a commercial protein delivery reagent (PULSin). For cases of the anti-β-tubulin and anti-NPC, HmA showed comparable delivery efficiency to their positive controls, but HmA with ability to deliver these antibodies into alive cells was still superior to positive controls delivering antibodies into dead cells through punching holes.Conclusion Our results indicate that this strategy is a feasible way to deliver various antibodies intracellularly while preserving their functions, which has great potential in various applications and treating many refractory diseases by intracellular antibody delivery.

✓ 已验证 产品关联 DOI PubMed 高影响因子
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Biomaterials Research · 2023 ·Vol. 27 ·期 1 ·1-20 · IF 11.3

Bionic natural small molecule co-assemblies towards targeted and synergistic Chemo/PDT/CDT

Fu Shiyao,Wang Mingao,Li Bin,Li Xu,Cheng Jianjun,Zhao Haitian,Zhang Hua,Dong Aijun,Lu Weihong,Yang Xin

Background Multi-component nano-delivery systems based on chemotherapy (chemo)- photodynamic therapy (PDT)- chemodynamic therapy (CDT) have gained increased attention as a promising strategy to improve clinical outcomes in cancer treatment. However, there remains a challenge in developing biodegradable, biocompatible, less toxic, yet highly efficient multicomponent nanobased drug delivery systems (DDS). Here, our study presents the screening and development of a novel DDS based on co-assemblies natural small molecule (NSMs). These molecules (oleanolic acid, and betulinic acid) are combined with photosensitizers Chlorine6 (Ce6) and Cu 2+ that are encapsulated by tumor cell membranes. This nanocarrier encapsulated in tumor cell membranes achieved good tumor targeting and a significant improvement in tumor accumulation. Methods A reprecipitation method was used to prepare the co-assembled nanocarrier, followed by the introduction of Cu 2 +  into the DDS (OABACe6 NPs). Then, by wrapping the surface of NPs with the cell membranes of 4T1 which is a kind of mouse breast cancer cells (CM@OABACe6/Cu NPs). and analysis of its structure and size distribution with UV–Vis, XPS, FT-IR, SEM, TEM, and DLS. The synergistic effects of in vitro chemotherapy, CDT and PDT and targeting were also validated by cellular and animal studies. Results It was shown that CM@OABACe6/Cu NPs achieved good tumor targeting and a significant improvement in tumor accumulation. In the composite nano-assembly, the NSMs work together with the Ce6 to provide effective and safe chemo and PDT. Moreover, the effect of reduced PDT due to the depletion of reactive oxygen species (ROS) by excess glutathione (GSH) in the tumor can be counteracted when Cu 2 +  is introduced. More importantly, it also confers CDT through a Fenton-like catalytic reaction with H 2 O overexpressed at the tumor site. Conclusions By constructing CM@OABACe6/Cu NPs with homologous targeting, we create a triple synergistic platform for cancer therapy using PDT, chemo, and CDT. We propose here a novel combinatorial strategy for designing more naturally co-assembled small molecules, especially for the development of multifunctional synergistic therapies that utilize NSMs.

CAS / MDL: 10125-13-0
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Cu/Co bimetallic conductive MOFs: Electronic modulation for enhanced nitrate reduction to ammonia

Peng Liu,Jianyue Yan,Hao Huang,Wenbo Song

Electrochemical reduction of nitrate to ammonia is an eco-friendly strategy to remove the nitrate pollution in waste effluents. Developing new-type electrocatalysts with high activity for NO 3 RR has attracted worldwide attention. Owing to the numerous active single-metal sites, electric conductivity and ordered in-plane porous structure, conductive metal–organic frameworks (cMOFs) are promising alternative to construct the next-generation NO 3 RR electrocatalysts. In this work, a bimetallic cMOF (Cu x Co y HHTP) is proposed for efficient NO 3 – electroreduction to ammonia and the synergy effect between different types of single-metal sites is also revealed. As the result, the optimal Cu 1 Co 1 HHTP exhibits an outstanding electrocatalytic activity with a high NH 3 yield rate of 299.9 μmol h −1 cm −2 and a large Faradic efficiency of 96.4%. Both theoretical and experimental results reveal that the Co sites can affect the electron structure of Cu sites in Cu 1 Co 1 HHTP slab and decrease the ΔG of potential determining step in NO 3 RR process. Moreover, the Co sites bring a higher selectivity to Cu active sites for reducing *NO 2 to *NO, rather than the desorption of NO 2 – . The bimetallic c-MOFs strategy will innovate the design concept of next-generation catalyst, paving the way to investigate catalytic mechanism of single-metal-atom and open up their application prospects.

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PROGRESS IN ORGANIC COATINGS · 2023 · IF 6.6

Nanoscale chemical heterogeneity enables the co-existence of opposing superhydrophobic and hygroscopic properties

Haiyan Zhang,Zhiguang Xu,Tao Zhang,Yan Zhao

Superhydrophobicity and hygroscopicity are two properties that are theoretically exclusive to each other. The fabrication of functional fabrics with these two properties remains very challenging. In this work, it is demonstrated that a non-sticky superhydrophobic and hygroscopic fabric coating can be prepared via the photo polymerization of hexadecyl acrylate and methacrylic acid. On coating surface , the phase-separation-induced chemical heterogeneity has a unique feature of possessing elevated continuous hydrophobic domain and depressed hydrophilic domain, as evidenced by atomic force microscopy measurement. The elevation of hydrophobic domain (i.e., depression of hydrophilic domain) allows the hydrophilic domain to make negligible contribution to the surface wettability to water drop, but can absorb water molecules, thus inducing the unique superhydrophobic but hygroscopic property. The coating has a very low total surface energy of 22.61 mN m −1 , with its polar part (0.01 mN m −1 ) being negligible, thereby showing a high static water contact angle of ~112° on flat glass slide. The coated polyester fabric shows a non-sticky superhydrophobicity with a static water contact angle of ~151° and a water shedding angle of ~10°, as well as good hygroscopic and anti-static properties. We anticipate that this novel coating and the reported strategy of generating the particular chemical heterogeneity may lead to the development of advanced special wettability coatings for various applications.

CAS / MDL: 26570-48-9
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Acta Biomaterialia · 2023 · IF 9.7

Stimuli-responsive heparin-drug conjugates co-assembled into stable nanomedicines for cancer therapy

Zaixiang Fang,Ling Lin,Zhiqian Li,Lei Gu,Dayi Pan,Yunkun Li,Jie Chen,Haitao Ding,Xiaohe Tian,Qiyong Gong,Kui Luo

The combination of chemotherapy and photodynamic therapy (PDT) has the potential to complement single-drug therapies, but chemotherapeutic agents and photosensitizers often have compromised therapeutic efficacies and strong toxic effects. In this study, we exploited nanotechnology to address this challenge by utilizing heparin as a carrier for co-delivery of chemotherapeutic drugs and photosensitizers for synergistic cancer therapy. Specifically, heparin-paclitaxel (HP-PTX) and heparin-pyropheophorbide-a (HP-Ppa) were synthesized by attaching paclitaxel (PTX), a small molecular chemotherapeutic drug, through a reactive oxygen species (ROS)-responsive linker and Ppa, a photosensitizer, to heparin, respectively. Two conjugates were co-assembled into a nanomedicine , HP-PP nanoparticles (NPs), for controllable co-delivery of Ppa and PTX into tumor cells. HP-PP NPs significantly enhanced the in vitro stability of HP-Ppa and the photostability of Ppa, and the synergistic actions of chemotherapy and PDT were confirmed by both in vitro and in vivo antitumor studies. Notably, HP-PP NPs enhanced tumor accumulation of Ppa up to 11-fold and the treatment of 4T1 tumor-bearing mice with HP-PP NPs resulted in a tumor growth inhibition of 98.1% without systemic toxicity. The strategy of co-assembly of heparin conjugates may offer great potential in enhancing the efficacy of combination therapy. Statement of significance We proposed a nano-delivery system, HP-PP NPs, which was constructed by co-assembly of heparin-paclitaxel (HP-PTX) and heparin-pyropheophorbide-a (HP-Ppa), to co-deliver PTX and Ppa for synergistic cancer therapy. HP-PP NPs enhanced the photostability and the in vitro stability of Ppa and HP-Ppa, and induced greater cytotoxicity than HP-PTX NPs or HP-Ppa NPs. This co-delivery system displays enhanced tumor accumulation and has a remarkable synergistic antitumor effect with a tumor growth inhibition of 98.1%.

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TRANSACTIONS OF NONFERROUS METALS SOCIETY OF CHINA · 2023 · IF 4.5

Synthesis and up-conversion luminescence of Ho3+ and Yb3+ co-doped La7P3O18 phosphors

Hao-tian ZHU,Hai-rui GUO,Qi-jing ZHENG,Chun-yan GUAN,Li-ping ZHU,Hai-bin LI,Jin-yu YANG

Ho 3+ and Yb 3+ co-doped La 7 P 3 O 18 up-conversion phosphors were prepared by a high-temperature solid-state process. XRD results reveal that the samples are mixtures of monoclinic structure La 7 P 3 O 18 crystals with P 21/ n space group and minor LaPO 4 crystals. UV—Vis DRS results indicate that La 7 P 3 O 18 crystal is an indirect semiconductor with an optical band gap of 4.10 eV. After 980 nm laser excitation, the Ho 3+ and Yb 3+ co-doped La 7 P 3 O 18 phosphors show the characteristic blue (486 nm), green (550 nm), and red (661 nm) luminescence peaks of Ho 3+ ions. The peak at 661 nm dominates in the up-conversion luminescence spectra of samples. Meanwhile, with the increase of Ho 3+ and Yb 3+ doping content, the up-conversion luminescence intensity increases first and then decreases. By increasing the doping contents of Ho 3+ and Yb 3+ up to 1 at.% and 10 at.%, respectively, concentration quenching may appear by an electric quadrupole– electric quadrupole interaction process. The pumping power dependence of luminescence indicates that the green and red emissions of samples are excited by a two-photon absorption process. The color coordinates of Ho 3+ and Yb 3+ co-doped La 7 P 3 O 18 crystals locate in the orange—red region.

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APPLIED SURFACE SCIENCE · 2023 · IF 6.7

2D porous Co-Mo nitride heterostructures nanosheets for highly effective electrochemical water splitting

Jie Zhu,Qixing Du,Muhammad Arif Khan,Hongbin Zhao,Jianhui Fang,Daixin Ye,Jiujun Zhang

A significant issue in the overall water splitting process is the development of bifunctional non-precious metal catalysts with high performance. Herein, we designed and synthesized heterogeneous structure of Co 5.47 N/MoN (Co-Mo-N) porous nanosheets in situ grown on nickel foam substrates by thermal ammonolysis of CoMoO 4 precursors. The special heterogeneous and porous nanosheet structure of Co-Mo-N not only provides abundance of active sites, but also accelerates the charge transfer due to the interaction between Co 5.47 N and MoN. Additionally, the differing energy band configurations of the various phases in heterostructure will cause charge transport at the interface, which would be advantageous for the surface electron modification of heterojunctions and further enhances the electrocatalytic performance. As a result, the Co-Mo-N heterostructure exhibited excellent OER and HER catalytic activity, with over potentials of 288 and 82 mV at 10 mA cm −2 , respectively. When using Co-Mo-N heterostructures as cathodes and anodes to achieve overall water splitting, a low voltage of 1.59 V is required to achieve a current density of 10 mA cm −2 . This research presents a novel approach to designing bifunctional non-precious metal catalysts for overall water splitting.

CAS / MDL: 12030-49-8 7440-06-4
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RSC Advances · 2023 ·Vol. 13 ·期 9 ·5667-5673 · IF 3.9

Preparation of novel β-CD/P(AA-co-AM) hydrogels by frontal polymerization

Bin Li,Haibo Qin,Ming Ma,Xiaojia Xu,Mengjing Zhou,Wenrui Hao,Zhigang Hu

In this paper, betaine (Bet) was used as a hydrogen bond acceptor (HBA), and acrylic acid (AA) and acrylamide (AM) were used as hydrogen bond donors (HBD) and mixed to form a deep eutectic solvent (DES). Different concentrations of β-cyclodextrin (β-CD) were dispersed in the DES, and a novel β-CD/P(AA-co-AM) hydrogel was prepared by frontal polymerization (FP). The characteristic structure and morphology of the hydrogels were analyzed using Fourier transform infrared (FTIR) spectroscopy and scanning electron microscopy (SEM), and the properties of the hydrogels were investigated. The results show that the mechanical properties of the hydrogel were improved by β-CD acting as a second cross-linking agent in the polymerization process, thus increasing the cross-link density of the hydrogel. Because the carboxyl groups contained in the acrylic acid dissociate under alkaline conditions, the composite hydrogel shows excellent pH responsiveness under alkaline conditions. Tetracycline hydrochloride was used as a drug model to test the drug loading and drug release performance of the hydrogels. With the increase of β-CD content, the loading capacity of the hydrogels for tetracycline hydrochloride gradually increased. The data of drug release indicated that the hydrogel has good drug delivery performance and has promising applications in drug delivery systems and other areas.

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APPLIED SURFACE SCIENCE · 2023 · IF 6.7

Promoting photoelectrochemical water oxidation of BiVO4 photoanode via Co-MOF-derived heterostructural cocatalyst

Dan Wang,Jiangli Gu,Hanlin Wang,Mingzhuang Liu,Yichun Liu,Xintong Zhang

The sluggish surface reaction kinetic is the bottleneck limiting the photoelectrochemical (PEC) water oxidation of BiVO 4 photoanode, especially for the porous structured BiVO 4 with high surface area. Here, Co-based metal–organic frameworks (MOFs) were modified on porous BiVO 4 photoanode followed by calcining in the N 2 atmosphere, forming BiVO 4 -MOF-N 2 photoanode. The MOF-derived heterostructural cocatalysts significantly enhanced the photocurrent density of BiVO 4 -MOF-N 2 , reaching 2.32 mA·cm −2 (1.23 V vs RHE), about 1.15 times that of BiVO 4 -MOF and 2.64 times that of pristine BiVO 4 . The comparative study of BiVO 4 -MOF-N 2 , BiVO 4 -MOF, and pristine BiVO 4 photoanodes suggested that the Co-MOF-derived heterostructural cocatalyst had a much stronger effect on promoting the surface reactions than pure MOF. The BiVO 4 -MOF-N 2 photoanode had the highest charge transfer efficiency of 63.1 % at 1.3 V vs RHE and the lowest charge transfer resistivity compared with BiVO 4 and BiVO 4 -MOF. Both Co-active centers and conductive carbon matrix contributed to the enhanced charge transfer of BiVO 4 -MOF-N 2 photoanode. A MOF-loading-time dependent PEC performance of BiVO 4 photoanode also indicated that the intermediate charge transfer process from BiVO 4 to active centers strongly affected the final charge transfer and PEC performances. This work provides new insights into the design of high-performance photoelectrochemical electrodes based on heterostructural cocatalysts.

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