ChemNanoMat
·
2021
·Vol. 7
·期 12
·1322-1329
·
IF 3.154
Jinglei Qin,Lanying Guo,Tingyu Yang,Xi Wu,Zhi Wang,Fang Xie,Hongshang Peng
Graphical A novel dopamine-modified epoxysilane was synthesized via a ring-opening reaction. Then, the photosensitizer ZnPc and photothermal-agent polydopamine were simultaneously introduced into nanoparticles by a facile encapsulation-reprecipitation method. The nanoparticles exhibited high photothermal conversion efficiency (η = 46.4%) and suitable photostability, apart from the capacity of 1 O 2 generation (Φ Δ =0.28). Based on the nanoparticles, improved therapeutic efficacy against tumor cells was achieved with synergetic treatment of PDT/PTT, even under hypoxia. A major obstacle to clinical photodynamic therapy (PDT) is tissue hypoxia in a solid tumor, which substantially reduces therapeutic efficacy by insufficient oxygen supply. To tackle this issue, herein, we reported a type of facilely prepared multifunctional nanoparticles (NPs) for combined treatment of PDT and photothermal therapy (PTT). A novel dopamine-modified epoxysilane (GSDA) was firstly synthesized from 3-glycidoxypropyl(trimethoxy) silane and dopamine via ring-opening reaction, which was subsequently incorporated into NPs along with zinc(II) phthalocyanine (ZnPc) via a reprecipitation-encapsulation method. Interestingly, polydopamine (PDA) was found to be automatically developed inside NPs by oxidative polymerization of dopamine monomers. Owing to strong-light-absorption PDA and ZnPc, the resultant biocompatible NPs exhibited high photothermal conversion efficiency (η=46.4%) and a decent singlet oxygen quantum yield (ΦΔ=0.28), respectively, under the irradiation of 808 nm and 660 nm light. Synergetic treatment was then performed on tumor cells using the multifunctional NPs, i. e., PDT followed by PTT, and enhanced phototherapeutic efficacy was achieved, particularly in the case of hypoxia. This work demonstrates that (i) the newly-synthesized GSDA might function as a bi-functional coupling agent for silica and PDA coating, and (ii) the simply-prepared NPs are very promising for synergetic PDT/PTT of solid tumors.
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Nano Research
·
2021
·Vol. 15
·期 3
·1973-1982
·
IF 8.897
Tan Xianjun,Ding Wenhui,Jiang Zhenying,Sun Linxiao,Huang Yuxiong
To better understand the mechanisms of hydrogen peroxide (H 2 O 2 )’s decomposition and reactive oxygen species (ROS)’s formation on the catalyst’s surface is always a critical issue for the environmental application of Fenton/Fenton-like reaction. We here report a new approach to activate H 2 O 2 in a co-catalytic Fenton system with oxygen incorporated MoS 2 , namely MoS 2− x O x nanosheets. The MoS 2− x O x nanosheets assisted co-catalytic Fenton system exhibited superior degradation activity of emerging antibiotic contaminants (e.g., sulfamethoxazole). Combining density functional theory (DFT) calculation and experimental investigation, we demonstrated that oxygen incorporation could improve the intrinsic conductivity of MoS 2− x O x nanosheets and accelerate surface/interfacial charge transfer, which further leads to the efficacious activation of H 2 O 2 . Moreover, by tuning the oxygen proportion in MoS 2− x O x nanosheets, we are able to modulate the generation of ROS and further direct the oriented-conversion of H 2 O 2 to surface-bounded superoxide radical (·O 2 surface − ). It sheds light on the generation and transformation of ROS in the engineered system (e.g., Fenton, Fenton-like reaction) for efficient degradation of persistent pollutants.
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Journal of the Taiwan Institute of Chemical Engineers
·
2021
·
IF 5.876
Tingyan Lu,Qian Li,Jiawei Shao,Linlin Wang,Ruixue Pang,Xiaying Wu,Xin Hu
Backgrounds Adsorption by adsorbents is accepted as a promising technology that can efficiently separate CO 2 from flue gas. Optimal adsorption performance can be obtained by specific solid adsorbents with excellent CO 2 adsorption capacity. Methods In this work, N, S co-doped porous carbons were synthesized from polyacrylonitrile fiber by a facile synthesis process i.e. hydrothermal treatment followed by KOH activation. N, S enriched hydrochar was obtained after hydrothermal treatment of polyacrylonitrile fiber and ammonium sulfide. Further KOH activation of hydrochar obtained N, S co-doped carbons with advanced porous structure. Significant findings This series of sorbents has the highest CO 2 uptake of 3.37 and 5.23 mmol g −1 at 1 bar, 25 °C and 0 °C, respectively. Detailed investigation revealed that the mutual effects of narrow microporostiy, N and S content are responsible for the CO 2 uptake of these adsorbents. Additionally, these adsorbents also show various good CO 2 capture properties such as excellent recyclability, reasonable CO 2 /N 2 selectivity, moderate heat of adsorption, fast adsorption kinetics, and good dynamic adsorption capacity. These findings suggest that N, S co-doped porous carbons derived from polyacrylonitrile fiber are potential promising sorbents for CO 2 capture.
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Biomedical Materials
·
2021
·Vol. 16
·期 6
·065024
·
IF 3.715
Ruochen Luo,Yiqian Huang,Xiaojing Yuan,Zuoying Yuan,Liwen Zhang,Janming Han,Yuming Zhao,Qing Cai
For craniofacial bone regeneration, how to promote vascularized bone regeneration is still a significant problem, and the controlled release of trace elements vital to osteogenesis has attracted attention. In this study, an ion co-delivery system was developed to promote angiogenesis and osteogenesis. Magnesium ions (Mg2+) and lanthanum ions (La3+) were selected as biosignal molecules because Mg2+ can promote angiogenesis and both of them can enhance bone formation. Microspheres made of poly(lactide-co-glycolide) were applied to load La2(CO3)3, which was embedded into a MgO/MgCO3-loaded cryogel made of photocrosslinkable gelatin methacryloyl to enable co-delivery of Mg2+ and La3+. Evaluations of angiogenesis and osteogenesis were conducted via both in vitro cell culture using human bone marrow mesenchymal stromal cells and in vivo implantation using a rat model with calvarial defect (5 mm in diameter). Compared to systems releasing only Mg2+ or La3+, the combination system demonstrated more significant effects on blood vessels formation, thereby promoting the regeneration of vascularized bone tissue. At 8 weeks post-implantation, the new bone volume/total bone volume ratio reached a value of 40.1 ± 0.9%. In summary, a properly designed scaffold system with the capacity to release ions of different bioactivities in a desired pattern can be a promising strategy to meet vascularized bone regeneration requirements.
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Chemical Science
·
2021
·Vol. 12
·期 43
·14432-14440
·
IF 9.825
Jing Yan,Yu Qin,Wen-Ting Fan,Wen-Tao Wu,Song-Wei Lv,Li-Ping Yan,Yan-Ling Liu,Wei-Hua Huang
Recently, stretchable electrochemical sensors have stood out as a powerful tool for the detection of soft cells and tissues, since they could perfectly comply with the deformation of living organisms and synchronously monitor mechanically evoked biomolecule release. However, existing strategies for the fabrication of stretchable electrochemical sensors still face with huge challenges due to scarce electrode materials, demanding processing techniques and great complexity in further functionalization. Herein, we report a novel and facile strategy for one-step preparation of stretchable electrochemical biosensors by doping ionic liquid and catalyst into a conductive polymer (poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate), PEDOT:PSS). Bis(trifluoromethane) sulfonimide lithium salt as a small-molecule plasticizer can significantly improve the stretchability and conductivity of the PEDOT:PSS film, and cobalt phthalocyanine as an electrocatalyst endows the film with excellent electrochemical sensing performance. Moreover, the functionalized PEDOT:PSS retained good cell biocompatibility with two extra dopants. These satisfactory properties allowed the real-time monitoring of stretch-induced transient hydrogen peroxide release from cells. This work presents a versatile strategy to fabricate conductive polymer-based stretchable electrodes with easy processing and excellent performance, which benefits the in-depth exploration of sophisticated life activities by electrochemical sensing.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Jinchao Fang,Yuji Chen,Chuanjie Fang,Liping Zhu
In this work, we report on a regenerable and robust adsorptive membrane with superb dynamic adsorption capacity towards dyes prepared by a controllable mussel-inspired co-deposition of dopamine (DA) and polyethyleneimine (PEI) on a polyvinylidene fluoride (PVDF) microfiltration membrane. The DA oxidative self-polymerization occurred to form polydopamine for high adhesion with the PVDF membrane. On the other hand, the PEI provided a large number of amino groups with high adsorption ability, and had both Michael addition and Schiff base reaction with DA to induce covalent interaction for high stability. In addition, the co-deposition process was controlled to happen on the membrane surface and inside the membrane bulk pores simultaneously. By these ingenious designs, the prepared adsorptive membrane thus showed high dynamic adsorption capacity (up to 188 mg g −1 ) and ultra-high removal ratio (＞99.9%) towards typical anionic dye of methyl blue. Not only that, the membrane could separate rapidly and selectively anionic dyes from dye mixtures. More importantly, the adsorptive membrane showed highly regenerative ability in NaOH solution (after 6 recovery cycles, the treating efficiency maintained higher than 95%), and good durability with robust resistance in acidic and alkaline environments. This work affords an innovative strategy and insight in fabricating the adsorptive membrane using mussel-inspired co-deposition for organic dye removal in water.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Pengchao Ren,Weifeng Tu,Chanchan Wang,Sifan Cheng,Wenqi Liu,Zhenzhou Zhang,Yun Tian,Yi-Fan Han
This study investigated the Cu-CeO 2 interactions for CO hydrogenation to methanol by applying rate measurements, chemical titration/desorption, together with in-situ/operando spectroscopy techniques under realistic reaction conditions. Ce components were enriched in the surface region of Cu/CeO 2 catalysts while Ce 3+ and Ce 4+ atoms co-existed during CO hydrogenation. The ratio of Ce 3+ to Cu 0 in the surface region of catalysts increased linearly with the Ce content. The turnover rates of CH 3 OH formation increased as a single-valued function of the ratio, irrespective to the individual contact extent between Cu and CeO 2 clusters or Ce content in the Cu/CeO 2 catalysts, indicating that the Cu 0 -Ce 3+ sites pair acts as active sites for CO hydrogenation to methanol over Ce-CeO 2 samples. This study also unraveled that formyl and formate species, as reactive surface intermediates, were co-adsorbed on the Cu 0 -Ce 3+ sites, and their hydrogenation routes occurred concurrently for CH 3 OH formation during CO-H 2 reactions.
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JOURNAL OF CONTROLLED RELEASE
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2021
·
IF 9.776
Shengmei Wang,Xuanjun Liu,Shengfeng Wang,Linqi Ouyang,Hui Li,Jinsong Ding,Guiming Deng,Wenhu Zhou
Discovery of BCR-ABL1 tyrosine kinase inhibitors (TKIs) has revolutionized the therapy of chronic myeloid leukemia (CML), a malignant myeloproliferative disease characterized by abnormal activation of BCR-ABL fusion oncoprotein with protein tyrosine kinase (PTK) activity. However, the long-term treatment outcomes with TKIs are strongly limited by multiple drug resistances, resulting in relapse albeit with initial high response rate. Here, we reported a realgar (As 4 S 4 ) nanocrystal-based delivery system to reverse drug resistance for synergistic CML therapy. While As 4 S 4 is extremely insoluble in water, bovine serum albumin (BSA) was rationally screened to effectively stabilize As 4 S 4 nanocrystal with uniformed size of ~40 nm. Imatinib (IMA), a representative TKIs, can be readily loaded into the hydrophobic domain of BSA to develop As 4 S 4 /IMA co-delivery system. Mechanistically, IMA inhibits PTK activity, while As 4 S 4 degrades BCR-ABL1, which co-contribute to tumor suppression via complementary pathways for synergistic effect. Moreover, the nanosystem was modified with folic acid (FA) to enable tumor targetability, which has been demonstrated both in vitro and in vivo, resulting in robust tumor growth inhibition and significantly prolonged mice survival without any noticeable adverse effects. This work designed a synergistic nanoplatform for targeted CML therapy, provided a strategy to address the key limitation of As 4 S 4 for biomedical applications, and highlighted the advantages of the combination between traditional Chinese and western medicine for diseases treatment.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2021
·
IF 5.316
Hang-bo Zheng,Yu-ling Li,Yuan-li Wang,Feng Ma,Peng-zhao Gao,Wen-ming Guo,Hang Qin,Xiao-pan Liu,Han-ning Xiao
The development of efficient, inexpensive, and stable hydrogen evolution reaction (HER) electrocatalysts is the key to large-scale water electrolysis technologies for hydrogen production. Constructing heterojunction electrocatalysts has become one of the effective strategies for designing high-performance HER electrocatalysts due to their unique heterogeneous interfaces. Herein, a new strategy of PH 3 assisted synthesis of metaphosphate is reported, which is used to construct Co(PO 3 ) 2 @NPC/MoS 2 heterostructures (where NPC is N-doped porous carbon). The results show that the formation of Co(PO 3 ) 2 @NPC/MoS 2 heterogeneous interfaces can optimize the electronic structure of the electrocatalyst and greatly improve its HER performance. As a result, a lower overpotential of 119 mV at 10 mA cm −2 is obtained in alkaline electrolyte . This work provides a new perspective for the design of high-performance electrocatalysts for electrocatalytic water splitting.
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MICROCHIMICA ACTA
·
2021
·Vol. 189
·期 1
·1-11
·
IF 5.833
Ma Junping,Bai Wushuang,Liu Xiaoli,Zheng Jianbin
Integrating other metal ions into mono-metallic metal–organic framework (MOF) to form bi-metallic MOF is an effective strategy to enhance the performance of MOFs from the internal structure. In this study, two-dimensional (2D) cobalt/zinc-porphyrin (Co/Zn-TCPP) MOF nanomaterials with different Co/Zn molar ratios were synthesised using a simple surfactant-assisted method, and novel dopamine (DA) sensing methods were constructed based on these materials. The characterisation results showed that all MOF with different Co/Zn molar ratios presented a nanofilm, and the Co and Zn elements were uniformly distributed. All sensors based on Co x Zn 100− x -TCPP had a certain catalytic performance to DA. Among them, the sensor based on CO 25 Zn 75 -TCPP showed the strongest signal response, indicating that the catalytic performance of MOF on DA can be adjusted by changing the Co/Zn molar ratio. The doping of metal ions improves the chemical environment of the pores, and increases the types and spatial arrangement of the active sites of the MOF, which is beneficial to the electron transfer and exchange with DA; Co 2+ and Zn 2+ active centres have a synergistic promotion effect, so the catalytic activity of MOF is significantly improved. The linear range at the potential of 0.1 V based on Co 25 Zn 75 -TCPP for DA was 5 nM–177.8 μM, with a detection limit of 1.67 nM (S/N = 3). The sensor exhibited a good selectivity for detecting DA. This research is expected to provide new ideas and references for constructing high-performance sensing interfaces and platforms. Graphical abstract
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JOURNAL OF THE CERAMIC SOCIETY OF JAPAN
·
2021
·Vol. 129
·期 3
·159-167
·
IF 1.224
Yonghuan HAN,Liwen YAN,Shichen XIE,Tao XU,Wei JING,Feng HOU
Nd3xY3−3xAl5O12 (Nd:YAG) powders with high uniformity were synthesized by reverse-titration co-precipitation method. The precipitation formation process and dispersion mechanism of Nd:YAG precursor in co-precipitation process were analyzed, and the influence of the preparation technology on the dispersion of powders was explored by adjusting the concentration of precipitator, alcohol-water solvent and ratio of composite dispersant. In addition, through the analysis of the precursor calcination process, combined with SEM and particle size analysis, it is shown that, under optimum processing conditions, the powders have excellent particle uniformity, narrow particle size distribution and appropriate crystal size when calcined at 1150 °C for 2 h.
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ACS Omega
·
2021
·
IF 3.512
Mingyu Zhang,Chaoyong Wang,Junkai Zhang,Gang Li,Li Gu
LiNi0.8Co0.1Mn0.1O2 (NCM811) became a research hot point because of its low cost, environmental friendliness, and excellent electrochemical performance. However, Li+/Ni2+ intermixing is an essential factor affecting its applicability. Doping could be an important method to improve the electrochemical performance of NCM811-based cathode materials. In this work, La and Al co-doped NCM811 was prepared by a solid-state method. Results from X-ray diffraction (XRD), scanning electron microscopy (SEM), and energy-dispersive spectroscopy (EDS) and electrochemical performance were discussed in depth. These showed that when La and Al doping concentrations were 1 and 0.5%, the samples showed the best performance. The as-improved performances were mainly attributed to the reduced Li+/Ni2+ intermixing, suppressed phase transition, and decreased potential polarization and impedance.
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