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CHEMICAL ENGINEERING JOURNAL · 2020 · IF 10.652

Mitochondria-targeted magnetic gold nanoheterostructure for multi-modal imaging guided photothermal and photodynamic therapy of triple-negative breast cancer

Bo Li,Qian Zhou,Haiyang Wang,Yongchao Zha,Peilian Zheng,Tong Yang,Dong Ma,Lin Qiu,Ximing Xu,Ye Hu,Anna Roig,Siming Yu,Wei Xue

Triple-negative breast cancer (TNBC) is a type of highly aggressive cancer that is hard to be cured by the commonly used chemotherapy, mainly due to the lack of effective tumor targeting ability of the current drugs and TNBC drug resistance. Therefore, development of novel strategies for precise and high-efficient therapy of TNBCs is urgently needed. In the present work, a multifunctional magnetic gold nanoheterostructure with photosensitizer Ce6 loading ( [email protected] ) was designed and synthesized for synergistic photothermal and photodynamic therapy (PTT/PDT) of TNBC. To improve the tumor targeting ability, cRGD and TPP cationic molecule, which can specifically target α v β 3 integrin of cancer cell membrane and mitochondria, respectively, were functionalized on the nanosystem obtaining [email protected] @RT. In vitro and in vivo fluorescent imaging demonstrated that cRGD and TPP functionalization largely enhanced the delivery-efficiency of [email protected] @RT into TNBC cells and tumors. Under 880 nm and 660 nm laser irradiations, [email protected] @RT exhibited strong hyperthermia effect and ROS generating ability, which exerted a synergistic anti-TNBC effect by completely suppressed the tumor growth of the nude mice model. Moreover, by integrating superparamagnetic and near infrared light absorption properties into a single nanocomposite , [email protected] @RT was proved to be able to realize magnetic resonance , X-ray computed tomography and photoacoustic tri-modal imaging of in vivo tumors. In all, we provide a novel strategy for precise delivery of functional nanosystems to TNBC tumors to achieve more satisfying treating outcome.

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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2020 · IF 7.489

Synthesis of EDTA-bridged CdS/g-C3N4 heterostructure photocatalyst with enhanced performance for photoredox reactions

Yi Xiao,Ting Wang,Ganhua Qiu,Kun Zhang,Changguo Xue,Benxia Li

Photocatalytic reactions represent a kind of green and sustainable chemical processes for organic transformations, but the efficiency is limited by the severe recombination and/or inadequate redox potentials of photoinduced charge carriers in photocatalysts . To address these issues, herein, the CdS-EDTA/g-C 3 N 4 heterostructures were designed according to Z-scheme photocatalytic mechanism and synthesized by the hydrothermal growth of CdS on g-C 3 N 4 nanoflakes with assistance of EDTA chelating agent. EDTA played multiple roles in the formation of CdS-EDTA/g-C 3 N 4 heterostructure photocatalysts, such as controlling the morphology of CdS nanostructures , linking CdS and g-C 3 N 4 together, and boosting the charge transfer between two semiconductors. The optimized CdS-EDTA/g-C 3 N 4 (10%) photocatalyst exhibited much higher activities toward the selective reduction of nitrophenol and the selective oxidation of benzyl alcohol , than those of CdS/g-C 3 N 4 heterostructures without EDTA. The enhanced photocatalysis of CdS-EDTA/g-C 3 N 4 can be ascribed to the efficient separation and suitable photoredox potentials of photoexcited charge carriers in the EDTA-bridged Z-scheme system. This work provides the inspiration for exploring inexpensive organic electron mediators for constructing all-solid-state Z-scheme photocatalysts and demonstrates the enhanced performance of Z-scheme photocatalysts for photoredox reactions of organic transformations.

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JOURNAL OF ASIA-PACIFIC ENTOMOLOGY · 2020 · IF 1.101

Development of lady beetle attractants from floral volatiles and other semiochemicals for the biological control of aphids

Jinhao Zhao,Zhongyan Wang,Zhongshan Li,Jiayu Shi,Ling Meng,Guorong Wang,Jingli Cheng,Yongjun Du

Aphids are among the most destructive phytophagous pests of host plants, because of their rapid reproduction, parthenogenesis, extensive crop damage, and the transmission of many plant viruses. Since lady beetles are important predatory natural enemies of aphids, developing lady beetle attractants to increase their field abundance is vital for aphid control. Floral volatiles and other semiochemicals are reportedly attractive to lady beetles. In this research, a total of 58 floral volatiles were tested by Y-tube olfactometer assays, among which 29 were highly attractive to both Harmonia axyridis (Coleoptera: Coccinellidae) and Coccinella septempunctata (Coleoptera: Coccinellidae). Meanwhile, the results of wind tunnel trials showed that only isoamyl acetate, α -humulene, trans -3-hexen-1-ol, methyl salicylate, and β -pinene lure these two species. Thereafter, 15 semiochemicals from pests, natural enemies, and pest-infested crops were mixed with the selected floral volatiles, to determine optimum formulations for attracting lady beetles through wind tunnels and further field trials. Eventually, formulas (1) α -humulene: β -pinene: methyl salicylate: trans -3-hexen-1-ol = 1:3:3:10; (5) α -humulene: β -pinene: methyl salicylate:1-nonanal = 1:3:3:10; (8) α -humulene: β -pinene: methyl salicylate: indole = 1:3:3:10 ( 1 , 5 , and 8 are labels used for the various formulations in field trials) were successfully verified to be attractive to lady beetles in both pumpkin and wheat fields. These formulations will be of great significance in developing integrated pest management strategies for aphid control.

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ELECTROCHIMICA ACTA · 2020 · IF 6.215

Tunable electronic properties of TiO2 nanocrystals by in situ dopamine functionalization for planar perovskite solar cells

Congcong Liu,Haijun Su,Chenyang Wei,Keyu Xie,Hongqiang Wang,Peng Zhai,Min Guo,Jun Zhang,Lin Liu

A high-quality TiO 2 electron transport layer (ETL) should possess a good energy-level alignment, perfect electron mobility, and excellent charge extraction efficiency. Nevertheless, the poor conductivity of amorphous TiO 2 film from low-temperature preparation is an inherent problem while the high-crystallined TiO 2 after high-temperature sintering (>450 °C) limits its application in the low-cost fabrication and flexible substrates. Here, we develop a low-temperature approach to in situ functionalize TiO 2 nanocrystals with dopamine molecules (DA-TiO 2 NCs) in the synthesis of the nanocrystals through a non-aqueous sol-gel method. We systematically investigate the tunable electronic properties of TiO 2 NCs with the variable DA modification and confirm that DA-TiO 2 can tailor the energy level alignment as well as increase the charge-extraction capacity, substantially reducing charge accumulation between the TiO 2 and perovskite layer. The in situ anchored amino groups (-NH 3 + ) not only preferentially boost the in-plane growth of perovskite grains but also induce the red-shift absorption of perovskite via the strong electrostatic interaction with Br − ions. Based on the DA-TiO 2 NCs ETLs, the power conversion efficiency of the fully ambient-processed planar FA x MA 1-x PbBr y I 3-y PSCs is optimized to 19.45%.

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APPLIED CATALYSIS B-ENVIRONMENTAL · 2020 · IF 16.683

Modulation of Lewis acidic-basic sites for efficient photocatalytic H2O2 production over potassium intercalated tri-s-triazine materials

Jingzhen Zhang,Chunyang Yu,Junyu Lang,Yongfeng Zhou,Baoxue Zhou,Yun Hang Hu,Mingce Long

Photocatalytic H 2 O 2 production (PHOP) on graphitic carbon nitride (GCN) at neutral pHs is limited by the sluggish oxidation of sacrificial alcohols and insufficient protons. In our work, the PHOP over a series of K intercalated triazine (KTCN) or tri-s-triazine units (KTTCN) reached 11–32 folds of GCN in the presence of only 0.5 vol% isopropanol, and a positive correlation between the H 2 O 2 production and the K contents was found. The critical role of K was revealed as that K intercalation creates Lewis acidic sites for isopropanol adsorption and strengthens Lewis basic sites for hydrogen abstraction and proton release. The improved alcohol oxidation and enhanced O 2 chemisorption synergistically result in dramatically accelerated PHOP over KTTCN. The findings provide the understanding of the preliminary active site dependent PHOP mechanism and bring insights for design of carbon nitride polymers with desirable photocatalytic performance.

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JOURNAL OF CATALYSIS · 2020 · IF 7.888

Layered double hydroxides supported atomically precise Aun nanoclusters for air oxidation of benzyl alcohol: Effects of size and active site structure

Yang Xu,Jin Li,Jian Zhou,Yufeng Liu,Zhuojun Wei,Hui Zhang

The effects of size and active site structure on catalytic activity were deeply investigated in air oxidation of benzyl alcohol over a series of Ni 3 Al-LDH (layered double hydroxides)-supported Au n nanocluster (NC) catalysts Au n /LDH (n = 25, 38, ~127), obtained by modified electrostatic adsorption of atomically precise Au 25 Capt 18 , Au 38 Capt 24 and Au ~127 -Capt (Capt: captopril) NCs followed proper calcination. Detailed characterizations show that the Au 25 /LDH, Au 38 /LDH and Au ~127 /LDH possess ultrafine Au NCs size of 1.2 ± 0.2, 1.4 ± 0.3 and 1.8 ± 0.5 nm, respectively, which are majorly dispersed on the edge sites of the small-sized LDH nanosheets (20–40 nm). All the catalysts exhibit excellent catalytic activities in air oxidation of benzyl alcohol without external base associated with the remarkable size- and active site structure-dependence. The catalyst Au 38 /LDH shows the highest activity with TOF of 1884 h −1 , which can be attributable to the ultrafine bi-icosahedron structure Au 38 NCs and the strongest Au 38 NCs – Ni-OH (LDH) synergistic effect facilitating the activation of α-C H bond of benzyl alcohol over more negatively charged Au sites upon XPS, CO-DRIFTs and kinetic isotope studies. The findings of the size- and active site structure-dependence of supported Au n cluster catalysts in the oxidation of benzyl alcohol provide important guiding principles for the rational design of supported Au n cluster catalysts.

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Polymer Chemistry · 2019 ·Vol. 10 ·期 43 ·5905-5912 · IF 4.76

Fast, selective and metal-free ring-opening polymerization to synthesize polycarbonate/polyester copolymers with high incorporation of ethylene carbonate using an organocatalytic phosphazene base

Chuanzhi Wei,Xinhui Kou,Shaofeng Liu,Zhibo Li

Ring-opening polymerization (ROP) is a powerful method used for converting cyclic monomers to polymers, but ethylene carbonate (EC), which has a five-membered ring, is an exception owing to the unfavorable thermodynamics of its ring-opening reaction unless the release of CO2. This behavior stems from the faster cyclization to form a stable five-membered ring in comparison to the direct ring-opening reaction. Hence, many attempts have been made to copolymerize EC with other cyclic monomers such as cyclic esters to overcome the thermodynamic barrier. In this context, the copolymerization of EC with various cyclic esters, including ε-caprolactone (CL), δ-valerolactone (VL) and L-lactide (LLA), has been successfully achieved using an organocatalytic phosphazene superbase, such as a cyclic trimeric phosphazene base (CTPB). The random copolymerizations proceeded fast with a turnover frequency (TOF) of 19 800 h−1 under mild polymerization conditions and afforded the corresponding copolymers without formation of the ether unit. Under all kinds of experimental conditions, no homopolymerization of EC occurred. The molecular structures of the obtained P(EC-co-CL) copolymers were characterized using 1H NMR and 13C NMR, which demonstrated that ca. 38 mol% EC can be incorporated within the copolymer chain depending on the different ratios of the EC and CL monomers. With the same catalytic system and under similar conditions, the amounts of EC incorporated into EC/VL (up to 26 mol%) and EC/LLA (ca. 4.8 mol%) copolymerizations were lower than that for the EC/CL copolymerization. 2D NMR (1H–1H correlated spectroscopy (COSY), 1H–13C heteronuclear single quantum coherence (HSQC) and 1H–13C heteronuclear multiple bond correlation (HMBC)) were performed to confirm the assignments in the 1H NMR and 13C NMR spectra of the copolymers and to better understand the chain structures of the copolymers. Therefore, polycarbonate/polyester copolymers with greater incorporation of EC were realized using a fast, selective and metal-free process.

CAS / MDL: 100-51-6 82654-98-6
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ACS Catalysis · 2019 · IF 12.221

Photocatalytic Coproduction of Deoxybenzoin and H2 through Tandem Redox Reactions

Nengchao Luo,Tingting Hou,Shiyang Liu,Bin Zeng,Jianmin Lu,Jian Zhang,Hongji Li,Feng Wang

Photocatalytic H2 evolution from organic feedstocks with simultaneous utilization of photogenerated holes achieves solar energy storage and coproduces value-added chemicals. Here we show visible-light H2 production from benzyl alcohol (BAL) with controllable generation of deoxybenzoin (DOB) or benzoin (BZ) through tandem redox reactions. Particularly, DOB synthesis circumvents the use of expensive feedstocks and environmentally unfriendly catalysts that are required previously. Under the irradiation of blue LEDs, the key of steering the major product to DOB rather than BZ is to decrease the conduction band bottom potentials of the ZnIn sulfide catalysts by increasing the Zn/In ratio, which results in the dehydration of intermediate hydrobenzoin (HB) to DOB proceeding in a redox-neutral mechanism and consuming an electron–hole pair. As a proof of concept, this method is used to synthesize DOB derivatives in gram scale.

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EUROPEAN POLYMER JOURNAL · 2019 · IF 3.621

Pyridyl-urea catalysts for the solvent-free ring-opening polymerization of lactones and trimethylene carbonate

Rui Feng,Suyun Jie,Pierre Braunstein,Bo-Geng Li

The ring-opening polymerization (ROP) of lactones is an effective method for the preparation of biocompatible and biodegradable aliphatic polyesters, for which the development of efficient organocatalysts with high activity and good controllability is highly desirable. A series of novel pyridyl-urea catalysts has been synthesized and applied in the solvent-free ROP of lactones and trimethylene carbonate. Combined with 7-methyl-1,5,7-triazabicyclo[4.4.0]dec-5-ene (MTBD), the pyridyl-urea/MTBD systems showed a fast and living/controlled behavior in the ROP, generating polymers with narrow molecular weight distributions. The influences of catalyst structure, type of base, pyridyl-urea/base ratio, feed ratio of monomer/initiator and reaction temperature on the catalytic properties were investigated. A possible mechanism was proposed on the basis of NMR titration and dilution experiments.

CAS / MDL: 100-51-6 65-85-0
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LWT-FOOD SCIENCE AND TECHNOLOGY · 2022 · IF 6.056

Contribution of microbial communities to flavors of Pixian Douban fermented in the closed system of multi-scale temperature and flow fields

Xiaoqing Ye,Yan Liu,Changbo Peng,Xi Guan,Yi Liu,Zhenming Che,Hongbin Lin,Xu Min,Qi Zhu,Wenwu Ding

In this study, Pixian Douban (PXDB) was produced in a closed system of multi-scale temperature and flow fields constructed with the materials of pseudoplastic fluid in a gradient steady-state temperature field. The flavors and microorganisms of PXDB in the MTFF were compared with those in the traditional process with original materials (TPOM) and the traditional process with materials of pseudoplastic fluid (TPPF). The contents of organic acids, free amino acids and flavors in the MTFF were higher than those in the TPPF and TPOM. Chitinophagaceae_Unclassified and Bradyrhizobium_Unclassified were the predominant bacteria while Phyllachora sp . UB03986 and Rhizopus oryzae were identified as the core fungi at the species levels in the processes. The correlation analysis showed that 26 bacterial and 6 fungal were significantly correlated with the flavors. The results indicated that the closed system of MTFF could improve the product quality and was helpful to realize the controllable PXDB production.

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DIAMOND AND RELATED MATERIALS · 2022 · IF 3.806

Guanine-derived nitrogen-doped carbon nanosheets for selective oxidation of benzyl alcohol

Shuchun Li,Yiling Ke,Xuefei Zhang,Shuchang Wu,Yiquan Chen,Zailai Xie

Nitrogen-doped carbon materials as metal-free catalysts have attracted considerable attention in selective oxidation of benzyl alcohol. However, the real active sites are still ambiguous due to complexities of surface functional groups and nitrogen species. Herein, a series of nitrogen-doped nanosheets with different N species content are simply fabricated, which exhibits excellent catalytic activity with 82–93 % conversion and 89–99 % selectivity in selective oxidation of benzyl alcohol into benzaldehyde. Moreover, it is demonstrated that the conversion of benzyl alcohol mainly depends on the hydroxyl functional groups, while both graphitic and pyridinic nitrogen are key factors to determine the selectivity of benzaldehyde. The present work demonstrates the structure-activity relationships between the catalytic performance for catalytic oxidation of benzyl alcohol and the surface functional groups of catalysts, paving the way for development of highly efficient nanocarbon catalysts.

CAS / MDL: 100-51-6 73-40-5
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DIAMOND AND RELATED MATERIALS · 2022 · IF 3.806

Enhanced activity of alcohol oxidation on nitrogen-doped carbon by FeN interaction

Shurui Xu,Baoqiang Lin,Qihang Huang,Wenting Qiu,Wenqian Yuan,Weirui Xu,Xingfeng Xue,Guoyu Zhong,Wenbo Liao,Wenlong Wang,Xiaobo Fu

Oat-derived N-doped carbon with tunable N content (OA-NCs) were synthesized and applied in alcohol oxidation to selectively produce aldehyde. OA-NCs exhibited unexpectedly high performance in the oxidation of benzyl alcohol, cinnamyl alcohol and furfuryl alcohol. N species were characterized to interpret its promoting effect on their catalytic activity . Oxidation activity of pyridinic N in OA-NCs was sensitive to their structure while reactivity assessment disclosed it was more active to convert alcohols in presence of Fe 3+ , rather than pyrrolic-N or graphite-N. The superoxide radical was evidenced as the most reactive oxygen species in this reaction. The strong metal-support interaction (MSI) between pyridinic N and Fe 3+ , indicated by DFT calculation, was determined to be critical for the high activity of OA-CNs catalysts. The present work provides the insight into the positive effect of N-metal interaction in carbon materials on O 2 activation and explores a green pathway for the selective production of aldehydes.

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