CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Rui Sun,Qiaojie Luo,Ying Wang,Hanwen Chu,Xiaodong Li,Zhiquan Shen,Weipu Zhu
Intravenously administered nanodrugs undergo a number of processes to generate therapeutic effects. The rational design of nanodrugs with high efficiency at every step of the drug deliver process is critical to their therapeutic efficiency. However, many reported nanodrugs that meet these requirements are too complex to prepare for practical use. Herein, we report a simplified and reproducible one step nanodrug fabrication strategy, with only two components, using supramolecular engineering. Di-adamantane-modified camptothecin was precisely synthesized as a prodrug with high purity. An amphiphilic biodegradable block copolymer with pendant β-cyclodextrin moieties on the hydrophobic block was then synthesized by controlled ring-opening polymerization and “click” chemistry. The co-self-assembly of the camptothecin prodrug and block copolymer in an aqueous medium, driven by host–guest interactions between the adamantine and β-cyclodextrin moieties, gave a camptothecin nanodrug with quantitative drug loading content and defined chemical composition. This nanodrug, which consists of a suitable size and stable core-crosslinked structure, has prolonged blood circulation and accumulates efficiently at tumor sites thus showing potent anti-tumor activity. This work provides a strategy to precisely fabricate nanodrugs that is reproducible, and which has great potential for bench-to-bedside translation.
研究领域:
药学
·
肿瘤学
·
生物材料学
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产品关联
DOI
高影响因子
iScience
·
2025
·
IF 4.1
Shouji Li,Xiaobin Li,Junyu Liu,Yuting Lin,Xuedan Zhang,Weiren Zhong,Juan Li,Caifa You,Dong Wang,Jisong zhang,Xu Xu,Xu-Min Cai,Can Yang Zhang
Aggregation-induced emission luminogens (AIEgens) have been extensively investigated and widely used in biomedical fields. However, AIEgens are mostly derived from petrochemicals, leading to challenges of renewability, sustainability and biocompatibility. Therefore, it’s of striking prospect to construct bioproduct-based AIEgens (BioAIEgens) based on the natural profits. Herein, we proposed a straight forward method named “Rotor-Alicyclic” strategy to prepare BioAIEgens with high fluorescence and produce reactive oxygen species (ROS) activities as well as high biosafety. We prepared four BioAIEgens by introducing two rotors and a naturally rigid alicyclic moiety into coumarin molecule. The AIE performances were evaluated, especially the fluorescence and production of ROS activities. Mechanistic study proved the two rotors introduction can destroy the planar structure, and the rigid alicyclic moiety can limit the molecular motion. Furthermore, the biosafety was carefully investigated in vitro and in vivo , demonstrating the high biocompatibility. Summarily, we developed a facial engineering method to prepare BioAIEgens.
研究领域:
化学
·
生物医学
·
材料科学
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产品关联
DOI
PubMed
高影响因子
Advanced Optical Materials
·
2024
·
IF 8
Zhihao Guan,Zhaorun Tang,Jianwen Zeng,Junjie Deng,Yuewei Zheng,Houbin Li,Xinghai Liu
Long-life room temperature phosphorescent (RTP) materials hold significant potential in the fields of optoelectronic devices, information encryption, and bio-imaging due to their excellent optical properties. However, achieving multi-color tunable RTP materials has proven challenging. In this study, molecular engineering strategies are employed to select precursor molecules with varying degrees of conjugation such as phthalic anhydride (PA), naphtho[2,3-c] furan-1,3-dione (23NA), and naphthalic anhydride (NA). By combining these guest molecules with a host boric acid matrix through a one-step microwave method, carbon dots (CDs)composites (PA@BA, 23NA@BA and NA@BA) exhibiting excellent RTP properties are successfully prepared. As the degree of precursor conjugation increased gradually, the phosphorescence color modulation of the composites demonstrates satisfactory transitions from blue to yellow. Notably, CDs are derived in situ within the boric acid matrix while covalent and hydrogen bonds formed between CDs and borate matrix effectively suppress nonradiative leaps and facilitate composite RTP activation. Furthermore, the boric acid matrix acts as insulation against oxygen diffusion and prevents quenching of triplet excitons by external factors. The rationality behind phosphorescence emission mechanism and wavelength modulation is further conformed by density functional theory (DFT) calculations. Finally, CDs composites are successfully applied for advanced message encryption of text and images.
研究领域:
材料科学
·
光学
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产品关联
DOI
高影响因子
ADVANCED SYNTHESIS & CATALYSIS
·
2018
·Vol. 361
·期 4
·803-812
·
IF 5.123
Xinjian Yin,Yayun Liu,Lijun Meng,Haisheng Zhou,Jianping Wu,Lirong Yang
Glutamate dehydrogenases (GluDHs) are promising biocatalysts for the synthesis of chiral α-amino acids by asymmetric reductive amination of α-keto acids. However, their strict substrate specificity limits their applications. To address this problem, we developed a molecular engineering method for GluDHs that enhances the asymmetric reductive amination of bulky α-keto acids. Based on rational design, a “cave” located in the active site pocket of Pp GluDH (GluDH from Pseudomonas putida ), which plays an essential role in substrate recognition, was tailored to facilitate the accepting of bulky substrates. Two mutants (A167G and V378A) were discovered to have significantly enhanced catalytic activity toward 2-oxo-4-[(hydroxy)(methyl)phosphinyl]butyric acid (PPO) and several other bulky substrates. This molecular engineering method was then applied to ten other GluDHs from different sources and with different properties. All engineered GluDHs acquired substantial improvements in PPO-oriented catalytic activity. The most efficient mutant of NADP + (nicotinamide adenine dinucleotide phosphate)-specific GluDHs showed up to 1820-fold increased activity and the specific activity reached 111.02 U/mg-protein. The NAD + (nicotinamide adenine dinucleotide)-specific GluDHs, which have no detectable wild type activity toward PPO, acquired a considerable level of activity (1.90–29.48 U/mg-protein). In batch production of L-phosphinothricin, these “cave-tailored” GluDHs exhibited markedly improved catalytic efficiencies compared with their wild types and ee values of >99%. The space-time yields (STY) varied from 818.16 to 1482.96 g ⋅ L −1 ⋅ d −1 , suggesting potential practical applications of these mutants.
研究领域:
生物化学
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酶工程
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合成生物学
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产品关联
DOI
高影响因子
ChemSusChem
·
2021
·Vol. 14
·期 8
·1847-1852
·
IF 8.928
Ya Zhang,Xiao-Yu Zhang,Kai Chen,Wei-Yin Sun
Graphical There by the grace of gourd : Cu 2 O modified by cucurbit[6]urils acts as an efficient supramolecular inorganic catalyst for the electrochemical CO 2 reduction reaction. In 0.5 m KHCO 3 , it demonstrates a maximum total faradaic efficiency (FE CO+formate ) of 93.96 % at −0.7 V vs. RHE Electrochemical conversion of CO 2 into value-added fuels and feedstocks attracts worldwide attention to mitigate energy and environmental problems. However, pursuing highly efficient electrocatalyst is still a challenge. In this study, cuprous oxide (Cu 2 O) modified by cucurbit[6]urils (Q[6]), a kind of rigid macromolecule, is found to act as an efficient supramolecular inorganic nanocomposite catalyst for the electrochemical CO 2 reduction reaction (CO 2 RR) to C 1 fuels. This catalyst affords a high total faradaic efficiency (FE CO+formate ) of 93.96 % at a potential of −0.7 V vs. reversible hydrogen electrode and over 85 % from −0.6 to −0.9 V in 0.5 M KHCO 3 , which is higher than that of pure Cu 2 O (39.89 %). The enhancements in selectivity and activity for CO 2 RR could significantly benefit from the strong CO 2 adsorption capacity and hydrophobic nature of the cavity of Q[6], which simultaneously trap gaseous reactants near the catalyst to tune the local environment and limit the diffusion of water molecules. This study provides a strategy to adjust catalytic environments through supramolecular engineering.
研究领域:
材料科学
·
环境科学
·
化学
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产品关联
DOI
PubMed
高影响因子
DYES AND PIGMENTS
·
2021
·
IF 4.889
Jianwen Tian,Muzhou Teng,Mu Song,Zhijia Li,Xiaoyong Zhang,Youqin Xu
Fluorescence imaging-guided tumor photodynamic therapy (PDT) has received increasing attention due to its higher resolution of fluorescence imaging and noninvasive treatment of PDT. Two problems of fluorescence aggregation-caused quenching (ACQ) and tumor microenvironment hypoxia are urgently resolved in traditional PDT with fluorescence imaging function, but there is still a lack of effective molecular engineering to design delicate photosensitizers (PSs) to overcome fluorescence ACQ and tumor hypoxia, simultaneously. Herein, we develop a feasible molecular engineering to design aggregation-induced emission (AIE)-active PSs with unique free radical (type I) reactive oxygen species (ROS) by researching molecular structure-property relationship, which possesses bright fluorescence at aggregation and low O 2 -dependent under the process of generating free radical ROS. The intersystem crossing (ISC) channel is activated when frequently enhance intramolecular charge transfer (ICT) effect in electron-rich AIEgens with typical heavy atoms, which ensure enough triplet energy generation to induce superoxide anion free radical (O 2 − ·) generation. In vitro fluorescence imaging and photo triggering biotoxicity evaluation both revealed that new AIE-active photogenerator is a promising candidate for fluorescence imaging-guided PDT.
研究领域:
生物医学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
POLYMER
·
2023
·
IF 4.6
Mengyu Xiao,Baoquan Wan,Xinmo Wang,Ming-Sheng Zheng,Yuchao Li,Yiyi Zhang,Jun-Wei Zha
Polyetherimide (PEI) for high-temperature energy storage still face the critical problem of low discharged energy density . The dramatic increase in leakage current is the basic reason for the deterioration of energy storage characteristics under elevated temperatures. Herein, a molecular engineering strategy is presented to suppress electrical conduction by introducing a high electron-affinity dianhydride structure into the main chain of PEI. The energy band structure of PEI is markedly affected by the dianhydride, which is illustrated by experimental research and density functional theory (DFT) calculations. Structures with high electron-affinity act as trap centers to capture carriers, significantly inhibiting conduction at elevated temperatures. Consequently, the PEI hybrid film exhibits a discharged energy density of 4.01 J/cm 3 and a charge-discharge efficiency of 91% at 150 °C. The high throughput and easy processing of the PEI hybrid film makes it a potential choice for energy storage under harsh conditions. This work represents a route for preparing polymer dielectrics with outstanding energy storage characteristics capable of operating in high temperature environments.
研究领域:
材料科学
·
能源技术
✓ 已验证
DOI
高影响因子
Journal of Materials Chemistry C
·
2022
·Vol. 10
·期 34
·12257-12265
·
IF 8.067
Jiaoyan Shi,Qiu Zhuang,Lipeng Wu,Ronghui Guo,Ling Huang,Weijin Li,Fan Wu,Aming Xie
Dielectric resonance tuning could improve the electromagnetic wave absorption (EMA) properties of materials; however, current strategies for dielectric resonance tuning are scarcely reported. Herein, we proposed a molecular engineering concept to obtain derived carbon materials via controlling the number of aromatic rings and steric/geometric structure of methylene inserted aromatic polymers (MAPs). The derived carbon materials are composed of repeat units, existing analogous dipole polarization, and further creating dielectric resonance loss, making the resultant MAP-derived carbon materials (MAPCs) demonstrate outstanding EMA performance. Particularly, the effective absorption bandwidth of MAPC-6 can reach 7.1 GHz, which is superior to that of state-of-the-art carbon materials. This work demonstrates the EMA ability can be significantly optimized through the molecular engineering structural design concept, paving the way to understand and tune the dielectric resonance in carbon materials, and offering promising EMA application perspectives.
研究领域:
材料科学
·
化学工程
✓ 已验证
DOI
高影响因子
MACROMOLECULES
·
2024
·
IF 5.1
Hao Zhan,Hao Zheng,Yongjie Dong,Qingqing Zhao,Xuebing Luo,Juan Peng
Despite recent advances in all-conjugated poly(3-alkylthiophene) (P3AT)-based block copolymers (BCPs) with identical backbones, investigations into the phase behavior of conjugated donor–acceptor (D–A) BCPs containing two disparate backbones are somewhat limited. Herein, we report tailoring the phase behavior of a series of new all-conjugated D–A BCPs, i.e., poly(3-alkylthiophene)-block-poly(isoindigo-alt-bithiophene) (P3AT-b-PII2T), by tuning their intrinsic factors (alkyl chains of P3ATs and block weight ratio of P3AT to PII2T) in conjunction with post thermal annealing. P3ATs include poly(3-hexylthiophene) (P3HT), poly(3-octylthiophene) (P3OT), and poly(3-decylthiophene) (P3DT), where the alkyl chain lengths gradually increase and approach that of PII2T. When the block weight ratio of P3AT to PII2T was approximately 1:1, the larger alkyl chain difference between the P3AT and PII2T blocks and the increased thermal annealing temperature favored microphase segregation (i.e., producing respective P3AT and PII2T crystals) over the crystallization of P3AT and PII2T as one block. Moreover, when the block weight ratios of P3OT to PII2T in P3OT-b-PII2T were changed to approximately 4:1 and 1:4, the major component dominated the crystallization of the entire BCPs, with depressed crystallization of the other minor component. The rule that similar alkyl chain length and a comparable block weight ratio between P3AT and PII2T favor their crystallization as one block can be readily extended to another conjugated D–A BCP, that is, poly(3-alkylthiophene)-block-poly(naphthalene diimide-alt-bithiophene) (P3AT-b-PNDI2T). This study highlights the phase behaviors in P3AT-b-PII2T and P3AT-b-PNDI2T BCPs tuned by synergistic molecular engineering and post thermal treatment, which could strengthen the fundamental understanding of conjugated D–A BCPs for their application in organic optoelectronic devices.
研究领域:
材料科学
·
高分子化学
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产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Yingjie Wang,Jinhang Zou,Congyu Zhao,Haipeng Jiang,Yuhuan Song,Le Zhang,Xin Li,Fengyou Wang,Lin Fan,Xiaoyan Liu,Maobin Wei,Lili Yang
Effective defect passivation and efficient charge transfer within polycrystalline perovskite grains and corresponding boundaries are necessary to achieve highly efficient perovskite solar cells (PSCs). Herein, focusing on the boundary location of g-C3N4 during the crystallization modulation on perovskite, molecular engineering of 4-carboxyl-3-fluorophenylboronic acid (BF) on g-C3N4 was designed to obtain a novel additive named BFCN. With the help of the strong bonding ability of BF with both g-C3N4 and perovskite and favorable intramolecular charge transfer within BFCN, not only has the crystal quality of perovskite films been improved due to the effective defects passivation, but the charge transfer has also been greatly accelerated due to the formation of additional charge transfer channels on the grain boundaries. As a result, the champion BFCN-based PSCs achieve the highest photoelectric conversion efficiency (PCE) of 23.71% with good stability.
研究领域:
材料科学
·
能源技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2024
·Vol. 34
·期 16
·2313241
·
IF 18.5
Cuicui Li,Liang Hu,Xiuyun Ren,Lu Lin,Changzhen Zhan,Qingsong Weng,Xiaoqi Sun,Xiaoliang Yu
Small molecule quinone compounds are attractive cathode materials for rechargeable aqueous zinc-organic batteries (AZOBs) because of their structural diversity and low-cost merits. Among them, nonpolar quinones are dominant given the relatively low solubilities in aqueous electrolytes. However, their poor electronic conductivity and accumulated Coulombic repulsion lead to underutilized active sites and sluggish redox kinetics. Here, polar 2,6-dimethoxy-1,4-benzoquinone ( m -DMBQ) works as an advanced AZOB cathode with unexpectedly superior performance over the nonpolar isomer of 2,5-dimethoxy-1,4-benzoquinone ( p -DMBQ). The asymmetric charge distribution of active centers in the p−π conjugated backbone of m -DMBQ induces reduced bandgap with improved electronic conductivity and redox activity, thus achieving a high specific capacity of 312 mAh g −1 approaching the theoretical limit. Additionally, the lowest unoccupied molecular orbital energy level is lowered for an increased average discharge voltage of 0.88 V. Characterizations and computational studies revealed boosted competitiveness of H + relative to Zn 2+ for significantly enhanced charge transfer kinetics and reversibility. As a result, the as-fabricated AZOB achieves a high energy density of 275 Wh kg −1 based on m -DMBQ along with high-rate capability and long-term cycling stability. This work provides a new molecular engineering strategy through regulating charge distribution symmetry for boosting charge storage in organic cathodes.
研究领域:
材料科学
·
电化学
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产品关联
DOI
高影响因子
ACS Nano
·
2024
·
IF 15.8
Feier Niu,Zhongchao Bai,Junming Chen,Qinfen Gu,Xuchun Wang,Jumeng Wei,Yueyuan Mao,Shi Xue Dou,Nana Wang
Rechargeable aqueous zinc ion batteries (AZIBs) have gained considerable attention owing to their low cost and high safety, but dendrite growth, low plating/stripping efficiency, surface passivation, and self-erosion of the Zn metal anode are hindering their application. Herein, a one-step in situ molecular engineering strategy for the simultaneous construction of hierarchical MoS2 double-layer nanotubes (MoS2-DLTs) with expanded layer-spacing, oxygen doping, structural defects, and an abundant 1T-phase is proposed, which are designed as an intercalation-type anode for “rocking-chair” AZIBs, avoiding the Zn anode issues and therefore displaying a long cycling life. Benefiting from the structural optimization and molecular engineering, the Zn2+ diffusion efficiency and interface reaction kinetics of MoS2-DLTs are enhanced. When coupled with a homemade ZnMn2O4 cathode, the assembled MoS2-DLTs//ZnMn2O4 full battery exhibited impressive cycling stability with a capacity retention of 86.6% over 10 000 cycles under 1 A g–1anode, outperforming most of the reported “rocking-chair” AZIBs. The Zn2+/H+ cointercalation mechanism of MoS2-DLTs is investigated by synchrotron in situ powder X-ray diffraction and multiple ex situ characterizations. This research demonstrates the feasibility of MoS2 for Zn-storage anodes that can be used to construct reliable aqueous full batteries.
研究领域:
材料科学
·
能源存储技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）