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【最新中稿作品】超疏水表面、光催化、生物传感核酸、肿瘤免疫

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题目:A Reactive Superhydrophobic Platform for Living Photolithography

作者:Xinjian Xie,Xinghao Chen,Pavel A. Levkin,Wenqian Feng

https://doi.org/10.1002/adma.202203619

具有区域功能的超疏水表面在生物技术、诊断应用、微化学合成和分析等领域有着广泛的应用。然而,由于它们的化学惰性,具有化学反应性的超疏水表面很难实现。可以用不同的密度和扩展种类的功能部分进一步改性的超疏水表面并不容易获得。

四川大学冯文骞研究员团队采用甲基丙烯酸2-(2-溴代异丁酰氧基)乙酯(BrMA)分子作为活性疏水单体,利用光引发相分离法一步制备出具有化学活性的超疏水聚合物表面。该表面在三(2-苯基吡啶)合铱(Ir(ppy) 3)的催化下,利用可见光(460 nm)轻松实现不同功能单体(如丙烯酸酯类单体)的表面原子转移自由基聚合(SI-ATRP)以及原子转移自由基加成(SI-ATRA),实现表面功能分子的可控修饰。该团队同时利用搭载数字光处理光刻设备(DLP printer或者LCD printer)实现了表面功能分子接枝密度、接枝链段(单段或多段)、以及接枝区域的高精度调控,从而赋予该表面高疏油特性,梯度刺激响应性以及蛋白酶催化剂的捕获特性,验证了在高通量筛选、多重防伪以及微流体生物芯片等领域的应用潜力。

图1. 活性超疏水表面制备方法以及表面光控修饰机理。

中稿作品 · 精选

▲1丨Vol.61 No.37 September 12, 2022

标题Title

Chromophore-Inspired Design of Pyridinium-Based Metal–Organic Polymers for Dual Photoredox Catalysis

摘要Abstract(滑动查看)

Endowing artificial advanced materials and systems with biomimetic self-regulatory intelligence is of paramount significance for the development of somatosensory soft robotics and adaptive optoelectronics. Herein, a bioinspired 2,4,6-Triphenylpyrylium (TPT+) functions as a classic organic photocatalyst and exhibits a noteworthy absorption in the visible range, strongly oxidizing excited states, and a somewhat unstable structure. Inspired by the nuclear chromophore and dual catalysis strategy, herein, we report a universal photoredox platform constructed by TPT+-mimic bridging ligands and reductive metal ions on the basis of metal–organic supramolecular systems for various organic couplings and molecular oxygen activation under visible-light irradiation. Significant photoinduced electron transfer and ligand-to-metal charge-transfer events are both integrated and regulated by the spatial and kinetic confinement effects of the structurally confined microenvironments, effectively improving the efficiency of electron transfer and radical–radical coupling processes in photocatalysis. This package deal provides a promising way for the design of novel photocatalysts and the development of versatile and sustainable synthetic chemistry. phototropism like a hollow stem of plants in nature. As a proof-of-concept demonstration, an adaptive photovoltaic system with solar energy harvesting maximization is illustrated. This work can provide insights into the development of artificial intelligent materials toward adaptive optoelectronics, intelligent soft robotics, and beyond.

封面论文链接:

https://doi.org/10.1002/anie.202204918

▲2丨Vol.32 No.37 September 12, 2022

标题Title

Biointerface Engineering with Nucleic Acid Materials for Biosensing Applications

摘要Abstract(滑动查看)

Molecular recognition at the biointerface plays a critical role in sensing molecular interactions (e.g., DNA hybridization) and extracellular changes, which can directly affect the detection performance of biosensors (e.g., sensitivity, specificity, and response dynamics). However, conventional sensing biointerfaces show low molecular recognition efficiency due to limited target accessibility. Engineering sensing biointerfaces to regulate the orientation, spacing, and density of surface-confined molecular probes offer an effective approach to improve molecular recognition at interfaces. Over the last decades, biointerface engineering with nucleic acid materials has advanced the fundamental understanding of DNA hybridization kinetics and facilitated the design of improved biosensing platforms for monitoring cellular activities and diagnosing relevant diseases. This review summarizes the recent progress in nucleic acid-based biointerface engineering. The development of nucleic acid materials that can be applied to specific diagnostic applications is briefly introduced. Then the roles of nucleic acids in tailoring the properties of nanosurfaces, cell surfaces, and macroscopic surfaces are discussed and their biosensing applications are comprehensively highlighted. Finally, future challenges and perspectives of emerging technologies and applications in the field are presented.

封面论文链接:

https://doi.org/10.1002/adfm.202201069

▲3丨Vol.22 No.17 September 14, 2022

标题Title

Programmable Bispecific Nano-immunoengager That Captures T Cells and Reprograms Tumor Microenvironment

摘要Abstract(滑动查看)

Immune checkpoint blockade (ICB) therapy has revolutionized clinical oncology. However, the efficacy of ICB therapy is limited by the ineffective infiltration of T effector (Teff) cells to tumors and the immunosuppressive tumor microenvironment (TME). Here, we report a programmable tumor cells/Teff cells bispecific nano-immunoengager (NIE) that can circumvent these limitations to improve ICB therapy. The peptidic nanoparticles (NIE-NPs) bind tumor cell surface α3β1 integrin and undergo in situ transformation into nanofibrillar network nanofibers (NIE-NFs). The prolonged retained nanofibrillar network at the TME captures Teff cells via the activatable α4β1 integrin ligand and allows sustained release of resiquimod for immunomodulation. This bispecific NIE eliminates syngeneic 4T1 breast cancer and Lewis lung cancer models in mice, when given together with anti-PD-1 antibody. The in vivo structural transformation-based supramolecular bispecific NIE represents an innovative class of programmable receptor-mediated targeted immunotherapeutics to greatly enhance ICB therapy against cancers.

封面论文链接:

https://doi.org/10.1021/acs.nanolett.2c00582

▲4丨Vol.434 No.19 October 12, 2022

封面期刊链接:

https://www.sciencedirect.com/journal/journal-of-molecular-biology

▲5丨Vol.32 No.26 June 24, 2022

期刊链接:

https://www.sciencedirect.com/journal/journal-of-materials-science-and-technology/issues

▲6丨Vol.40 No.20 October 15, 2022

标题Title

Palladium-Catalyzed Intramolecular Dehydrogenative Arylboration of Alkenes

摘要Abstract(滑动查看)

The palladium-catalyzed borylative cyclization via C—H activation has been developed. By this chemistry, the indole-fused dihydro-pyrrole motif, which is a kind of important unit in natural products and bio-active molecules, could be constructed and installed with a boric ester group. Furthermore, the utilities of products have been illustrated by the study of further transformations. Importantly, by using chiral ligand, the enantioselectivity of this borylative cyclization reaction could be controlled. Moreover, the borylative mechanism, which should proceed through a Pd(II)/Pd(IV) catalytic cycle, has been proposed based on the DFT calculations.

封面论文链接:

https://doi.org/10.1002/cjoc.202200317

▲7 No.3 June, 2022

封面期刊链接:

https://spj.sciencemag.org/ultrafastscience/

▲8丨Vol.6 No.6 March 2022

标题Title

Structure-performance interplay of rhodium-based catalysts for syngas conversion to ethanol

摘要Abstract(滑动查看)

Ethanol as a fuel additive and energy carrier has been received much attention recently due to the importance of carbon neutralization and reduction of carbon emissions. The current ethanol product strongly relies on grain fermentation, which competes with human food. The conversion of syngas (a mixture of CO and H2) to ethanol has provided an alternative route that avoids competition with food. In this process, rhodium nanoparticle catalysts have exhibited unique catalytic properties, but there is still a gap in meeting the demand. The performances of these catalysts are strongly related to the geometric and electronic structures of the Rh species, where the controlled cleavage of C–O in CO, hindered deep hydrogenation to methane, and selective C–C coupling to ethanol are highly desirable. This review discusses the reaction mechanism of Rh-catalyzed ethanol production from syngas and summarizes the recent progress in Rh catalysts related to improving catalytic activity, ethanol selectivity, and durability. Based on these results, the structure-performance interplay of rhodium-based catalysts is briefly concluded. Particularly, zeolite-fixed Rh-based nanoparticles are highlighted, which might guide the development of more efficient catalysts via Rh-zeolite synergism.

封面论文链接:

https://doi.org/10.1039/D1QM01457A

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