يعرض 1 - 10 نتائج من 15 نتيجة بحث عن '"Zhihua Lin"', وقت الاستعلام: 0.74s تنقيح النتائج
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    المصدر: The Journal of Organic Chemistry. 87:351-362

    الوصف: Compared with the impressive achievements of catalytic carbonyl-olefin metathesis (CCOM) mediated by Lewis acid catalysts, exploration of the CCOM through Brønsted acid-catalyzed approaches remains quite challenging. Herein, we disclose a synthetic protocol for the construction of a valuable polycycle scaffold through the CCOM with the inexpensive, nontoxic phosphomolybdic acid as a catalyst. The current annulations could realize carbonyl-olefin, carbonyl-alcohol, and acetal-alcohol in situ CCOM reactions and feature mild reaction conditions, simple manipulation, and scalability, making this strategy a promising alternative to the Lewis acid-catalyzed COM reaction.

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    المصدر: Inorganic Chemistry. 60:12129-12135

    الوصف: To date, numerous zirconium cluster-based metal-organic frameworks (Zr-MOFs) with attractive physical properties have been achieved thanks to tailorable organic linkers and versatile Zr clusters. Nevertheless, in comparison with the most-used high-symmetry organic linkers, low-symmetry linkers have rarely been exploited in the construction of Zr-MOFs. Despite challenges in predicting the structure and topology of the MOF, linker desymmetrization presents opportunities for the design of Zr-MOFs with unusual topologies and unexpected functionalities. Herein, we report for the first time the construction of two robust Zr-MOFs (IAM-7 and IAM-8) from two pyrrolo-pyrrole-based low-symmetry tetracarboxylate linkers with a rare rhombic shape. The low symmetry of the linkers arises from the asymmetric pyrrolo-pyrrole core and the varying branch lengths, which play a critical role in the structural diversity between IAM-7 and IAM-8 seen from the structural analysis and lead to hydrophilic channels that contain uncoordinated carboxylate groups in the structure of IAM-7. Furthermore, the proton conductivity of IAM-7 displays a high temperature and humidity dependence where the proton conductivity increases from 2.84 × 10-8 S cm-1 at 30 °C and 40% relative humidity (RH) to 1.42 × 10-2 S cm-1 at 90 °C and 95% RH, making it among one of the most conductive Zr-MOFs. This work not only enriches the library of Zr-MOFs but also offers a platform for the design of low-symmetry linkers toward the structural diversity or irregularity of MOFs as well as their structure-related properties.

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    المصدر: ACS Applied Materials & Interfaces. 12:18715-18722

    الوصف: Through an "isoreticular expansion" strategy, a large number of highly porous zirconium-based metal-organic frameworks (Zr-MOFs) have been achieved using extended organic linkers in the past few years. However, interpenetrated Zr-MOFs with ftw topology have scarcely been reported, mainly owing to the used bulky tetratopic linkers that effectively prevent the network interpenetration. Here, we report a new family of zirconium and lanthanide (Ln) MOFs with ftw topology, constructed by hexanuclear Zr or Ln (Ln = Eu, Tb, Gd, Dy, Tm, Yb, Nd, and Er) clusters and a spirobifluorene-center tetracarboxylate linker. Our studies reveal that the isostructural Zr and Ln MOFs are all doubly interpenetrated with ultrahigh thermal and chemical stability. The observed unusual interpenetration can be attributed to the specific geometry of the spirobifluorene-center tetratopic linker. Gas adsorption studies show that the interpenetrated Zr-MOF is still highly porous and exhibits high performance for CO2 storage, which can be attributed to the strong CO2 binding environment contributed by the reduced pore size. In addition, the presented MOFs display strong characteristic luminescence in the UV-vis-NIR region. Moreover, the incorporation of the spiro-center linker into the framework can efficiently produce two-photon-excited photoluminescence with a large action cross-section value, which also benefited from the high packing density of the nonlinear optical chromophore linker in the interpenetrated structure.

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    المصدر: Langmuir. 36:7039-7045

    الوصف: We report a carbonaceous nanomotor with a characteristic flask-like hollow structure that can autonomously move under the propulsion of oxygen bubbles. The carbonaceous nanoflask (CNF) motor was fabricated by encapsulating platinum nanoparticles (Pt NPs) into the hollow cavity of the CNF. The internally encapsulated Pt NPs act as catalysts to decompose hydrogen peroxide (H2O2) fuel into oxygen bubbles. The generated oxygen bubbles recoil the motion of the CNF motors. Besides, the velocity of CNF motors can be controlled by adjusting the concentration of the H2O2 solution. The motion velocity increases with the increase of H2O2 concentration, up to 109.25 μm s-1 at 10% H2O2. This study provides important implications for understanding the motion behaviors of nanomotors with an internal cavity, and the self-propelled CNF motors as smart carrier systems have potential applications in the future.

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    المصدر: ACS Nano. 13:12758-12766

    الوصف: Chemically driven colloidal motors capable of implementing different movements under a common environment are of great importance for various complex tasks. However, the key parameters underlying different motion behaviors are incompletely understood. Here, we demonstrate that carbonaceous nanoflask (CNF) motors move spontaneously in glucose powered by the cascade reaction of glucose oxidase and catalase, and their directional propulsion can be premeditated by controlling the surface wettability of nanomotors. The hydrophilic CNF motors move from the round-bottom to the opening neck (backward), whereas the hydrophobic CNF motors swim from the opening neck to the round-bottom (forward). We demonstrate that the backward motion of the hydrophilic CNF motors is driven by the local glucose gradient due to self-diffusiophoresis, and the forward movement of the hydrophobic CNF motors is caused by the locally produced glucose acid gradient. The fluid simulation reveals that the hydrophilic and hydrophobic CNF motors correspond to the puller and pusher models, respectively. Our study offers a minimal strategy to manipulate the direction of motion of motors for specific applications and to change the hydrodynamic behaviors of glucose-powered motors.

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    المصدر: Inorganic Chemistry. 58:12748-12755

    الوصف: Presented herein is a group of highly stable Zr-based metal-organic frameworks with bowl-shaped dihydroanthracene-based tetratopic linkers as building blocks. Structural analysis reveals that these frameworks are all two-dimensional but comprise three distinct connectivities of Zr6 nodes. By using the steric hindrance of the nonplanar linker, the connectivity of Zr6 node can be tuned from 8-c to unusual 4-c. Further, through either one-pot synthesis or postsynthetic linker installation strategies, the connectivity of Zr6 node can be tuned from 8-c to 10-c by the insertion of a secondary linear dicarboxylate linker, from which not only the temperature-dependent flexibility of the structure can be effectively controlled with enhanced rigidity and thermal stability but also a scaffold for postsynthetic metalation of Pd(II) catalyst for Heck coupling reaction is offered.

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    المصدر: ACS Applied Materials & Interfaces. 11:23392-23400

    الوصف: Photodynamic therapy (PDT) is a promising cancer therapeutic strategy, which typically kills cancer cells through converting nontoxic oxygen into reactive oxygen species using photosensitizers (PSs). However, the existing PDTs are still limited by the tumor hypoxia and poor targeted accumulation of PSs. To address these challenges, we here report an acoustically powered and magnetically navigated red blood cell-mimicking (RBCM) micromotor capable of actively transporting oxygen and PS for enhanced PDT. The RBCM micromotors consist of biconcave RBC-shaped magnetic hemoglobin cores encapsulating PSs and natural RBC membrane shells. Upon exposure to an acoustic field, they are able to move in biological media at a speed of up to 56.5 μm s-1 (28.2 body lengths s-1). The direction of these RBCM micromotors can be navigated using an external magnetic field. Moreover, RBCM micromotors can not only avoid the serum fouling during the movement toward the targeted cancer cells but also possess considerable oxygen- and PS-carrying capacity. Such fuel-free RBCM micromotors provide a new approach for efficient and rapid active delivery of oxygen and PSs in a biofriendly manner for future PDT.

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    المصدر: Inorganic Chemistry. 57:6210-6213

    الوصف: We present here the synthesis of one enantiomeric pair of metal-organic framework materials comprised of a unique multioriented double-helix structure from an achiral spirocenter ligand. Our study clearly shows that the chiral MOF material encompasses concurrently multiple nonlinear-optical functions in the solid state: the noncentrosymmetric structural feature brings the chiral MOF high second-harmonic-generation efficiency; the incorporation of the spirocenter ligand can efficiently produce two-photon-excited photoluminescence with a larger-action cross-sectional value.

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    المصدر: ACS Nano. 12:2539-2545

    الوصف: We report a magnetically actuated peanut-shaped hematite colloid motor that can not only move in a rolling or wobbling mode in fluids but also perform single cell manipulation and patterning in a noncontact way. The peanut motor in a rolling mode can reach a maximal velocity of 10.6 μm s–1 under a rotating magnetic field of 130 Hz and 6.3 mT and achieve a more precisely controllable motion in predefined tracks. While in a wobbling mode, the motor reaches a maximal velocity of 14.5 μm s–1 under a conical rotating magnetic field of 80 Hz and 6.3 mT and can climb over steep slopes to adapt the motor for more complex environments. The fluid flow simulation results reveal that the difference between two movement modes mostly comes from the distribution discrepancy of the flow fields near the motors. Through the integration of the rolling and wobbling movement, these peanut motors can autonomously transport and release cells to a predefined site and thus form complex cell patterns without a physical contact. Su...