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121.
Taotao Feng Wenliang Ji Yue Zhang Fei Wu Qiao Tang Huan Wei Prof. Lanqun Mao Prof. Meining Zhang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(52):23651-23655
Electrochemical sensing performance is often compromised by electrode biofouling (e.g., proteins nonspecific binding) in complex biological fluids; however, the design and construction of a robust biointerface remains a great challenge. Herein, inspired by nature, we demonstrate a robust polydopamine-engineered biointerfacing, to tailing zwitterionic molecules (i.e., sulfobetaine methacrylate, SBMA) through Michael Addition. The SBMA-PDA biointerface can resist proteins nonspecific binding in complex biological fluids while enhancing interfacial electron transfer and electrochemical stability of the electrode. In addition, this sensing interface can be integrated with tissue-implantable electrode for in vivo analysis with improved sensing performance, preserving ca. 92.0% of the initial sensitivity after 2 h of implantation in brain tissue, showing low acute neuroinflammatory responses and good stability both in normal and in Parkinson′s disease (PD) rat brain tissue. 相似文献
122.
Prof. Ping Yu Huan Wei Peipei Zhong Yifei Xue Dr. Fei Wu Dr. Yang Liu Prof. Junjie Fei Prof. Lanqun Mao 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(50):22841-22847
The development of new principles and techniques with high neuronal compatibility for quantitatively monitoring the dynamics of neurochemicals is essential for deciphering brain chemistry and function but remains a great challenge. We herein report a neuron-compatible method for in vivo neurochemical sensing by powering a single carbon fiber through spontaneous bipolar electrochemistry as a new sensing platform. By using ascorbic acid as a model target to prove the concept, we found that the single-carbon-fiber-powered microsensor exhibited a good response, high stability and, more importantly, excellent neuronal compatibility. The microsensor was also highly compatible with electrophysiological recording, thus enabling the synchronous recording of both chemical and electrical signals. The sensing principle could be developed for in vivo monitoring of various neurochemicals in the future by rationally designing and tuning the electrochemical reactions at the two poles of the carbon fiber. 相似文献
123.
Dr. Li-Li Wang Dr. Mao Quan Ti-Long Yang Zhao Chen Prof. Dr. Wei Jiang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(52):24025-24032
Optical chirality sensing has attracted a lot of interest due to its potential in high-throughput screening in chirality analysis. A molecular sensor is required to convert the chirality of analytes into optical signals. Although many molecular sensors have been reported, sensors with wide substrate scope remain to be developed. Herein, we report that the amide naphthotube-based chirality sensors have an unprecedented wide scope for chiroptical sensing of organic molecules. The substrates include, but are not limited to common organic products in asymmetric catalysis, chiral molecules with inert groups or remote functional groups from their chiral centers, natural products and their derivatives, and chiral drugs. The effective chirality sensing is based on biomimetic recognition in water and on effective chirality transfer through guest-induced formation of a chiral conformation of the sensors. Furthermore, the sensors can be used in real-time monitoring on reaction kinetics in water and in determining absolute configurations and ee values of the products in asymmetric catalysis. 相似文献
124.
Dr. Feifei You Dr. Jiawei Wan Dr. Jian Qi Dr. Dan Mao Prof. Nailiang Yang Prof. Qinghua Zhang Prof. Lin Gu Prof. Dan Wang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(2):731-734
Precise control of the micro-/nanostructures of nanomaterials, such as hollow multi-shelled structures (HoMSs), has shown its great advantages in various applications. Now, the crystal structure of building blocks of HoMSs are controlled by introducing the lattice distortion in HoMSs, for the first time. The lattice distortion located at the nanoscale interface of SnS2/SnO2 can provide additional active sites, which not only provide the catalytic activity under visible light but also improve the separation of photoexcited electron–hole pairs. Combined with the efficient light utilization, the natural advantage of HoMSs, a record catalytic activity was achieved in solid–gas system for CO2 reduction, with an excellent stability and 100 % CO selectivity without using any sensitizers or noble metals. 相似文献
125.
Dr. Fang Hu Guobin Qi Dr. Kenry Dr. Duo Mao Dr. Shiwei Zhou Dr. Min Wu Dr. Wenbo Wu Prof. Bin Liu 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(24):9374-9378
Protected by the host cells, the hidden intracellular bacteria are typically difficult to kill by common antibiotics and cannot be visualized without complex cellular pretreatments. Herein, we successfully developed a bacteria-metabolizable dual-functional probe TPEPy-d -Ala, which is based on d -alanine and a photosensitizer with aggregation-induced emission for fluorescence turn-on imaging of intracellular bacteria in living host cells and photodynamic ablation in situ. Once metabolically incorporated into bacterial peptidoglycan, the intramolecular motions of TPEPy-d -Ala are inhibited, leading to an enhanced fluorescent signal, which allows the clear visualization of the intracellular bacteria. Moreover, TPEPy-d -Ala can effectively ablate the labeled intracellular bacteria in situ owing to covalent ligation to peptidoglycan, yielding a low intracellular minimum inhibitory concentration (MIC) of 20±0.5 μg mL−1, much more efficient than that of a commonly used antibiotic, vancomycin. 相似文献
126.
Yunwen Tao Zheng Pei Nicole Bellonzi Yuezhi Mao Zhu Zou Wanzhen Liang Zhibo Yang Yihan Shao 《International journal of quantum chemistry》2020,120(6):e26123
In the modeling of spin-crossing reactions, it has become popular to directly explore the spin-adiabatic surfaces. Specifically, through constructing spin-adiabatic states from a two-state Hamiltonian (with spin-orbit coupling matrix elements) at each geometry, one can readily employ advanced geometry optimization algorithms to acquire a “transition state” structure, where the spin crossing occurs. In this work, we report the implementation of a fully-variational spin-adiabatic approach based on Kohn-Sham density functional theory spin states (sharing the same set of molecular orbitals) and the Breit-Pauli one-electron spin-orbit operator. For three model spin-crossing reactions (predissociation of N2O, singlet-triplet conversion in CH2, and CO addition to Fe(CO)4), the spin-crossing points were obtained. Our results also indicated the Breit-Pauli one-electron spin-orbit coupling can vary significantly along the reaction pathway on the spin-adiabatic energy surface. On the other hand, due to the restriction that low-spin and high-spin states share the same set of molecular orbitals, the acquired spin-adiabatic energy surface shows a cusp (ie, a first-order discontinuity) at the crossing point, which prevents the use of standard geometry optimization algorithms to pinpoint the crossing point. An extension with this restriction removed is being developed to achieve the smoothness of spin-adiabatic surfaces. 相似文献
127.
Adam Jaffe Stephanie A. Mack Yu Lin Wendy L. Mao Jeffrey B. Neaton Hemamala I. Karunadasa 《Angewandte Chemie (International ed. in English)》2020,59(10):4017-4022
We show that the onset pressure for appreciable conductivity in layered copper‐halide perovskites can decrease by ca. 50 GPa upon replacement of Cl with Br. Layered Cu–Cl perovskites require pressures >50 GPa to show a conductivity of 10?4 S cm?1, whereas here a Cu–Br congener, (EA)2CuBr4 (EA=ethylammonium), exhibits conductivity as high as 2×10?3 S cm?1 at only 2.6 GPa, and 0.17 S cm?1 at 59 GPa. Substitution of higher‐energy Br 4p for Cl 3p orbitals lowers the charge‐transfer band gap of the perovskite by 0.9 eV. This 1.7 eV band gap decreases to 0.3 eV at 65 GPa. High‐pressure X‐ray diffraction, optical absorption, and transport measurements, and density functional theory calculations allow us to track compression‐induced structural and electronic changes. The notable enhancement of the Br perovskite's electronic response to pressure may be attributed to more diffuse Br valence orbitals relative to Cl orbitals. This work brings the compression‐induced conductivity of Cu‐halide perovskites to more technologically accessible pressures. 相似文献
128.
Wenjun Yang Bo Ling Bowen Hu Haolin Yin Jianyou Mao Patrick J. Walsh 《Angewandte Chemie (International ed. in English)》2020,59(1):161-166
An umpolung 1,4‐addition of aryl iodides to enals promoted by cooperative (terpy)Pd/NHC catalysis was developed that generates various bioactive β,β‐diaryl propanoate derivatives. This system is not only the first reported palladium‐catalyzed arylation of NHC‐bound homoenolates but also expands the scope of NHC‐induced umpolung transformations. A diverse array of functional groups such as esters, nitriles, alcohols, and heterocycles are tolerated under the mild conditions. This method also circumvents the use of moisture‐sensitive organometallic reagents. 相似文献
129.
Wei-Er Liu Dr. Mao Quan Hang Zhou Dr. Liu-Pan Yang Prof. H. Y. Au-Yeung Prof. Wei Jiang 《Chemphyschem》2020,21(20):2249-2253
The thermodynamically unstable, colourless closed-ring isomer of spiropyran can be stabilized in water by the anti-configurational isomer of amide naphthotube. The influence of the binding on the thermodynamics and kinetics of spiropyran have been studied. The complex was further used to prepare a test paper that allows naked-eye detection of toxic paraoxon. 相似文献
130.