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571.
Wenyuan Lyu Dr. Yang Liu Jingyi Zhou Datong Chen Dr. Xin Zhao Dr. Ruiqi Fang Dr. Fengliang Wang Prof. Yingwei Li 《Angewandte Chemie (International ed. in English)》2023,62(42):e202310733
Photocatalytic conversion of low-concentration CO2 is considered as a promising way to simultaneously mitigate the environmental and energy issues. However, the weak CO2 adsorption and tough CO2 activation process seriously compromise the CO production, due to the chemical inertness of CO2 molecule and the formed fragile metal-C/O bond. Herein, we designed and fabricated oxygen vacancy contained Co3O4 hollow nanoparticles on ordered macroporous N-doped carbon framework (Vo−HCo3O4/OMNC) towards photoreduction of low-concentration CO2. In situ spectra and ab initio molecular dynamics simulations reveal that the constructed oxygen vacancy is able to break the local structural symmetry of Co−O−Co sites. The formation of asymmetric active site switches the CO2 configuration from a single-site linear model to a multiple-sites bending one with a highly stable configuration, enhancing the binding and structural polarization of CO2 molecules. As a result, Vo−HCo3O4/OMNC shows unprecedent activity in the photocatalytic conversion of low-concentration CO2 (10 % CO2/Ar) under laboratory light source or even natural sunlight, affording a syngas yield of 337.8 or 95.2 mmol g−1 h−1, respectively, with an apparent quantum yield up to 4.2 %. 相似文献
572.
Shiwei Tao Dr. Baris Demir Dr. Ardeshir Baktash Yutong Zhu Dr. Qingbing Xia Prof. Yalong Jiao Yuying Zhao Dr. Tongen Lin Dr. Ming Li Dr. Miaoqiang Lyu Prof. Ian Gentle Prof. Lianzhou Wang Dr. Ruth Knibbe 《Angewandte Chemie (International ed. in English)》2023,62(39):e202307208
The irreversibility of anion intercalation-deintercalation is a fundamental issue in determining the cycling stability of a dual-ion battery (DIB). In this work, we demonstrate that using a partially fluorinated carbonate solvent can drive a beneficial fluorinated secondary interphase layer formation. Such layer facilitates reversible anion (de−)intercalation processes by impeding solvent molecule co-intercalation and the associated graphite exfoliation. The enhanced reversibility of anion transport contributes to the overall cycling stability for a Zn-graphite DIB—a high Coulombic efficiency of 98.5 % after 800 cycles, with an attractive discharge capacity of 156 mAh g−1 and a mid-point discharge voltage of ≈1.7 V (at 0.1 A g−1). In addition, the formed fluorinated secondary interphase suppresses the self-discharge behavior, preserving 29 times of the capacity retention rate compared to the battery with a commonly used carbonate solvent, after standing for 24 hours. This work provides a simple and effective strategy for addressing the critical challenges in graphite-based DIBs and contributes to fundamental understanding to help accelerate their practical application. 相似文献
573.
Dr. Wentao Xu Dr. Nikita Hanikel Dr. Kirill A. Lomachenko Dr. Cesare Atzori Dr. Alicia Lund Dr. Hao Lyu Zihui Zhou Prof. Dr. C. Austen Angell Prof. Dr. Omar M. Yaghi 《Angewandte Chemie (International ed. in English)》2023,62(16):e202300003
We report a synthetic strategy to link titanium-oxo (Ti-oxo) clusters into metal-organic framework (MOF) glasses with high porosity though the carboxylate linkage. A new series of MOF glasses was synthesized by evaporation of solution containing Ti-oxo clusters Ti16O16(OEt)32, linkers, and m-cresol. The formation of carboxylate linkages between the Ti-oxo clusters and the carboxylate linkers was confirmed by Fourier-transform infrared (FT-IR) spectroscopy. The structural integrity of the Ti-oxo clusters within the glasses was evidenced by both X-ray absorption near edge structure (XANES) and 17O magic-angle spinning (MAS) NMR. After ligand exchange and activation, the fumarate-linked MOF glass, termed Ti-Fum, showed a N2 Brunauer–Emmett–Teller (BET) surface areas of 923 m2 g−1, nearly three times as high as the phenolate-linked MOF glass with the highest BET surface area prior to this report. 相似文献
574.
Li Ji Cui Xiancai Lin Qilang Lyu Xiaolin Wang Qian Yu Yan Yang Chengkai 《Journal of Solid State Electrochemistry》2023,27(6):1383-1389
Journal of Solid State Electrochemistry - As people possess more safety conscious, the issue of electrolytes is attracting concern. The gel polymer electrolyte offers high ionic conductivity,... 相似文献
575.
Shan Erfang Yu Zhiqiang Lyu Wenrong 《4OR: A Quarterly Journal of Operations Research》2023,21(3):533-545
4OR - The egalitarian principle has been widely adopted in designing solution concepts for cooperative games. In light of egalitarianism, we introduce two egalitarian values satisfying union... 相似文献
576.
Dr. Yu Zhang Dr. Shaobo Han Dr. Shangqian Zhu Dr. Ruhui Chen Tiehuai Li Dr. Zhiheng Lyu Dr. Ming Zhao Prof. Dr. Meng Gu Prof. Dr. Minhua Shao Prof. Dr. Younan Xia 《Angewandte Chemie (International ed. in English)》2023,62(52):e202314634
Surface ligands play an important role in shape-controlled growth and stabilization of colloidal nanocrystals. Their quick removal tends to cause structural deformation and/or aggregation to the nanocrystals. Herein, we demonstrate that the surface ligand based on poly(vinylpyrrolidone) (PVP) can be slowly removed from Pd nanosheets (NSs, 0.93±0.17 nm in thickness) by simply aging the colloidal suspension. The aged Pd NSs show well-preserved morphology, together with significantly enhanced stability toward both e-beam irradiation and electrocatalysis (e.g., ethanol oxidation). It is revealed that the slow desorption of PVP during aging forces the re-exposed Pd atoms to reorganize, facilitating the surface to transform from being nearly perfect to defect-rich. The resultant Pd NSs with abundant defects no longer rely on surface ligand to stabilize the atomic arrangement and thus show excellent structural and electrochemical stability. This work provides a facile and effective method to maintain the integrity of colloidal nanocrystals by slowly removing the surface ligand. 相似文献
577.
Dr. Jing Lyu Yinghao Li Zishan Li Prof. Piotr Polanowski Prof. Jeremiasz K. Jeszka Prof. Krzysztof Matyjaszewski Prof. Wenxin Wang 《Angewandte Chemie (International ed. in English)》2023,62(5):e202212235
Radical polymerization (RP) of multivinyl monomers (MVMs) provides a facile solution for manipulating polymer topology and has received increasing attention due to their industrial and academic significance. Continuous efforts have been made to understand their mechanism, which is the key to regulating materials structure. Modelling techniques have become a powerful tool that can provide detailed information on polymerization kinetics which is inaccessible by experiments. Many publications have reported the combination of experiments and modelling for free radical polymerization (FRP) and reversible-deactivation radical polymerizations (RDRP) of MVMs. Herein, a minireview is presented for the most important modelling techniques and their applications in FRP/RDRP of MVMs. This review hopes to illustrate that the combination of modelling and wet experiments can be a great asset to polymer researchers and inspire new thinking for the future MVMs experiment optimization and product design. 相似文献
578.
In signal quantization, it is well-known that introducing adaptivity to quantization schemes can improve their stability and accuracy in quantizing bandlimited signals. However, adaptive quantization has only been designed for one-dimensional signals. The contribution of this paper is two-fold: (i) we propose the first family of two-dimensional adaptive quantization schemes that maintain the same mathematical and practical merits as their one-dimensional counterparts, and (ii) we show that both the traditional 1-dimensional and the new 2-dimensional quantization schemes can effectively quantize signals with jump discontinuities, which immediately enable the usage of adaptive quantization on images. Under mild conditions, we show that by using adaptivity, the proposed method is able to reduce the quantization error of images from the presently best to the much smaller , where s is the number of jump discontinuities in the image and P () is the total number of samples. This -fold error reduction is achieved via applying a total variation norm regularized decoder, whose formulation is inspired by the mathematical super-resolution theory in the field of compressed sensing. Compared to the super-resolution setting, our error reduction is achieved without requiring adjacent spikes/discontinuities to be well-separated, which ensures its broad scope of application. We numerically demonstrate the efficacy of the new scheme on medical and natural images. We observe that for images with small pixel intensity values, the new method can significantly increase image quality over the state-of-the-art method. © 2022 Wiley Periodicals, Inc. 相似文献
579.
Acta Mechanica Sinica - The turbulent Poiseuille flow between two parallel plates is one of the simplest possible physical situations, and it has been studied intensively. In this paper, we propose... 相似文献