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61.
Lewis R. Thomas-Hargreaves Yu-Qian Liu Zhong-Hua Cui Sudip Pan Magnus R. Buchner 《Journal of computational chemistry》2023,44(3):397-405
The bonding situation in the tricoordinated beryllium phenyl complexes [BePh3]−, [(pyridine)BePh2] and [(trimethylsilyl-N-heterocyclic imine)BePh2] is investigated experimentally and computationally. Comparison of the NMR spectroscopic properties of these complexes and of their structural parameters, which were determined by single crystal X-ray diffraction experiments, indicates the presence of π-interactions. Topology analysis of the electron density reveals elliptical electron density distributions at the bond critical points and the double bond character of the beryllium-element bonds is verified by energy decomposition analysis with the combination of natural orbital for chemical valence. The present beryllium-element bonds are highly polarized and the ligands around the central atom have a strong influence on the degree of π-delocalization. These results are compared to related triarylboranes. 相似文献
62.
建立了凝胶渗透色谱(GPC)-气相色谱-离子阱质谱同时检测桔梗原药和当归提取物中101种农药残留的分析方法。方法采用乙腈超声辅助提取桔梗原药和当归提取物,浓缩提取液至近干后用乙酸乙酯-环己烷(1∶1, v/v)复溶,采用凝胶渗透色谱法(选取40 cm长、内径20 mm的凝胶渗透色谱柱)对样品进行净化,弃去前段含脂类、色素等杂质的流出液,收集17~30 min洗脱液并旋转蒸发浓缩至近干,甲苯1 mL定容上机。选用DB-5MS毛细管色谱柱分离待测物,通过离子阱质谱实现对101种农药残留的高效检测。方法通过优化前处理条件和离子阱二级质谱参数,有效降低了复杂中药基质对待测化合物的干扰,最大限度提高了样品中农药的定量准确性和回收率,101种农药3水平添加的平均回收率为58.3%~108.9%,每个添加水平10次独立重复测定的相对标准偏差为0.4%~16.5%,检出限(LOD)范围为0.2~40.0 μg/kg,可满足当前韩国、日本、欧洲规定的最大残留限量(maximum residue limits, MRLs)要求。方法具有操作简单快速、灵敏度高、重复性好等特点,凝胶渗透色谱技术的应用克服了固相萃取小柱净化容量不足的弊端,离子阱技术的应用可以进一步排除共流出基体杂质的干扰,提高定量和定性的准确性,检测效果优于常用的气相色谱-质谱法,是对中药中同时分析多种农药残留检测方法的有益补充。 相似文献
63.
Wu Yonglin Cui Hongdi Liu Xiaojuan Zhong Xiaohui Li Zhifeng Wang Chunxiang Dmytro Sydorov 《Journal of Solid State Electrochemistry》2023,27(6):1501-1510
Journal of Solid State Electrochemistry - Ni-rich layered cathode materials LiNixCoyMn(1-x–y)O2 (x ≥ 0.8) suffer from capacity decay due to structural deterioration during... 相似文献
64.
Yunshan Liu Haojie Zhang Wanqing Zhang Prof. Bernard P. Binks Prof. Zhenggang Cui Prof. Jianzhong Jiang 《Angewandte Chemie (International ed. in English)》2023,62(5):e202210050
A ferrocene surfactant can be switched between single and double head form (FcN+C12/Fc+N+C12) triggered by redox reaction. FcN+C12 can neither stabilize an O/W emulsion alone nor an oil-in-dispersion emulsion in combination with alumina nanoparticles due to the steric hindrance of the ferrocene group. However, such steric hindrance can be overcome by increasing the charge density in Fc+N+C12, so that oil-in-dispersion emulsions can be co-stabilized by Fc+N+C12 and alumina nanoparticles at very low concentrations (1×10−7 M (≈50 ppb) and 0.001 wt %, respectively). Not only can reversible formation/destabilization of oil-in-dispersion emulsions be achieved by redox reaction, but also reversible transformation between oil-in-dispersion emulsions and Pickering emulsions can be obtained through reversing the charge of alumina particles by adjusting the pH. The results provide a new protocol for the design of surfactants for stabilization of smart oil-in-dispersion emulsions. 相似文献
65.
Cong Yu Zhengdong Guo Lifeng Yang Jiyu Cui Sen Chen Yawen Bo Xian Suo Qihan Gong Shang Zhang Prof. Xili Cui Shengbao He Prof. Huabin Xing 《Angewandte Chemie (International ed. in English)》2023,62(16):e202218027
Adsorptive separation is an energy-efficient alternative, but its advancement has been hindered by the challenge of industrially potential adsorbents development. Herein, a novel ultra-microporous metal-organic framework ZU-901 is designed that satisfies the basic criteria raised by ethylene/ethane (C2H4/C2H6) pressure swing adsorption (PSA). ZU-901 exhibits an “S” shaped C2H4 curve with high sorbent selection parameter (65) and could be mildly regenerated. Through green aqueous-phase synthesis, ZU-901 is easily scalable with 99 % yield, and it is stable in water, acid, basic solutions and cycling breakthrough experiments. Polymer-grade C2H4 (99.51 %) could be obtained via a simulating two-bed PSA process, and the corresponding energy consumption is only 1/10 of that of simulating cryogenic distillation. Our work has demonstrated the great potential of pore engineering in designing porous materials with desired adsorption and desorption behavior to implement an efficient PSA process. 相似文献
66.
Xiaoyang Chen Dannan Zheng Linye Jiang Zhiguo Wang Xinyu Duan Dong Cui Shuang Liu Yuan Zhang Xiaomin Yu Jingyan Ge Jian Xu 《Angewandte Chemie (International ed. in English)》2023,62(23):e202218140
Chiral sulfones are recurrent motifs in pharmaceuticals and bioactive molecules. Although chemical methods have been developed to afford α- or β- chiral sulfones, these protocols rely heavily on the pre-synthesis of structurally complicated starting materials and chiral metal complexes. Herein, we described a photoenzymatic approach for the radical-mediated stereoselective hydrosulfonylation. Engineered variants of ene reductases provide efficient biocatalysts for this transformation, enabling to achieve a series of β-chiral sulfonyl compounds with high yields (up to 92 %) and excellent e.r. values (up to 99 : 1). 相似文献
67.
Lei Lv Ruihu Lu Jiexin Zhu Ruohan Yu Dr. Wei Zhang Enhui Cui Xingbao Chen Yuhang Dai Lianmeng Cui Dr. Jiong Li Prof. Liang Zhou Prof. Wei Chen Dr. Ziyun Wang Prof. Liqiang Mai 《Angewandte Chemie (International ed. in English)》2023,62(25):e202303117
Bismuth-based materials have been recognized as promising catalysts for the electrocatalytic CO2 reduction reaction (ECO2RR). However, they show poor selectivity due to competing hydrogen evolution reaction (HER). In this study, we have developed an edge defect modulation strategy for Bi by coordinating the edge defects of bismuth (Bi) with sulfur, to promote ECO2RR selectivity and inhibit the competing HER. The prepared catalysts demonstrate excellent product selectivity, with a high HCOO− Faraday efficiency of ≈95 % and an HCOO− partial current of ≈250 mA cm−2 under alkaline electrolytes. Density function theory calculations reveal that sulfur tends to bind to the Bi edge defects, reducing the coordination-unsaturated Bi sites (*H adsorption sites), and regulating the charge states of neighboring Bi sites to improve *OCHO adsorption. This work deepens our understanding of ECO2RR mechanism on bismuth-based catalysts, guiding for the design of advanced ECO2RR catalysts. 相似文献
68.
Xiaoyu Liu Haolin Lu Prof. Shengli Zhu Prof. Zhenduo Cui Prof. Zhaoyang Li Prof. Shuilin Wu Prof. Wence Xu Prof. Yanqin Liang Prof. Guankui Long Prof. Hui Jiang 《Angewandte Chemie (International ed. in English)》2023,62(13):e202300800
It is challenging to design one non-noble material with balanced bifunctional performance for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) for commercial sustainability at a low cost since the different electrocatalytic mechanisms are not easily matchable for each other. Herein, a self-standing hybrid system Ni18Fe12Al70, consisting of Ni2Al3 and Ni3Fe phases, was constructed by laser-assisted aluminum (Al) incorporation towards full water splitting. It was found that the incorporation of Al could effectively tune the morphologies, compositions and phases. The results indicate that Ni18Fe12Al70 delivers an extremely low overpotential to trigger both HER (η100=188 mV) and OER (η100=345 mV) processes and maintains a stable overpotential for 100 h, comparable to state-of-the-art electrocatalysts. The synergistic effect of Ni2Al3 and Ni3Fe alloys on the HER process is confirmed based on theoretical calculation. 相似文献
69.
Yutong Pi Linxia Cui Prof. Wenhao Luo Dr. Haitao Li Dr. Yanfu Ma Dr. Na Ta Xinyao Wang Prof. Rui Gao Prof. Dan Wang Prof. Qihua Yang Prof. Jian Liu 《Angewandte Chemie (International ed. in English)》2023,62(43):e202307096
Mimicking the structures and functions of cells to create artificial organelles has spurred the development of efficient strategies for production of hollow nanoreactors with biomimetic catalytic functions. However, such structure are challenging to fabricate and are thus rarely reported. We report the design of hollow nanoreactors with hollow multishelled structure (HoMS) and spatially loaded metal nanoparticles. Starting from a molecular-level design strategy, well-defined hollow multishelled structure phenolic resins (HoMS-PR) and carbon (HoMS-C) submicron particles were accurately constructed. HoMS-C serves as an excellent, versatile platform, owing to its tunable properties with tailored functional sites for achieving precise spatial location of metal nanoparticles, internally encapsulated (Pd@HoMS-C) or externally supported (Pd/HoMS-C). Impressively, the combination of the delicate nanoarchitecture and spatially loaded metal nanoparticles endow the pair of nanoreactors with size–shape-selective molecular recognition properties in catalytic semihydrogenation, including high activity and selectivity of Pd@HoMS-C for small aliphatic substrates and Pd/HoMS-C for large aromatic substrates. Theoretical calculations provide insight into the pair of nanoreactors with distinct behaviors due to the differences in energy barrier of substrate adsorption. This work provides guidance on the rational design and accurate construction of hollow nanoreactors with precisely located active sites and a finely modulated microenvironment by mimicking the functions of cells. 相似文献
70.
Pengzhou Li Dr. Meng Liao Dr. Shuquan Cui Jiaxin Li Dr. Lei Ye Yibei Yang Chuang Wang Prof. Bingjie Wang Prof. Huisheng Peng 《Angewandte Chemie (International ed. in English)》2023,62(17):e202300705
Flexible batteries based on gel electrolytes with high safety are promising power solutions for wearable electronics but suffer from vulnerable electrode-electrolyte interfaces especially upon complex deformations, leading to irreversible capacity loss or even battery collapse. Here, a supramolecular sol-gel transition electrolyte (SGTE) that can dynamically accommodate deformations and repair electrode-electrolyte interfaces through its controllable rewetting at low temperatures is designed. Mediated by the micellization of polypropylene oxide blocks in Pluronic and host-guest interactions between α-cyclodextrin (α-CD) and polyethylene oxide blocks, the high ionic conductivity and compatibility with various salts of SGTE afford resettable electrode-electrolyte interfaces and thus constructions of a series of highly durable, flexible aqueous zinc batteries. The design of this novel gel electrolyte provides new insights for the development of flexible batteries. 相似文献