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981.
Yan‐mei Shi Lin Mei Jun‐xia Zhang Kai Hu Xi Zhang Zhu‐zhu Li Ming‐san Miao Xiu‐min Li 《Electroanalysis》2020,32(7):1507-1515
A new electrochemical sensor material has been fabricated via the non‐covalent functionalization of reduced graphene oxide (rGO) and soluble tetramino zincphthalocyanines (ZnPc‐NH2). Immobilization of uricase onto the synthesized nanohybrids can evidently improve the electrocatalytic activity and selectivity. The obtained composite membrane possesses a great enhancement of electron transfer rate and excellent synergistic electrocatalytic effect toward uric acid (UA) oxidation under the working potential at 0.620 V vs. Ag/AgCl with a scan rate of 0.125 V/s. The effects of the experimental parameters on the electrochemical oxidation responses of UA were investigated and optimized in detail. Under the optimized conditions, the peak currents were proportional to the UA concentration in a range from 0.5 to 100 μmol/L with detection limit of 0.15 μmol/L. Moreover, the developed sensor was applied for UA determination in human urine samples with high accuracy and satisfactory recovery, which is envisioned to have promising applications in monitoring UA in clinical research. 相似文献
982.
Wenchao Zhang Chuangang Hu Zaiping Guo Liming Dai 《Angewandte Chemie (International ed. in English)》2020,59(9):3470-3474
Metal–CO2 batteries have attracted much attention owing to their high energy density and use of greenhouse CO2 waste as the energy source. However, the increasing cost of lithium and the low discharge potential of Na–CO2 batteries create obstacles for practical applications of Li/Na–CO2 batteries. Recently, earth‐abundant potassium ions have attracted considerable interest as fast ionic charge carriers for electrochemical energy storage. Herein, we report the first K–CO2 battery with a carbon‐based metal‐free electrocatalyst. The battery shows a higher theoretical discharge potential (E?=2.48 V) than that of Na–CO2 batteries (E?=2.35 V) and can operate for more than 250 cycles (1500 h) with a cutoff capacity of 300 mA h g?1. Combined DFT calculations and experimental observations revealed a reaction mechanism involving the reversible formation and decomposition of P121/c1‐type K2CO3 at the efficient carbon‐based catalyst. 相似文献
983.
Chao Liu Jing Wang Jingjing Wan Yan Cheng Rong Huang Chaoqi Zhang Wenli Hu Guangfeng Wei Chengzhong Yu 《Angewandte Chemie (International ed. in English)》2020,59(9):3630-3637
Amorphous metal–organic frameworks (aMOFs) are an emerging family of attractive materials with great application potential, however aMOFs are usually prepared under harsh conditions and aMOFs with complex compositions and structures are rarely reported. In this work, an aMOF‐dominated nanocomposite (aMOF‐NC) with both structural and compositional complexity has been synthesized using a facile approach. A ligand‐competition amorphization mechanism is proposed based on experimental and density functional theory calculation results. The aMOF‐NC possesses a core–shell nanorod@nanosheet architecture, including a Fe‐rich Fe‐Co‐aMOF core and a Co‐rich Fe‐Co‐aMOF shell in the core–shell structured nanorod, and amorphous Co(OH)2 nanosheets as the outer layer. Benefiting from the structural and compositional heterogeneity, the aMOF‐NC demonstrates an excellent oxygen evolution reaction activity with a low overpotential of 249 mV at 10.0 mA cm?2 and Tafel slope of 39.5 mV dec?1. 相似文献
984.
Nan Wu Po‐Hsiu Chien Yumin Qian Yutao Li Henghui Xu Nicholas S. Grundish Biyi Xu Haibo Jin Yan‐Yan Hu Guihua Yu John B. Goodenough 《Angewandte Chemie (International ed. in English)》2020,59(10):4131-4137
Li+‐conducting oxides are considered better ceramic fillers than Li+‐insulating oxides for improving Li+ conductivity in composite polymer electrolytes owing to their ability to conduct Li+ through the ceramic oxide as well as across the oxide/polymer interface. Here we use two Li+‐insulating oxides (fluorite Gd0.1Ce0.9O1.95 and perovskite La0.8Sr0.2Ga0.8Mg0.2O2.55) with a high concentration of oxygen vacancies to demonstrate two oxide/poly(ethylene oxide) (PEO)‐based polymer composite electrolytes, each with a Li+ conductivity above 10?4 S cm?1 at 30 °C. Li solid‐state NMR results show an increase in Li+ ions (>10 %) occupying the more mobile A2 environment in the composite electrolytes. This increase in A2‐site occupancy originates from the strong interaction between the O2? of Li‐salt anion and the surface oxygen vacancies of each oxide and contributes to the more facile Li+ transport. All‐solid‐state Li‐metal cells with these composite electrolytes demonstrate a small interfacial resistance with good cycling performance at 35 °C. 相似文献
985.
Chao Hu Tao Wang Matthias Rudolph Thomas Oeser Abdullah M. Asiri A. Stephen K. Hashmi 《Angewandte Chemie (International ed. in English)》2020,59(22):8522-8526
A novel gold‐catalyzed cycloisomerization of 1,6‐diynes was achieved, providing an atom‐economic approach to a diverse set of bicyclo[2.2.1]hept‐5‐en‐2‐ones in moderate to good yields. With unsymmetrical starting materials with two different internal alkynyl substituents, to some extent, the regioselectivity could be controlled by both electronic and steric factors. This unprecedented reactivity pattern may inspire new and unconventional strategies for the preparation of bridged ring systems. 相似文献
986.
[Fe]‐hydrogenase is an efficient biological hydrogenation catalyst. Despite intense research, Fe complexes mimicking the active site of [Fe]‐hydrogenase have not achieved turnovers in hydrogenation reactions. Herein, we describe the design and development of a manganese(I) mimic of [Fe]‐hydrogenase. This complex exhibits the highest activity and broadest scope in catalytic hydrogenation among known mimics. Thanks to its biomimetic nature, the complex exhibits unique activity in the hydrogenation of compounds analogous to methenyl‐H4MPT+, the natural substrate of [Fe]‐hydrogenase. This activity enables asymmetric relay hydrogenation of benzoxazinones and benzoxazines, involving the hydrogenation of a chiral hydride transfer agent using our catalyst coupled to Lewis acid‐catalyzed hydride transfer from this agent to the substrates. 相似文献
987.
Rui‐Ting Gao Dan He Lijun Wu Kan Hu Xianhu Liu Yiguo Su Lei Wang 《Angewandte Chemie (International ed. in English)》2020,59(15):6213-6218
Increasing long‐term photostability of BiVO4 photoelectrode is an important issue for solar water splitting. The NiOOH oxygen evolution catalyst (OEC) has fast water oxidation kinetics compared to the FeOOH OEC. However, it generally shows a lower photoresponse and poor stability because of the more substantial interface recombination at the NiOOH/BiVO4 junction. Herein, we utilize a plasma etching approach to reduce both interface/surface recombination at NiOOH/BiVO4 and NiOOH/electrolyte junctions. Further, adding Fe2+ into the borate buffer electrolyte alleviates the active but unstable character of etched‐NiOOH/BiVO4, leading to an outstanding oxygen evolution over 200 h. The improved charge transfer and photostability can be attributed to the active defects and a mixture of NiOOH/NiO/Ni in OEC induced by plasma etching. Metallic Ni acts as the ion source for the in situ generation of the NiFe OEC over long‐term durability. 相似文献
988.
Fast, mass, and low‐cost production of high‐quality graphene, which is alluring, remains a great challenge, even though some approaches have shown potential for mass synthesis of graphene. Very recently a great breakthrough was made by Tour and co‐workers (Nature 2020, 577, 647–651): in just a second, easily exfoliated and highly crystalline graphene was produced from abundant carbon‐containing species by cost‐effective flash Joule heating with a low energy input of 7.2 kJ per gram graphene. Such an ultrafast, economic, and scalable process for high‐quality graphene production can be considered as a milestone in the graphene field and is highlighted in this article. 相似文献
989.
Xiangchuan Meng Zhi Xing Xiaotian Hu Zengqi Huang Ting Hu Licheng Tan Fengyu Li Yiwang Chen 《Angewandte Chemie (International ed. in English)》2020,59(38):16602-16608
Perovskite solar cells (PSCs) are a promising photovoltaic technology for stretchable applications because of their flexible, light‐weight, and low‐cost characteristics. However, the fragility of crystals and poor crystallinity of perovskite on stretchable substrates results in performance loss. In fact, grain boundary defects are the “Achilles’ heel” of optoelectronic and mechanical stability. We incorporate a self‐healing polyurethane (s‐PU) with dynamic oxime–carbamate bonds as a scaffold into the perovskite films, which simultaneously enhances crystallinity and passivates the grain boundary of the perovskite films. The stretchable PSCs with s‐PU deliver a stabilized efficiency of 19.15 % with negligible hysteresis, which is comparable to the performance on rigid substrates. The PSCs can maintain over 90 % of their initial efficiency after 3000 hours in air because of their self‐encapsulating structure. Importantly, the self‐healing function of the s‐PU scaffold was verified in situ. The s‐PU can release mechanical stress and repair cracks at the grain boundary on multiple levels. The devices recover 88 % of their original efficiency after 1000 cycles at 20 % stretch. We believe that this ingenious growth strategy for crystalline semiconductors will facilitate development of flexible and stretchable electronics. 相似文献
990.
Xuemin Ye Beibei Ye Jiahui Xu Mei Fang Danqi Dong Congcong Wu Xupin Lin Yehui Hu Xiaoji Cao Weimin Mo 《Journal of separation science》2020,43(17):3546-3554
In this work, a novel quick, easy, cheap, effective, rugged, and safe technique with hydrophobic natural deep eutectic solvent as both extractant and analyte protectant was developed and combined with gas chromatography–tandem mass spectrometry to analyze pyrethroid residues in tomatoes. Eight hydrophobic natural deep eutectic solvents were first evaluated as analyte protectants and those with decanoic acid or lactic acid as hydrogen bond donor were demonstrated to be effective in compensating for the matrix effects of pyrethroids in the gas chromatography system. Hence, they were added to solvent standards for correcting the quantitation errors instead of matrix‐matched calibration standards. Then the abilities of these acid‐based deep eutectic solvents to extract pyrethriods from tomatoes were evaluated. Results showed the recoveries of all pyrethroids reached to over 80% with only 5 mL menthol:decanoic acid (1:1) used, and good phase separation was easily achieved without the addition of inorganic salt in the extraction step, indicating hydrophobic natural deep eutectic solvent could be a green substitute for acetonitrile in the quick, easy, cheap, effective, rugged, and safe extraction. Compared with the conventional method, the proposed protocol improved the recoveries, reduced the matrix effects, and simplified the extraction step, demonstrating to be an effective, fast, and green method. 相似文献