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91.
Caleb J. Hiller Dr. Chi Chung Lee Dr. Martin T. Stiebritz Lee A. Rettberg Prof. Dr. Yilin Hu 《Chemistry (Weinheim an der Bergstrasse, Germany)》2019,25(10):2389-2395
Nitrogenase utilizes an ATP-dependent reductase to deliver electrons to its catalytic component to enable two important reactions: the reduction of N2 to NH4+, and the reduction of CO to hydrocarbons. The two nitrogenase-based reactions parallel the industrial Haber–Bosch and Fischer–Tropsch processes, yet they occur under ambient conditions. As such, understanding the enzymatic mechanism of nitrogenase is crucial for the future development of biomimetic strategies for energy-efficient production of valuable chemical commodities. Mechanistic investigations of nitrogenase has long been hampered by the difficulty to trap substrates and intermediates relevant to the nitrogenase reactions. Recently, we have successfully captured CO on the Azotobacter vinelandii V-nitrogenase via two approaches that alter the electron fluxes in a controlled manner: one approach utilizes an artificial electron donor to trap CO on the catalytic component of V-nitrogenase in the resting state; whereas the other employs a mismatched reductase component to reduce the electron flux through the system and consequently accumulate CO on the catalytic component of V-nitrogenase. Here we summarize the major outcome of these recent studies, which not only clarified the catalytic relevance of the one-CO (lo-CO) and multi-CO (hi-CO) bound states of nitrogenase, but also pointed to a potential competition between N2 and CO for binding to the same pair of reactive Fe sites across the sulfur belt of the cofactor. Together, these results highlight the utility of these strategies in poising the cofactor at a well-defined state for substrate- or intermediate-trapping via controlled alteration of electron fluxes, which could prove beneficial for further elucidation of the mechanistic details of nitrogenase-catalyzed reactions. 相似文献
92.
Dr. Longhai Zhang Prof. Tong Wei Dr. Zimu Jiang Prof. Zhuangjun Fan 《Chemistry (Weinheim an der Bergstrasse, Germany)》2019,25(19):5022-5027
To optimize the cycle life and rate performance of lithium-ion batteries (LIBs), ultra-fine Fe2O3 nanowires with a diameter of approximately 2 nm uniformly anchored on a cross-linked graphene ribbon network are fabricated. The unique three-dimensional structure can effectively improve the electrical conductivity and facilitate ion diffusion, especially cross-plane diffusion. Moreover, Fe2O3 nanowires on graphene ribbons (Fe2O3/GR) are easily accessible for lithium ions compared with the traditional graphene sheets (Fe2O3/GS). In addition, the well-developed elastic network can not only undergo the drastic volume expansion during repetitive cycling, but also protect the bulk electrode from further pulverization. As a result, the Fe2O3/GR hybrid exhibits high rate and long cycle life Li storage performance (632 mAh g−1 at 5 A g−1, and 471 mAh g−1 capacity maintained even after 3000 cycles). Especially at high mass loading (≈4 mg cm−2), the Fe2O3/GR can still deliver higher reversible capacity (223 mAh g−1 even at 2 A g−1) compared with the Fe2O3/GS (37 mAh g−1) for LIBs. 相似文献
93.
Ya-Xin Li Fang-Fang Fan Jie Wang Dr. Liliana Cseh Dr. Min Xue Dr. Xiang-Bing Zeng Prof. Goran Ungar 《Chemistry (Weinheim an der Bergstrasse, Germany)》2019,25(60):13739-13747
Wedge-shaped molecules, such as dendrons, are among the most important building blocks for directed supramolecular self-assembly. Here we present a new approach aimed at widening the range and complexity of potential mesophases by introducing double-tapered mesogens. Two series of compounds are presented, both alkali metal salts (Li, Na, Cs) of 3,4,5-tris-alkoxybenzoic acid with a second tapered tris-alkoxyaryl group attached at the end of an alkoxy chain. The double-tapered compounds all display an unusual hexagonal columnar phase consisting of one ionic and three non-ionic columns per unit cell. The cation size has an unexpectedly drastic effect on unit cell size. Unlike most columnar phases, the current phases show unusually high dimensional stability on heating, and high stiffness in spite of being 80–85 % aliphatic, attributed to their molecular topology. The described approach may lead to co-assemblies of multifunctional materials, for example, parallel p- and n-semiconducting nanowires or parallel ionic and electronic conductors. 相似文献
94.
Chenyang Fan Chonglin Song Gang Lv Jiangjun Wei Xuyang Zhang Yuehan Qiao Ye Liu 《Proceedings of the Combustion Institute》2019,37(4):4821-4829
Post injection has significant benefit in the reduction of diesel soot emissions. Therefore, there is a need to understand the effect of post-injection strategy on soot physicochemical properties and reactivity because they play an important role in soot oxidation process that governs the final soot emissions. This work focuses on the impact of post injection on the physicochemical properties and reactivity of diesel in-cylinder soot using a main plus post injection (M*P) and a single injection (M) strategy. The soot was sampled by a developed total cylinder sampling system, and the dividing points of soot formation-dominant and oxidation-dominant phases were used for studying the impacts of post injection on the characteristics of in-cylinder soot. The physicochemical properties of the soot samples, including primary particle size, nanostructure, carbon chemical state and surface functional groups, were characterized. The soot reactivity was evaluated in terms of peak temperature, burnout temperature and apparent activation energy. In the oxidation-dominant phase, the M*P soot initially possesses smaller primary particle size, shorter fringe length, larger tortuosity, lower sp2/sp3 hybridization ratio of carbon atoms and higher content of aliphatic CH groups than the M soot. The beneficial influence of physicochemical properties on soot reactivity when using post injection is validated by the thermogravimetric data, which shows that the M*P soot is more reactive than the M soot at the onset of the oxidation-dominant phase. In the M*P case, the soot generated from the main-injection combustion has lower reactivity than the soot from the post-injection combustion after they experience the soot formation-dominant phase. The results indicate that the use of post injection leads to in-cylinder soot with physicochemical properties that favor reactivity. The enhancement of reactivity means that the soot will be more readily oxidized in the subsequent combustion process, and consequently contributes to a reduction in final soot emissions. 相似文献
95.
96.
Acta Mathematicae Applicatae Sinica, English Series - This paper considers a competing risks model for right-censored and length-biased survival data from prevalent sampling. We propose a... 相似文献
97.
In the present work, a visible-light-driven Ag/AgBr/ZnFe2O4 photocatalyst has been successfully synthesized via a deposition–precipitation and photoreduction method. The crystal structure, chemical composition, morphology and optical properties of the as-prepared nanocomposites were characterized by X-ray diffraction spectroscopy, X-ray photoelectron spectroscopy, scanning electron microscopy, high-resolution transmission electron microscopy, energy-dispersive X-ray spectroscope, UV–vis diffuse reflectance spectroscopy and photoluminescence. The photocatalytic activities of the Ag/AgBr/ZnFe2O4 nanocomposites were evaluated through the photodegradation of gaseous toluene and methyl orange (MO) under visible light. The results revealed that the as-prepared Ag/AgBr/ZnFe2O4 nanocomposite exhibited excellent photocatalytic activity. The degrading efficiency of MO could still reach 90% after four cycles, and the Ag/AgBr/ZnFe2O4 nanocomposite could be recycled easily by a magnet. Additionally, the enhanced photocatalytic mechanism was discussed according to the trapping experiments, which indicated that the photo-generated holes (h+) and •O2− played important roles in photodegradation process. At last, a possible photocatalytic oxidation pathways of toluene was proposed based on the results of GC–MS. The Ag/AgBr/ZnFe2O4 composites showed potential application for efficient removal of organic pollutant. 相似文献
98.
Zhi Sun Mengfan Zhao Lihua Zuo Shengnan Zhou Feng Fan Qingquan Jia Lianping Xue Hanbing Li Jian Kang Xiaojian Zhang 《Journal of separation science》2022,45(2):518-528
Juglandis Mandshuricae Cortex is the bark of Juglans mandshurica Maxim., which has been used as a folk medicine plant in China and India. In this study, an ultra-high performance liquid chromatography–quadrupole/orbitrap high-resolution mass spectrometry method was developed to clarify and quantify the chemical profiling of Juglandis Mandshuricae Cortex rapidly. A total of 113 compounds were characterized. Among them, seven flavonoids were simultaneously quantified in 15 min, including myricetin, myricetrin, taxifolin, kaempferol, quercetin, quercitrin, and naringenin. The method was validated for accuracy, precision, and the limits of detection and quantification. All calibration curves showed a good linear relationship (r > 0.9990) within test ranges. The intra- and inter-day relative standard deviations were less than 2.16%. Accuracy validation showed that the recovery was between 95.6 and 101.3% with relative standard deviation values below 2.85%. The validated method was successfully applied to determine the contents of seven flavones in Juglandis Mandshuricae Cortex from seven sources and the contents of these places were calculated respectively. This method provides a theoretical basis for further developing the medicinal value of Juglandis Mandshuricae Cortex. 相似文献
99.
Mingshuai He Heshui Yu Peng Lei Shengjie Huang Juanning Ren Wenjing Fan Lifeng Han Haiyang Yu Yuefei Wang Ming Ren Miaomiao Jiang 《Molecules (Basel, Switzerland)》2021,26(5)
Trimethylamine N-oxide (TMAO), as a gut-derived metabolite, has been found to be associated with enhanced risk for atherosclerosis and cardiovascular disease. We presented a method for targeted profiling of TMAO and betaine in serum and food samples based on a combination of one-step sample pretreatment and proton nuclear magnetic resonance spectroscopy. The key step included a processing of sample preparation using a selective solid-phase extraction column for retention of basic metabolites. Proton signals at δ 3.29 and δ 3.28 were employed to quantify TMAO and betaine, respectively. The developed method was examined with acceptable linear relationship, precision, stability, repeatability, and accuracy. It was successfully applied to detect serum levels of TMAO and betaine in TMAO-fed mice and high-fructose-fed rats and also used to determine the contents of TMAO and betaine in several kinds of food, such as fish, pork, milk, and egg yolk. 相似文献
100.
Wang Dongliang Su Xin Fan Zongliang Wen Zhuoyu Li Ning Yang Yong 《Catalysis Surveys from Asia》2021,25(4):347-361
Catalysis Surveys from Asia - Benzene methylation over zeolite offers an alternative route to produce high-value toluene or para-xylene directly from benzene and C1 chemical sources, especially for... 相似文献