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101.
102.
We present a simple model to rationalize the effects of environment on the reaction barrier frequencies derived from free energy profiles. These frequencies are relevant in deviations of a rate constant from its transition state theory value and in determining which environmental dynamics participate in the reaction. In particular, this simple model can be used to understand the changes in the reaction barrier frequencies of an enzymatic catalyzed reaction and the corresponding uncatalyzed process in aqueous solution, a change which has implications for dynamical environmental effects on the enzymatic reaction. Two possible cases are analyzed, in which the polarity (charge separation/localization) of the reacting system increases or decreases as the reaction advances. A simple modeling of the environment′s effects allows the explanation of an unusual “inverse” effect on the reaction frequencies, that is, a free energy barrier lowering accompanied by an increase of the reaction frequency, a behavior observed in some enzymes. The model predictions are successfully compared with results from full simulations for four different enzyme reactions. 相似文献
103.
Dr. Weinan Xing Dr. Shengming Yin Dr. Wenguang Tu Dr. Guanyu Liu Dr. Shuyang Wu Dr. Haojing Wang Prof. Markus Kraft Dr. Guangyu Wu Prof. Rong Xu 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(3):1187-1191
A simple solvent ligation effect was successfully used to disrupt the growth of a model compound, Fe[(OH)(O3P(CH2)2CO2H)]⋅H2O (MIL-37), into an extended 2D structure by replacing water with dimethylformamide (DMF) as the solvent during the synthesis. Owing to the lack of −OH group, which provides the corner-sharing (binding) oxygen atoms for the octahedra, an amorphous and porous structure is formed. When Fe3+ is partially replaced by Ni2+, the amorphous structure remains and the resultant binary metal catalyst displays excellent photocatalytic oxygen evolution activity with almost 100 % yield achieved under visible light irradiation using [Ru(bpy)3]2+ as the photosensitizer. This study opens up new possibilities of using the simple solvent effect to synthesize high surface area metal phosphonates for catalytic and other applications. 相似文献
104.
This paper investigates mixed free and forced convection of non-Newtonian fluids from a vertical isothermal plate embedded
in a homogenous porous medium. A mathematical model is developed based on the modified Darcy's law and boundary-layer approximations,
and the exact similarity solution is obtained as well as an integral solution. These two solutions agree within 3% for aiding
flows and 10% for opposing flows. It is found that, non-Newtonian characteristics of fluids have appreciable influences on
velocity profiles, temperature distributions and flow regimes. 相似文献
105.
本文对钢丝帘线/橡胶复合材料中的钢丝帘线泊松比的定义提出了新的见解,建议用钢丝帘线横截面变化率代替其横向应变,并提出了利用扫描电子显微镜测定截面变化率的实验方法 相似文献
106.
研究了不同脉冲次数强流脉冲电子束表面改性对CuFe10合金组织及性能的影响。强流脉冲电子束处理CuFe10合金的重熔表面出现了火山坑和直径为100nm到1μm的富铁球,表明了强流脉冲电子束处理CuFe10合金表面发生了液相分离。强流脉冲电子束脉冲轰击30次后,CuFe10合金表面的显微硬度与耐蚀性能均得到显著改善,主要是由于强流脉冲电子束轰击处理CuFe10合金表层引发的快速熔凝过程中表面发生了液相分离及晶粒细化的缘故。 相似文献
107.
A simple, efficient, and general method has been developed for the synthesis of coumarin derivatives through a one‐pot reaction of aromatic aldehydes, 2,2‐dimethyl‐1,3‐dioxane‐4,6‐dione and 5,5‐dimethyl‐1,3‐cyclohexanedione, in the presence of TEBA under solvent‐free conditions using grinding methods. The mild reaction conditions, simple protocol, high yields, and cleaner reaction make this protocol practical and economically attractive. 相似文献
108.
An efficient and facile synthesis of 4,6-diarylpyrimidin-2(1H)-one via a Biginelli-like reaction of aromatic aldehydes, aromatic ketones, and urea in the presence of NaOH under solvent-free conditions using a heating method has been developed. Compared with the classical reaction conditions, this new synthetic method has the advantages of excellent yields, shorter reaction time, and mild reaction conditions. 相似文献
109.
A facile one-pot synthesis of 5-(trifluoromethyl)-4,7-dihydrotetrazolo[1,5-a]pyrimidine derivatives is described via a three-component reaction of aldehydes with 5-aminotetrazole and ethyl 4,4,4-trifluoro-3-oxobutanoate or 4,4,4-trifluoro-1-phenylbutane-1,3-dione in ionic liquid. This method has the advantages of short synthetic route, operational simplicities, good yields, ecofriendliness, and recyclability of the solvent. 相似文献
110.
Three kinds of novel aromatic diamine-based benzoxazines containing naphthalene, propane-2,2-diyldibenzene and neopentyl groups in the backbone, respectively (designated as BAPNCP, BAPBACP and BAPNPGCP, respectively), were synthesized and characterized. In addition, the effects of backbone structures on curing behaviors of the monomers and thermal and flammability properties of the resulting polymers were systematically studied. The results indicated that BAPNPGCP displayed the highest enthalpy of the curing reaction associated with the ring-opening of benzoxazine, which was due to the effect of benzoxazine ring content per unit mass. Interestingly, the 5 wt% weight loss temperature and char residue after thermogravimetric test for poly(BAPNPGCP) were 8 °C and 7% higher than those of poly(BAPBACP). Meanwhile, the total heat release of poly(BAPNPGCP) was less than half of that for poly(BAPBACP), indicating the substantial effect of benzoxazine ring content on flammability and char formation. Furthermore, it was found that poly(BAPNCP) gave the best thermal stability and flame retardancy, which was due to the synergistic effect between naphthalene group and benzoxazine ring content. This study provides new insight into the curing behavior of benzoxazine and further understanding on the high performance of polybenzoxazine. 相似文献