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41.
QI Yuxue LI Tingting HU Yajie XIANG Jiahong SHAO Wenqian CHEN Wenhua MU Xueqin LIU Suli CHEN Changyun YU Min MU Shichun 《高等学校化学研究》2022,38(5):1282-1286
Constructing atomically dispersed active sites with densely exposed and dispersed double metal-Sx catalytic sites for favorable OER catalytic activity remains rare and challenging. Herein, we design and construct a Fe1Sx@Co3S4 electrocatalyst with Fe single atoms epitaxially confined in Co3S4 nanosheets for catalyzing the sluggish alkaline oxygen evolution reaction(OER). Consequently, in ultralow concentration alkaline solutions(0.1 mol/L KOH), such a catalyst is highly active and robust for OER with low overpotentials of 300 and 333 mV at current densities of 10 and 30 mA/cm2, respectively, accompanying long-term stability without significant degradation even for 350 h. In addition, Fe1Sx@Co3S4 shows a turnover frequency(TOF) value of 0.18 s−1, nearly three times that of Co3S4(0.07 s−1), suggesting the higher atomic utilization of Fe single atoms. Mössbauer and in-situ Raman spectra confirm that the OER activity of Fe1Sx@Co3S4 origins from a thin catalytic layer of Co(Fe)OOH that interacts with trace-level Fe species in the electrolyte, creating dynamically stable active sites. Combined with experimental characterizations, it suggests that the most active S-coordinated dual-metal site configurations are 2S-bridged (Fe-Co)S4, in which Co-S and Fe-S moieties are shared with two S atoms, which can strongly regulate the adsorption energy of reaction intermediates, accelerating the OER reaction kinetics. 相似文献
42.
Density Functional Theory Mechanistic Study of Boron‐Catalyzed N‐Alkylation of Amines with Formic Acid: Formic Acid Activation by Silylation Reaction 下载免费PDF全文
New methodology for the alkylation of amines is an intriguing issue in both academia and industry. Recently, several groups reported the metal‐free B(C6F5)3‐catalyzed N‐alkylation of amines, but the mechanistic details of these important reactions are unclear. Herein, a computational study was performed to elucidate the mechanism of the N‐alkylation of amines with formic acid catalyzed by the Lewis acid B(C6F5)3 in the presence of hydrosilane. We found that the reaction started with the activation of formic acid through a novel model. Then, the high electrophilicity of the C center of the formic acid unit and the nucleophilic character of the amine resulted in a C?N coupling reaction. Finally, two sequential silyl‐group and H? transfer steps occurred to generate the final product. Upon comparing the reaction barrier and the hydrogenation of indole, our mechanism is more favorable than that proposed by the group of Yu and Fu. 相似文献
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In this paper, firstly, we characterize some rings by strict Mittag-Leffler conditions. Then, we investigate when Gorenstein projective modules are Gorenstein flat by employing tilting modules and cotorsion pairs. Finally, we study the direct limits of Gorenstein projective modules. 相似文献
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Allyloxy polyethoxy ether (APEG) and succinic anhydride were used to prepare allyloxy polyethoxy carboxylate (APEL). 8-Hydroxy-1,3,6-pyrene trisulfonic acid trisodium salt (PY) was reacted with allyl chloride to produce fluorescent monomer 8-allyloxy-1,3,6-pyrene trisulfonic acid trisodium salt (PA). APEL and PA were copolymerized with maleic anhydride (MA) to synthesize PA tagged no phosphate and nitrogen free CaSO4 inhibitor MA–APEL–PA. Structures of PA, APEG, APEL, and MA–APEL–PA were identified by 1H NMR. The observation shows that the dosage of MA–APEL–PA plays an important role on CaSO4 inhibition. The effect on formation of CaSO4 was investigated with scanning electron microscope (SEM) analysis. Relationship between MA–APEL–PA’s fluorescent intensity and its dosage was studied. Correlation coefficient R 2 of MA–APEL–PA fluorescent intensity and MA–APEL–PA dosage is 0.9991. 相似文献
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The present paper is concerned with the convergence problem of the variants of the Chebyshev–Halley iteration family with parameters for solving nonlinear operator equations in Banach spaces. Under the assumption that the first derivative of the operator satisfies the Hölder condition of order p, a convergence criterion of order 1+p for the iteration family is established. An application to a nonlinear Hammerstein integral equation of the second kind is provided. 相似文献
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根据强非局域介质构成的平面介质波导中同频率和同极化的多光束共同传输模型方程,求得了任意斜入射多光束相互作用的精确解析解。基于强非局域介质空间双光孤子的相互作用原理,提出了利用全同孤子作为信号光来实现全光互联,但实现的逻辑也仅仅局限于短距离作用,还对全光开关抑或反相器作了详细叙述,通过实例给出了这类设计的优化方案。 相似文献
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We study the quark loop effects on the dressed gluon propagator and also on the quark propagator itself. We find that the gluon propagators are different in two phases. The quark mass effects on the gluon propagator are small but not negligible. We also study the current quark mass dependence on the bag constant. 相似文献