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61.
Previously, master equation (ME) simulations using semiclassical transition state theory (SCTST) and high-accuracy extrapolated ab initio thermochemistry (HEAT) predicted rate constants in excellent agreement with published experimental data over a wide range of pressure and temperatures ≳250 K, but the agreement was not as good at lower temperatures. Possible reasons for this reduced performance are investigated by (a) critically evaluating the published experimental data and by investigating; (b) three distinct ME treatments of angular momentum, including one that is exact at the zero- and infinite-pressure limits; (c) a hindered-rotor model for HOCO that implicitly includes the cis- and trans-conformers; (d) possible empirical adjustments of the thermochemistry; (e) possible empirical adjustments to an imaginary frequency controlling tunneling; (f) including or neglecting the prereaction complex PRC1; and (g) its possible bimolecular reactions. Improvements include better approximations to factors in SCTST and using the Hill and van Vleck treatment of angular momentum coupling. Evaluation of literature data does not reveal any specific shortcomings, but the stated uncertainties may be underestimated. All ME treatments give excellent fits to experimental data at T ≥ 250 K, but the discrepancy at T < 250 K persists. Note that each ME model requires individual empirical energy transfer parameters. Thermochemical adjustments were unable to match the experimental H/D kinetic isotope effects. Adjusting an imaginary frequency can achieve good fits, but the adjustments are unacceptably large. Whether PRC1 and its possible bimolecular reactions are included had little effect. We conclude that none of the adjustments is an improvement over the unadjusted theory. Note that only one set of experimental data exists in the regime of the discrepancy with theory, and data for DO + CO are scanty. 相似文献
62.
Yingying Zhang Jiarui Wu Siwen Cui Wutao Wei Weihua Chen Rui Pang Zijie Wu Liwei Mi 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(3):584-591
Selection of the friction electrode materials is crucial to the performance of a triboelectric nanogenerator (TENG). In the present study, a metal–organic coordination complex containing organosulfonate counteranions with electron-donating ability was synthesized through the coordination-driven self-assembly approach under mild reaction conditions and was chosen as a positive electrode material to construct a triboelectric nanogenerator, exhibiting high-output performance with a peak value of short circuit current density of 98.6 μA and an output voltage of 1180 V. As a practical application, it was shown to light up 1488 commercial green LEDs and power an anticorrosion system device to protect metals from corrosion. 相似文献
63.
Roger M. Bialy Dr. Monsur M. Ali Prof. Dr. Yingfu Li Prof. Dr. John D. Brennan 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(22):5085-5092
We report a method to detect proteins via suppression of rolling circle amplification (RCA) by using an appropriate aptamer as the linear primer (denoted as an aptaprimer) to initiate RCA. In the absence of a protein target, the aptaprimer is free to initiate RCA, which can produce long DNA products that are detected via binding of a fluorescent intercalating dye. Introduction of a target causes the primer region within the aptamer to become unavailable for binding to the circular template, inhibiting RCA. Using SYBR Gold or QuantiFluor dyes as fluorescent probes to bind to the RCA reaction product, it is possible to produce a generic protein-modulated RCA assay system that does not require fluorophore- or biotin-modified DNA species, substantially reducing complexity and cost of reagents. Based on this modulation of RCA, we demonstrate the ability to produce both solution and paper-based assays for rapid and quantitative detection of proteins including platelet derived growth factor and thrombin. 相似文献
64.
Ji Wang Nan Li Yuxia Xu Prof. Dr. Huan Pang 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(29):6402-6422
Metal–organic framework (MOF) and covalent organic framework (COF) nanosheets are a new type of two-dimensional (2D) materials with unique design principles and various synthesis methods. They are considered ideal electrochemical devices due to the ultrathin thickness, easily tunable molecular structure, large porosity and other unique properties. There are two common methods to synthesize 2D MOF/COF nanosheets: bottom-up and top-down. The top-down strategy mainly includes ultrasonic assisted exfoliation, electrochemical exfoliation and mechanical exfoliation. Another strategy mainly includes interface synthesis, modulation synthesis, surfactant-assisted synthesis. In this Review, the development of ultrathin 2D nanosheets in the field of electrochemistry (supercapacitors, batteries, oxygen reduction, and hydrogen evolution) is introduced, and their unique dimensional advantages are highlighted. 相似文献
65.
Xinxin Lin Prof. Zheng Fang Cuilian Zeng Chenlong Zhu Xinyan Pang Chengkou Liu Wei He Jindian Duan Ning Qin Prof. Kai Guo 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(60):13738-13742
A non-oxidant and metal-free strategy for synthesizing iso-coumarin by using a continuous electrochemical microreactor to initiate an oxidative cyclization reaction of o-(1-alkynyl) benzoate and radicals. This efficient and clean continuous electrosynthesis method not only avoids the complicated gas protection operation and production of by-products in the batch processes, but also help to overcome the difficulty that batch metal catalysis and electrocatalysis are difficult to scale up, and has the potential for pilot-scale experiment. 相似文献
66.
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68.
Chong Saehwa Riley Brian J. Nienhuis Emily T. Lee Dongjin McCloy John S. 《Journal of chemical crystallography》2021,51(3):293-300
Journal of Chemical Crystallography - Four different rare-earth oxyapatites of Ca2RE8(SiO4)6O2 (RE?=?Pr, Tb, Ho, Tm) were synthesized using a solution-based method followed by drying,... 相似文献
69.
Nonlinear Dynamics - This paper focuses on the problem of nonlinear system identification by proposing an improved approach for existing frequency-domain nonlinear identification through feedback... 相似文献
70.