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81.
Lulu Wang Jinmiao Wang Chuanbin Fan Caifeng Bi Xia Zhang Dongmei Zhang Mei Wang Yuhua Fan 《应用有机金属化学》2020,34(9):e5767
Two novel Co (II)- coordination polymers (CPs) based on 2,5-bis(4-carboxylpheny)-1,3,4-oxadiazole (bcpo), namely [Co/(bcpo)0.5(tib)(H2O)2]n (1) and [Co (bcpo)0.5(bidpe)(H2O)2]n (2) (tib = 1,3,5-tirs(1-imidazolyl)benzene, bidpe = 4,4′-bis (imidazolyl)diphenyl ether) have been synthesized under solvothermal conditions and characterized by powder X-ray diffraction (PXRD), single crystal X-ray diffraction, photochemistry as well as electrochemistry. The investigation of the photo-degradation methyl blue and methyl violet (MB, MV) properties of CPs 1–2 demonstrates that CP 1 shows great performance for the degradation of MB, and CP 2 could efficiently degrade MB/MV. Meanwhile, the possible photo-degradation mechanism has been proposed and explored. Simultaneously, electrochemistry studies show that both CPs 1 and 2 can catalyze water oxidation under an alkaline condition at the potential around 1.20 V vs. NHE with relatively low overpotential of 330–510 mV vs. NHE. 相似文献
82.
In this work, kinetic of H2S conversion to H2 molecule on the surface of Pt(111) is studied using kinetic Monte Carlo simulation. The results of simulation were fitted to the experimental temperature-programed desorption spectra. The good agreement between the empirical and the simulated data confirms the proposed mechanism and kinetic data (activated energies and pre-exponential factors). The influence of variables such as temperature and concentrations of H2S and H2 on the overall results of hydrogen production is studied. The condition is proposed in which the best yield of reaction at minimum temperature is obtained. Results show that platinum is a perfect catalyst for converting H2S to H2 and it has a perfect performance (98%) after 5 μs at low temperature of 227°C. 相似文献
83.
A detailed chemical kinetic model has been developed for supercritical water oxidation (SCWO) of methylamine, CH3NH2, providing insight into the intermediates and final products formed in this process as well as the dominant reaction pathways. The model was adapted from previous mechanisms, with a revision of the peroxyl radical chemistry to include imine formation, which has recently been identified as the dominant gas-phase pathway in amine oxidation. The developed model can reproduce previous experimental data on methylamine consumption and major product formation to reasonable accuracy, although with deficiencies in describing the induction time. Our simulations indicate that oxidation of the •CH2NH2 radical to methanimine, CH2NH, is the major channel in methylamine SCWO, with subsequent hydrolysis of CH2NH providing the experimentally observed reaction products ammonia and formaldehyde. Integral-averaged reaction rates were used to identify major reaction pathways, and a first-order sensitivity analysis indicated that the concentration of CH3NH2 is most sensitive to OH radical kinetics. Overall, this work clarifies the importance of imine chemistry in the oxidation of nitrogen-containing compounds and indicates that they are necessary to model these compounds in SCWO processes. 相似文献
84.
Herein a well-sealed and thermostated kinetics assembly is designed and built, which can run stirred at different reaction temperatures. With the reaction assembly above and the volumetric method together, the hydrogen peroxide (H2O2) decomposition reaction kinetics is systematically investigated under a variety of reaction conditions over a copper-doped buserite-type layer manganese oxide (referred to as Cu-buserite) as a heterogeneous catalyst. The overall second-order rate law is fitted out by the linear regression analysis, with the reaction orders with respect to both H2O2 and Cu-buserite determined to each be equal to 1, and then explicitly explained by the proposed Michaelis-Menten like mechanism. The apparent activation energy Ea is estimated as 33.5 ± 2.5 kJ mol−1. 相似文献
85.
Hidehisa Kawashima Itsuki Ozawa Masashi Kijima 《Journal of polymer science. Part A, Polymer chemistry》2020,58(13):1747-1756
Rigid and little moldable curdlan, a linear β-1,3-glucan having intra- and interchain hydrogen bonds, was reacted with several alkyl isocyanates, which gave thermoplastic curdlan alkyl carbamates (CrdC) with degree of substitution about 2. The alkyl carbamation at hydroxy groups in the glucan skeleton effectively broke the interchain hydrogen bonds of curdlan and increased flexibility of CrdC, while the newly formed carbamate moieties could moderately keep the hydrogen bonding ability in CrdC. Elongating the alkyl groups in the carbamate side chains increased solubility in organic solvents and thermoplasticity of CrdC, which enabled to make homogeneous and free-standing films by both methods of solution-casting and hot-pressing. 相似文献
86.
Dr. Ying Wang Dr. Wenming Sun Xiaofei Ling Xiangkai Shi Dr. Lanlan Li Prof. Yida Deng Dr. Cuihua An Dr. Xiaopeng Han 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(18):4097-4103
The development of high-efficiency, low-cost, and earth-abundant electrocatalysts for overall water splitting remains a challenge. In this work, Ni-modified MoS2 hybrid catalysts are grown on carbon cloth (Ni-Mo-S@CC) through a one-step hydrothermal treatment. The optimized Ni-Mo-S@CC catalyst shows excellent hydrogen evolution reaction (HER) activity with a low overpotential of 168 mV at a current density of 10 mA cm−2 in 1.0 m KOH, which is lower than those of Ni-Mo-S@CC (1:1), Ni-Mo-S@CC (3:1), and pure MoS2. Significantly, the Ni-Mo-S@CC hybrid catalyst also displays outstanding oxygen evolution reaction (OER) activity with a low overpotential of 320 mV at a current density of 10 mA cm−2, and remarkable long-term stability for 30 h at a constant current density of 10 mA cm−2. Experimental results and theoretical analysis based on density functional theory demonstrate that the excellent electrocatalytic performance can be attributed mainly to the remarkable conductivity, abundant active sites, and synergistic effect of the Ni-doped MoS2. This work sheds light on a unique strategy for the design of high-performance and stable electrocatalysts for water-splitting electrolyzers. 相似文献
87.
Chunyu Qiu Suqi He Dr. Yuan Wang Prof. Qingxiang Wang Prof. Chuan Zhao 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(18):4120-4127
Interface engineering has been applied as an effective strategy to boost the electrocatalytic performance because of the strong coupling and synergistic effects between individual components. Here, we engineered vertically aligned FeOOH/CoO nanoneedle array with a synergistic interface between FeOOH and CoO on Ni foam (NF) by a simple impregnation method. The synthesized FeOOH/CoO exhibits outstanding electrocatalytic activity and stability for both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) in an alkaline medium. For the overall water splitting, the bifunctional FeOOH/CoO nanoneedle catalyst requires only a cell voltage of 1.58 V to achieve a current density of 10 mA cm−2, which is much lower than that required for IrO2//Pt/C (1.68 V). The FeOOH/CoO catalyst has been successfully applied for solar cell-driven water electrolysis, revealing its great potential for commercial hydrogen production and solar energy storage. 相似文献
88.
Yoichi Makimizu Nhat Truong Nguyen Jiri Tucek Hyo-Jin Ahn JeongEun Yoo Mahshid Poornajar Imgon Hwang Stepan Kment Prof. Dr. Patrik Schmuki 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(12):2685-2692
Photoelectrochemical (PEC) water splitting is a promising method for the conversion of solar energy into chemical energy stored in the form of hydrogen. Nanostructured hematite (α-Fe2O3) is one of the most attractive materials for a highly efficient charge carrier generation and collection due to its large specific surface area and the short minority carrier diffusion length. In the present work, the PEC water splitting performance of nanostructured α-Fe2O3 is investigated which was prepared by anodization followed by annealing in a low oxygen ambient (0.03 % O2 in Ar). It was found that low oxygen annealing can activate a significant PEC response of α-Fe2O3 even at a low temperature of 400 °C and provide an excellent PEC performance compared with classic air annealing. The photocurrent of the α-Fe2O3 annealed in the low oxygen at 1.5 V vs. RHE results as 0.5 mA cm−2, being 20 times higher than that of annealing in air. The obtained results show that the α-Fe2O3 annealed in low oxygen contains beneficial defects and promotes the transport of holes; it can be attributed to the improvement of conductivity due to the introduction of suitable oxygen vacancies in the α-Fe2O3. Additionally, we demonstrate the photocurrent of α-Fe2O3 annealed in low oxygen ambient can be further enhanced by Zn-Co LDH, which is a co-catalyst of oxygen evolution reaction. This indicates low oxygen annealing generates a promising method to obtain an excellent PEC water splitting performance from α-Fe2O3 photoanodes. 相似文献
89.
Dr. Shu Min Tan Dr. Carmen C. Mayorga-Martinez Prof. Zdeněk Sofer Prof. Martin Pumera 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(29):6479-6483
Efficient exfoliation and downsizing of Sb2S3 and Bi2S3 layered compounds by using scalable bipolar electrochemistry on their suspensions in aqueous media are here demonstrated. The resulting samples were characterized in detail by transmission electron microscopy, energy-dispersive X-ray spectroscopy, and X-ray photoelectron spectroscopy; their electrochemistry toward hydrogen evolution was also investigated. Hydrogen evolution ability of exfoliated Sb2S3 and Bi2S3 was investigated and compared to the bulk counterparts. 相似文献
90.
Dr. Shuangyan Wu Dr. Mingchang Zhu Dr. Ying Zhang Prof. Marina Kosinova Prof. Vladimir P. Fedin Prof. Enjun Gao 《Chemistry (Weinheim an der Bergstrasse, Germany)》2020,26(14):3137-3144
As a hot topic of global concern, the distinguishing and detecting of antibiotic pollution is crucial owing to its adverse effect on ecosystems and human health stemming from excessive use and poor management. Herein, a water-stable lanthanide coordination polymer sensor (Dy-TCPB) with multiple emitting centers is prepared. The versatile Dy-TCPB can conveniently differentiate various antibiotics, and displays a self-calibration luminescent response to nitrofurazone (NFZ) and furazolidone (FZD). Each antibiotic exhibits notable correlation to a unique combination of the two ligand-to-Dy ion emission intensity ratios, enabling two-dimensional fingerprint recognition. Furthermore, the novel self-calibration sensor demonstrates effective recognition of NFZ and FZD with excellent sensitivity and selectivity, and detection limits as low as 0.0476 and 0.0482 μm for NFZ and FZD, respectively. The synthetic approach for the fabrication of a singular coordination polymer exhibiting multiple emissions provides a promising strategy for the development of facile and effective ratiometric sensors. 相似文献