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81.
Single atom catalysts (SACs) have attracted much attention in recent years. As an essential group in SACs, M−X−C (X=nonmetallic element) materials have been demonstrated to be efficient in many reactions. However, identifying the active sites on M−X−C, especially under working conditions, is still challenging, which is crucial for chemists to further understand the mechanism underlying the reaction and better design proper SACs for specific reactions. Herein, the types and characterization of M−X−C are comprehensively summarized and discussed in this review. In addition to the basic information above, the challenges and opportunities remaining in this field will be also proposed to present a perspective to the research on the next step. 相似文献
82.
Wenjuan Ma Guangzhe Yao Xuhua Huang Qi Jia Jiayuan Shen Yanxu Chang Huizi Ouyang Jun He 《Journal of separation science》2020,43(5):865-876
We investigated crude Aster tataricus, vinegar‐processed Aster tataricus, honey‐processed Aster tataricus, and steamed Aster tataricus as a case study and developed a comprehensive strategy integrating quantitative analysis and chemical pattern recognition methods for the evaluation and differentiation of Aster tataricus from different regions, as well as related processed products. In the study, 15 batches of raw Aster tataricus collected from seven provinces were analyzed. A sensitive and rapid ultra‐high performance liquid chromatography with tandem mass spectrometry method for simultaneous determination of 15 compounds was established to evaluate the quality of raw and processed Aster tataricus. Furthermore, multivariate statistical techniques were applied to compare the differences among Aster tataricus samples. As a result, the herbs collected from seven provinces were divided into two categories, and chlorogenic acid was the most important component distinguishing between the regions. Moreover, all of the raw and processed samples were classified by partial least squares discriminant analysis based on the 15 analyzed compounds. Results showed that raw Aster tataricus, vinegar‐processed Aster tataricus, honey‐processed Aster tataricus, and steamed Aster tataricus were clustered in four different areas. Shionone, chlorogenic acid and kaempferol were the significant constituents differentiating the raw and differently processed Aster tataricus samples. 相似文献
83.
Construction of 3D tissues by various types of cells with specific characteristics is an important and fundamental technology in tissue reconstruction medicine and animal‐free diagnosis system. To do so, an excellent extracellular matrix (ECM) is needed for encapsulation of cells and maintaining cell activity. Spontaneously forming hydrogel matrix is used by complexation between two water‐soluble polymers, 2‐methacryloyloxyethyl phosphorylcholine polymer bearing phenylboronic acid groups and poly(vinyl alcohol). Two cytokines for cell proliferation are immobilized in the hydrogel matrix to control the activities of the encapsulated cells. The cytokine‐immobilized hydrogel matrix can encapsulate both L929 fibroblasts and normal human dermal fibroblasts under mild condition. The physical properties of the hydrogel matrix can follow the proliferation process of the encapsulated cells. The encapsulated cells secrete ECM in the polymer hydrogel networks upon 3D culturing for 7 days. Consequently, the tissue‐mimicking ECM hybrid hydrogels are fabricated successfully. 相似文献
84.
The integration technology of hydrogen preparation–hydrogen storage not only can utilize hydrogen energy efficiently but also can improve the selectivity of the electrode maximally. In the present work, the structure and composition of the PtNi catalyst was characterized by X-ray diffraction (XRD); and its electrochemical properties, morphology, and surface binding energy were analyzed by cyclic voltammetry (CV) and linear scanning voltammetry (LSV), scanning electron microscopy equipped with energy-dispersive spectrometry (SEM-EDS), and X-ray photoelectron spectroscopy (XPS), respectively. The effects of different acid etching treatments (e.g., etching time, etchant concentration, and etching temperature) on the structure and surface active sites were investigated by the orthogonal experiment. The experimental results reveal that after etching with 0.5 mol/L of perchloric acid for 0.5 h at 60°C, the electrode weight loss of the PtNi catalyst is mainly attributed to the large loss of Ni atoms in film layer. This results in the reduced alloy phase in film layer and the appearance of Pt characteristic diffraction peak. The relative content of Pt on the surface of the film electrode increases significantly, and the total number of active sites also increases correspondingly. The binding energy of Pt4f7/2 decreases by 0.19 eV, and the number of active sites involved in hydrogen release decreases, indicative of the reduced promotion effect of the PtNi catalyst on hydrogen release. 相似文献
85.
采用沉淀法制备了ZrO2,CeO2和Ce0.7Zr0.3O2载体,并用浸渍法制备负载型Pt催化剂。考察了500和900℃焙烧催化剂的丙烷完全氧化性能和水汽对丙烷氧化反应的影响。对于500℃焙烧的催化剂,催化剂的丙烷氧化活性顺序为:Pt/ZrO2-500>Pt/CeO2-500>Pt/Ce0.7Zr0.3O2-500;而经900℃焙烧的催化剂活性顺序为:Pt/ZrO2-900>Pt/Ce0.7Zr0.3O2-900>Pt/CeO2-900。反应气氛中水汽的存在对两种Pt/ZrO2催化剂的活性均有抑制作用(T50温度均提高了10~15℃);而对于Pt/CeO2-500催化剂有抑制作用(T50温度提高10℃),但对Pt/CeO2-900催化剂活性有促进作用(T50温度下降25℃);对于两种Pt/Ce0.7Zr0.3O2催化剂活性具有促进作用(T50温度均下降5~25℃)。表征结果表明催化剂的活性与其表面Pt物种价态密切相关,催化剂表面上Pt0物种有利于活性的提高。Pt/Ce0.7Zr0.3O2-500催化剂中只含有氧化态Pt物种(Pt^2+),而Pt/Ce0.7Zr0.3O2-900催化剂中则含有部分金属态Pt物种,因此其活性高于Pt/Ce0.7Zr0.3O2-500催化剂。 相似文献
86.
Dr. Yanmei Shi Wei Du Dr. Wei Zhou Dr. Changhong Wang Shanshan Lu Dr. Siyu Lu Prof. Bin Zhang 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(50):22656-22660
Transition metal chalcogenides (TMCs) are efficient oxygen evolution reaction (OER) pre-electrocatalysts, and will in situ transform into metal (oxy)hydroxides under OER condition. However, the role of chalcogen is not fully elucidated after oxidation and severe leaching. Here we present the vital promotion of surface-adsorbed chalcogenates on the OER activity. Taking NiSe2 as an example, in situ Raman spectroscopy revealed the oxidation of Se-Se to selenites (SeO32−) then to selenates (SeO42−). Combining the severe Se leaching and the strong signal of selenates, it is assumed that the selenates are rich on the surface and play significant roles. As expected, adding selenites to the electrolyte of Ni(OH)2 dramatically enhance its OER activity. And sulfates also exhibit the similar effect, suggesting the promotion of surface-adsorbed chalcogenates on OER is universal. Our findings offer unique insight into the transformation mechanism of materials during electrolysis. 相似文献
87.
Dr. Jin-Xia Liang Prof. Dr. Jian Lin Prof. Dr. Jingyue Liu Prof. Dr. Xiaodong Wang Prof. Dr. Tao Zhang Prof. Dr. Jun Li 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(31):12968-12975
Herein, we report a theoretical and experimental study of the water-gas shift (WGS) reaction on Ir1/FeOx single-atom catalysts. Water dissociates to OH* on the Ir1 single atom and H* on the first-neighbour O atom bonded with a Fe site. The adsorbed CO on Ir1 reacts with another adjacent O atom to produce CO2, yielding an oxygen vacancy (Ovac). Then, the formation of H2 becomes feasible due to migration of H from adsorbed OH* toward Ir1 and its subsequent reaction with another H*. The interaction of Ir1 and the second-neighbouring Fe species demonstrates a new WGS pathway featured by electron transfer at the active site from Fe3+−O⋅⋅⋅Ir2+−Ovac to Fe2+−Ovac⋅⋅⋅Ir3+−O with the involvement of Ovac. The redox mechanism for WGS reaction through a dual metal active site (DMAS) is different from the conventional associative mechanism with the formation of formate or carboxyl intermediates. The proposed new reaction mechanism is corroborated by the experimental results with Ir1/FeOx for sequential production of CO2 and H2. 相似文献
88.
Prof. Nobutaka Fujieda Kyohei Umakoshi Yuta Ochi Dr. Yosuke Nishikawa Prof. Sachiko Yanagisawa Prof. Minoru Kubo Prof. Genji Kurisu Prof. Shinobu Itoh 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(32):13487-13492
The dinuclear copper enzyme, tyrosinase, activates O2 to form a (μ-η2:η2-peroxido)dicopper(II) species, which hydroxylates phenols to catechols. However, the exact mechanism of phenolase reaction in the catalytic site of tyrosinase is still under debate. We herein report the near atomic resolution X-ray crystal structures of the active tyrosinases with substrate l -tyrosine. At their catalytic sites, CuA moved toward l -tyrosine (CuA1 → CuA2), whose phenol oxygen directly coordinates to CuA2, involving the movement of CuB (CuB1 → CuB2). The crystal structures and spectroscopic analyses of the dioxygen-bound tyrosinases demonstrated that the peroxide ligand rotated, spontaneously weakening its O−O bond. Thus, the copper migration induced by the substrate-binding is accompanied by rearrangement of the bound peroxide species so as to provide one of the peroxide oxygen atoms with access to the phenol substrate's ϵ carbon atom. 相似文献
89.
Dynamic bifurcation of a modified Kuramotoben Sivashinsky equation with higher-order nonlinearity 下载免费PDF全文
Under the periodic boundary condition, dynamic bifurcation and stability in the modified Kuramoto—Sivashinsky equation with a higher-order nonlinearity μ(ux)puxx are investigated by using the centre manifold reduction procedure. The result shows that as the control parameter crosses a critical value, the system undergoes a bifurcation from the trivial solution to produce a cycle consisting of locally asymptotically stable equilibrium points. Furthermore, for cases in which the distances to the bifurcation points are small enough, one-order approximations to the bifurcation solutions are obtained. 相似文献
90.
Vibration control of the finite L-shaped beam structures based on the active and reactive power flow
LIU ChunChuan LI FengMing TANG Liang & HUANG WenHu P.O.Box School of Astronautics Harbin Institute of Technology Harbin China P.O.Box National Laboratory of Space Intelligent Control Beijing Institute of Control Engineering Beijing 《中国科学:物理学 力学 天文学(英文版)》2011,(2)
This paper analyzes the physical meaning of the active and reactive power flow in the finite L-shaped beams and studies the active vibration control of the structures based on the active and reactive power flow.The traveling wave approach is used to calculate the structural dynamic responses.Because the error of control force is inevitable in practical applications,the effects of the error of control force on the control results are studied.The study indicates that the error of control force has pronounced ... 相似文献