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排序方式: 共有6528条查询结果,搜索用时 15 毫秒
1.
Qianqian Fan Zirui Liu Feng Qiu Prof. Yong Mao Prof. Qingju Liu Prof. Longzhou Zhang 《Chemistry (Weinheim an der Bergstrasse, Germany)》2022,28(63):e202202700
The artificially accurate design of nonmetal electrocatalysts’ active site has been a huge challenge because no pure active species with the specific structure could be strictly controlled by traditional synthetic methods. Species with a multiconfiguration in the catalyst hinder identification of the active site and the subsequent comprehension of the reaction mechanism. We have developed a novel electro-assisted molecular assembly strategy to obtain a pure pentagon ring on perfect graphene avoiding other reconstructed structures. More importantly, the active atom was confirmed by the subtle passivation process as the topmost carbon atom. Recognition of the carbon-defect electrocatalysis reaction mechanism was first downsized to the single-atom scale from the experimental perspective. It is expected that this innovative electro-assisted molecular assembly strategy could be extensively applied in the active structure-controlled synthesis of nonmetal electrocatalysts and verification of the exact active atom. 相似文献
2.
Dr. Yong-Sheng Wei Dr. Liming Sun Miao Wang Dr. Jinhua Hong Dr. Lianli Zou Hongwen Liu Dr. Yu Wang Dr. Mei Zhang Dr. Zheng Liu Prof. Yinwei Li Prof. Satoshi Horike Prof. Kazu Suenaga Prof. Qiang Xu 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(37):16147-16156
Understanding the thermal aggregation behavior of metal atoms is important for the synthesis of supported metal clusters. Here, derived from a metal–organic framework encapsulating a trinuclear FeIII2FeII complex (denoted as Fe3) within the channels, a well-defined nitrogen-doped carbon layer is fabricated as an ideal support for stabilizing the generated iron nanoclusters. Atomic replacement of FeII by other metal(II) ions (e.g., ZnII/CoII) via synthesizing isostructural trinuclear-complex precursors (Fe2Zn/Fe2Co), namely the “heteroatom modulator approach”, is inhibiting the aggregation of Fe atoms toward nanoclusters with formation of a stable iron dimer in an optimal metal–nitrogen moiety, clearly identified by direct transmission electron microscopy and X-ray absorption fine structure analysis. The supported iron dimer, serving as cooperative metal–metal site, acts as efficient oxygen evolution catalyst. Our findings offer an atomic insight to guide the future design of ultrasmall metal clusters bearing outstanding catalytic capabilities. 相似文献
3.
Wang Hay Kan Chenxi Wei Dongchang Chen Tao Bo Bao‐Tian Wang Yan Zhang Yangchao Tian Jun‐Sik Lee Yijin Liu Guoying Chen 《Advanced functional materials》2019,29(17)
Lithium‐rich disordered rock‐salt oxides have attracted great interest owing to their promising performance as Li‐ion battery cathodes. While experimental and theoretical efforts are critical in advancing this class of materials, a fundamental understanding of key property changes upon Li extraction is largely missing. In the present study, single‐crystal synthesis of a new disordered rock‐salt cathode material, Li1.3Ta0.3Mn0.4O2 (LTMO), and its use as a model compound to investigate Li concentration–driven evolution of local cationic ordering, charge compensation, and chemical distribution are reported. Through the combined use of 2D and 3D X‐ray nanotomography, it is shown that Li removal accompanied by oxygen oxidation is correlated with the development of morphological defects such as particle cracking. Chemical heterogeneity, quantified by subparticle level distribution of Mn valence state, is minimal during Mn redox, which drastically increases upon the formation of cracks during oxygen redox. Density functional theory and bond valence sum mismatch calculations reveal the presence of local short‐range ordering in the pristine oxide, which gradually disappears along with the extraction of Li. The study suggests that with cycling the transformation into true cation–disordered state can be expected, which likely impacts the voltage profile and obtainable energy density of the oxide cathodes. 相似文献
4.
Dekun Wu Dr. Qing Xu Dr. Jing Qian Prof. Xiaopeng Li Prof. Yuhan Sun 《Chemistry (Weinheim an der Bergstrasse, Germany)》2019,25(12):3105-3111
Covalent organic frameworks (COFs) are a new class of crystalline porous polymers comprised mainly of carbon atoms, and are versatile for the integration of heteroatoms such as B, O, and N into the skeletons. The designable structure and abundant composition render COFs useful as precursors for heteroatom-doped porous carbons for energy storage and conversion. Herein, we describe a multifunctional electrochemical catalyst obtained through pyrolysis of a bimetallic COF. The catalyst possesses hierarchical pores and abundant iron and cobalt nanoparticles embedded with standing carbon layers. By integrating these features, the catalyst exhibits excellent electrochemical catalytic activity in the oxygen reduction reaction (ORR), with a 50 mV positive half-wave potential, a higher limited diffusion current density, and a much smaller Tafel slope than a Pt-C catalyst. Moreover, the catalyst displays superior electrochemical performance toward the hydrogen evolution reaction (HER), with overpotentials of −0.26 V and −0.33 V in acidic and alkaline aqueous solution, respectively, at a current density of 10 mA cm−2. The overpotential in the catalysis of the oxygen evolution reaction (OER) was 1.59 V at the same current density. 相似文献
5.
Michiel Janssen Prof. Dirk E. De Vos 《Chemistry (Weinheim an der Bergstrasse, Germany)》2019,25(45):10724-10734
The practical application of Shilov-type Pt catalysis to the selective hydroxylation of terminal aliphatic C−H bonds remains a formidable challenge, due to difficulties in replacing PtIV with a more economically viable oxidant, particularly O2. We report the potential of employing FeCl2 as a suitable redox mediator to overcome the kinetic hurdles related to the direct use of O2 in the Pt reoxidation. For the selective conversion of butyric acid to γ-hydroxybutyric acid (GHB), a significantly enhanced catalyst activity and stability (turnover numbers (TON)>30) were achieved under 20 bar O2 in comparison to current state-of-the-art systems (TON<10). In this regard, essential reaction parameters affecting the overall activity were identified, along with specific additives to attain catalyst stability at longer reaction times. Notably, deactivation by reduction to Pt0 was prevented by the addition of monodentate pyridine derivatives, such as 2-fluoropyridine, but also by introducing varying partial pressures of N2 in the gaseous atmosphere. Finally, stability tests revealed the involvement of PtII and FeCl2 in catalyzing the non-selective overoxidation of GHB. Accordingly, in situ esterification with boric acid proved to be a suitable strategy to maintain enhanced selectivities at much higher conversions (TON>60). Altogether, a useful catalytic system for the selective hydroxylation of primary aliphatic C−H bonds with O2 is presented. 相似文献
6.
Yaping Chen Dr. Kun Rui Prof. Jixin Zhu Prof. Shi Xue Dou Dr. Wenping Sun 《Chemistry (Weinheim an der Bergstrasse, Germany)》2019,25(3):703-713
Developing clean and sustainable energies as alternatives to fossil fuels is in strong demand within modern society. The oxygen evolution reaction (OER) is the efficiency-limiting process in plenty of key renewable energy systems, such as electrochemical water splitting and rechargeable metal–air batteries. In this regard, ongoing efforts have been devoted to seeking high-performance electrocatalysts for enhanced energy conversion efficiency. Apart from traditional precious-metal-based catalysts, nickel-based compounds are the most promising earth-abundant OER catalysts, attracting ever-increasing interest due to high activity and stability. In this review, the recent progress on nickel-based oxide and (oxy)hydroxide composites for water oxidation catalysis in terms of materials design/synthesis and electrochemical performance is summarized. Some underlying mechanisms to profoundly understand the catalytic active sites are also highlighted. In addition, the future research trends and perspectives on the development of Ni-based OER electrocatalysts are discussed. 相似文献
7.
Dong-Soo Yoon Jae Sung Roh Sung-Man Lee Hong Koo Baik 《Journal of Electronic Materials》2003,32(8):890-898
The effect of a thin RuOx layer formed on the Ru/TiN/doped poly-Si/Si stack structure was compared with that on the RuOx/TiN/doped poly-Si/Si stack structure over the post-deposition annealing temperature ranges of 450–600°C. The Ru/TiN/poly-Si/Si
contact system exhibited linear behavior at forward bias with a small increase in the total resistance up to 600°C. The RuOx/TiN/poly-Si/Si contact system exhibited nonlinear characteristics under forward bias at 450°C, which is attributed to no
formation of a thin RuOx layer at the RuOx surface and porous-amorphous microstructure. In the former case, the addition of oxygen at the surface layer of the Ru film
by pre-annealing leads to the formation of a thin RuOx layer and chemically strong Ru-O bonds. This results from the retardation of oxygen diffusion caused by the discontinuity
of diffusion paths. In particular, the RuOx layer in a nonstoichiometric state is changed to the RuO2-crystalline phase in a stoichiometric state after post-deposition annealing; this phase can act as an oxygen-capture layer.
Therefore, it appears that the electrical properties of the Ru/TiN/poly-Si/Si contact system are better than those of the
RuOx/TiN/poly-Si/Si contact system. 相似文献
8.
针对VO2薄膜在微测辐射热计上的应用,采用射频反应溅射法,在室温下制备氧化钒薄膜;研究了氧分压对薄膜沉积速率、电学性质及成分的影响.通过调节氧分压,先获得成分接近VO2的非晶化薄膜,再在400℃空气中氧化退火,便可制得高电阻温度系数,低电阻率的VO2薄膜,电阻温度系数约为-4%/℃,薄膜方块电阻为R□为100—300kΩ;薄膜在室温下沉积,400℃下退火的制备方法与微机电加工(micro electromechanic
关键词:
二氧化钒
电阻温度系数
氧分压
射频反应溅射法 相似文献
9.
Results of two urgent and practically important directions of research on the indirect oxidation of organic compounds by highly reactive intermediates generated electrochemically from oxygen (HO2
–, HO2
·, HO·) are considered and orderly arranged. The studies in question are the indirect synthesis and mineralization of organic toxicants in waste water. 相似文献
10.
Ya. I. Kurys’ N. S. Netyaga V. G. Koshechko V. D. Pokhodenko 《Theoretical and Experimental Chemistry》2007,43(5):334-342
A guest-host nanocomposite based on electroconducting polyaniline doped with 12-phosphotungstic acid and V2O5 as well as its bifunctional analog containing not more than 5 mass% nanosized platinum were obtained. A study was carried
out on the structure of these nanocomposites, their redox characteristics, and electrocatalytic activity in the reduction
of oxygen. These nanocomposites were found to display catalytic properties in the electrochemical reduction of oxygen, while
the presence of even a slight amount of nanosized platinum in the bifunctional composite leads to a significant increase in
its electrocatalytic activity.
__________
Translated from Teoreticheskaya i éksperimental’naya Khimiya, Vol. 43, No. 5, pp. 307–314, September–October, 2007. 相似文献