29 May 12:32
by Shengnan Sun,
Yuanmiao Sun,
Ye Zhou,
Shibo Xi,
Xiao Ren,
Bicheng Huang,
Hanbin Liao,
Luyuan Paul Wang,
Yonghua Du,
Zhichuan J. Xu
The oxygen evolution activity of Co‐based spinel oxides is dominated by the catalytically critical TMO6 octahedra. Pushing more active Co into octahedral sites and shifting the oxygen charge to octahedral Co significantly enhance the activity.
Abstract
Cobalt spinel oxides are a class of promising transition metal (TM) oxides for catalyzing oxygen evolution reaction (OER). Their catalytic activity depends on the electronic structure. In a spinel oxide lattice, each oxygen anion is shared amongst its four nearest transition metal cations, of which one is located within the tetrahedral interstices and the remaining three cations are in the octahedral interstices. This work uncovered the influence of oxygen anion charge distribution on the electronic structure of the redox‐active building block Co−O. The charge of oxygen anion tends to shift toward the octahedral‐occupied Co instead of tetrahedral‐occupied Co, which hence produces strong orbital interaction between octahedral Co and O. Thus, the OER activity can be promoted by pushing more Co into the octahedral site or shifting the oxygen charge towards the redox‐active metal center in CoO6 octahedra.
17 Jun 23:27
by Hong‐Bao
Sun
,
Liang
Gong
,
Yu‐Biao
Tian
,
Jin‐Gui
Wu
,
Xia
Zhang
,
Jie
Liu
,
Zhengyan
Fu
,
Prof.
Dawen
Niu
Angewandte Chemie International Edition, EarlyView.
29 Sep 12:21
by kewei Wang, Liming Yang, Xi wang, Liping Guo, Guang Cheng, Chun Zhang, Shangbin Jin, Bien Tan, Andrew Cooper
Abstract
Covalent triazine frameworks (CTFs) are normally synthesized by ionothermal methods. The harsh synthetic conditions and associated limited structural diversity do not benefit for further development and practical large-scale synthesis of CTFs. Herein we report a new strategy to construct CTFs (CTF-HUSTs) via a polycondensation approach, which allows the synthesis of CTFs under mild conditions from a wide array of building blocks. Interestingly, these CTFs display a layered structure. The CTFs synthesized were also readily scaled up to gram quantities. The CTFs are potential candidates for separations, photocatalysis and for energy storage applications. In particular, CTF-HUSTs are found to be promising photocatalysts for sacrificial photocatalytic hydrogen evolution with a maximum rate of 2647 μmol h−1 g−1 under visible light. We also applied a pyrolyzed form of CTF-HUST-4 as an anode material in a sodium-ion battery achieving an excellent discharge capacity of 467 mAh g−1.
Layered allrounder: A novel polycondensation approach enables the construction of covalent triazine frameworks (CTFs) under mild conditions from a wide array of building blocks. The resulting CTFs present a new type of layered material with potential applications in separations, photocatalysis, and energy storage.
28 May 11:48
by Jumei Li, Jingyue Liu, Yin Yang and Dong Qin
Journal of the American Chemical Society
DOI: 10.1021/jacs.5b03528
18 Mar 22:22
by Matthew G. Cowan, William M. McDanel, Hans H. Funke, Yuki Kohno, Douglas L. Gin, Richard D. Noble
Abstract
Following removal of coordinated CH3CN, the resulting complexes [AgI(2,2′-bipyridine)][BF4] (1) and [AgI(6,6′-dimethyl-2,2′-bipyridine)][OTf] (2) show ethene/ethane sorption selectivities of 390 and 340, respectively, and corresponding ethene sorption capacities of 2.38 and 2.18 mmol g−1 when tested at an applied gas pressure of 90 kPa and a temperature of (20±1) °C. These ethene/ethane selectivities are 13 times higher than those reported for known solid sorbents for ethene/ethane separation. For 2, ethene sorption reached 90 % of equilibrium capacity within 15 minutes, and this equilibrium capacity was maintained over the three sorption/desorption cycles tested. The rates of ethene sorption were also measured. To our knowledge, these are the first complexes, designed for olefin/paraffin separations, which have open silver(I) sites. The high selectivities arise from these open silver(I) sites and the relatively low molecular surface areas of the complexes.
Site unseen: The coordination complexes 1 and 2, having open silver(I) sites, were prepared and investigated for ethene/ethane binding. These complexes display ethene/ethane selectivity of up to 13 times higher than comparable solid sorbents, ethene loadings of up to 2.38 mmol g−1, and saturation of silver(I) sites of up to 0.96 molethene/molsilver(I). Tf=trifluoromethanesulfonyl.