Single-crystal metals have distinctive properties owing to the absence of grain boundaries and strong anisotropy. Commercial single-crystal metals are usually synthesized by bulk crystal growth or by deposition of thin films onto substrates, and they are expensive and small. We prepared extremely large single-crystal metal foils by “contact-free annealing” from commercial polycrystalline foils. The colossal grain growth (up to 32 square centimeters) is achieved by minimizing contact stresses, resulting in a preferred in-plane and out-of-plane crystal orientation, and is driven by surface energy minimization during the rotation of the crystal lattice followed by “consumption” of neighboring grains. Industrial-scale production of single-crystal metal foils is possible as a result of this discovery.
Fast charging rate and large energy storage are becoming key elements for the development of nextgeneration batteries, targeting high-performance electric vehicles. Developing electrodes with high volumetric and gravimetric capacity that could be operated at a high rate is the most challenging part of this process. Using silicon as the anode material, which exhibits the highest theoretical capacity as a lithium-ion battery anode, we report a binder-free electrode that interconnects carbon-sheathed porous silicon nanowires into a coral-like network and shows fast charging performance coupled to high energy and power densities when integrated into a full cell with a high areal capacity loading. The combination of interconnected nanowires, porous structure, and a highly conformal carbon coating in a single system strongly promotes the reaction kinetics of the electrode. This leads to fast-charging capability while maintaining the integrity of the electrode without structural collapse and, thus, stable cycling performance without using binder and conductive additives. Specifically, this anode shows high specific capacities (over 1200 mAh g −1 ) at an ultrahigh charging rate of 7 C over 500 charge−discharge cycles. When coupled with a commercial LiCoO 2 or LiFePO 4 cathode in a full cell, it delivers a volumetric energy density of 1621 Wh L −1 with a LiCoO 2 cathode and a power density of 7762 W L −1 with a LiFePO 4 cathode.
Single‐crystal electron diffraction has shown to be powerful for structure determination of nano‐ and submicron‐sized crystals that are too small to be studied by single‐crystal X‐ray diffraction. However, it has been very challenging to obtain high quality electron diffraction data from beam sensitive crystals such as metal–organic frameworks (MOFs). It is even more difficult to locate guest species in the pores of MOF crystals. Here, we present synthesis of a novel porous cobalt MOF with 1D channels, [Co2(Ni‐H4TPPP)]⋅2 DABCO⋅6 H2O, (denoted Co‐CAU‐36; DABCO=1,4‐diazabicyclo[2.2.2]octane), and its structure determination using continuous rotation electron diffraction (cRED) data. By combining a fast hybrid electron detector with low sample temperature (96 K), high resolution (0.83–1.00 Å) cRED data could be obtained from eight Co‐CAU‐36 crystals. Independent structure determinations were conducted using each of the eight cRED datasets. We show that all atoms in the MOF framework could be located. More importantly, we demonstrate for the first time that organic molecules in the pores, which were previously difficult to find, could be located using the cRED data. A comparison of eight independent structure determinations using different datasets shows that structural models differ only on average by 0.03(2) Å for the framework atoms and 0.10(6) and 0.16(12) Å for DABCO and water molecules, respectively.
The phase transition
from the kinetically favored tetragonal form
II into the thermodynamically stable hexagonal form I is the general
phenomenon and core issue in application of polybutene-1-based materials.
It is known that the variation of molecular structure by copolymerizing
counits and the imposition of external stretching both greatly affect
the phase transition. In this work, a series of butene-1/4-methyl-1-pentene
(4M1P) random copolymers were synthesized with the dimethylpyridylamidohafnium/organoboron
catalyst, where the 4M1P incorporated is the counit type of depressing
II–I phase transition. Mechanical tests were combined with
the in-situ wide-angle X-ray diffraction (WAXD) method to study the
competing effects of the presence of 4M1P counits and stretching on
the II–I phase transition. First of all, the quiescent experiments
reveal that addition of 4M1P counits not only slows down transition
kinetics but also decreases the ultimate form I fraction in the transition
plateau. The 4M1P concentration ≥3.40 mol % is high enough
to completely impede the II–I phase transition even when the
aging time is as long as 4 months. Second, the stretching-induced
phase transition was explored with the combined structural and mechanical
information from WAXD and mechanical characterizations, respectively.
The influence of stretching stimuli in the phase transition varies
with 4M1P concentration. For low 4M1P concentration ≤1.00 mol
%, stretching significantly accelerates the transition kinetics and
induces the complete transition of form II. For intermediate 4M1P
concentration 3.40 mol %, stretching effectively triggers the occurrence
of the II–I phase transition, which does not start under quiescent
conditions but only induces partial transition until fracture. For
high 4M1P concentration ranging from 7.80 to 30.1 mol %, stretching
just orientates the form II crystallites without starting any phase
transition to form I. Third, as the concentration of 4M1P counits
is increased, the phase transition is accomplished with different
orientations, which determines the microscopic stress applied to lamellae.
Then, detailed kinetics of the II–I phase transition was correlated
to the stretching stimuli of the total true stress, component stresses
parallel and perpendicular to the c-axis in the crystal
lattice. It was interesting to find that transition kinetics is dominated
by the component stress perpendicular to the c-axis
for the off-axis orientation pathway. For the molecular mechanism
of the phase transition, this indicates that the activated chain lateral
slip is the dominant process for nucleation of form I within original
form II.
Inspired by biological attachment systems, we fabricated the honeycomb structural films with different diameters by breath figure (BF) method, which were similar to the patterned octopus suckers. The experimental results showed, besides different van der Waals forces between the polystyrene (PS) surfaces and water, another important factor; that is, different negative pressures produced by different volumes of sealed air could be a crucial factor for the different adhesions. So the water adhesive forces of the as-prepared films can be effectively controlled from relative high to relative low adhesion by varying the pore diameters, which effectively adjusted the negative pressures produced by the pores. This unique adhesive phenomenon of honeycomb structure will be very useful for manipulating water droplet behaviors, as well as controlling liquid collection and transportation. These findings are interesting and helpful for us to further understand the biological attachment systems and to optimize the design of artificial analogues.
We present a microfluidic approach for single-molecule studies of the temperature-dependent behavior of biomolecules, using a platform that combines microfluidic sample handling, on-chip temperature control, and total internal reflection fluorescence (TIRF) microscopy of surfaceimmobilized biomolecules. With efficient, rapid, and uniform heating by microheaters and in situ temperature measurements within a microfluidic flowcell by micro temperature sensors, closedloop, accurate temperature control is achieved. To demonstrate its utility, the temperaturecontrolled microfluidic flowcell is coupled to a prism-based TIRF microscope and is used to investigate the temperature-dependence of ribosome and transfer RNA (tRNA) structural dynamics that are required for the rapid and precise translocation of tRNAs through the ribosome during protein synthesis. Our studies reveal that the previously characterized, thermally activated transitions between two global conformational states of the pre-translocation (PRE) ribosomal complex persist at physiological temperature. In addition, the temperature-dependence of the rates of transition between these two global conformational states of the PRE complex reveal welldefined, measurable, and disproportionate effects, providing a robust experimental framework for investigating the thermodynamic activation parameters that underlie transitions across these barriers.
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