Search Results
Architecture engineering of carbonaceous anodes for high‐rate potassium‐ion batteries
The limited lithium resource in earth's crust has stimulated the pursuit of alternative energy storage technologies to lithium‐ion battery. Potassium‐ion batteries (KIBs) are regarded as a kind of promising candidate for large‐scale energy storage owing to the high abundance and low cost of potassium resources. Nevertheless, further development and wide application of KIBs are still challenged by several obstacles, one of which is their fast capacity deterioration at high rates. A considerable amount of effort has recently been devoted to address this problem by developing advanced carbonaceous anode materials with diverse structures and morphologies. This review presents and highlights how the architecture engineering of carbonaceous anode materials gives rise to high‐rate performances for KIBs, and also the beneficial conceptions are consciously extracted from the recent progress. Particularly, basic insights into the recent engineering strategies, structural innovation, and the related advances of carbonaceous anodes for high‐rate KIBs are under specific concerns. Based on the achievements attained so far, a perspective on the foregoing, and proposed possible directions, and avenues for designing high‐rate anodes, are presented finally.
Ultrafast vibrational dynamics of the DNA backbone at different hydration levels mapped by two-dimensional infrared spectroscopy
DNA oligomers are studied at 0% and 92% relative humidity, corresponding to N < 2 and N > 20 water molecules per base pair. Two-dimensional (2D) infrared spectroscopy of DNA backbone modes between 920 and 1120 cm(-1) maps fluctuating interactions at the DNA surface. At both hydration levels, a frequency fluctuation correlation function with a 300 fs decay and a slow decay beyond 10 ps is derived from the 2D lineshapes. The fast component reflects motions of DNA helix, counterions, and water shell. Its higher amplitude at high hydration level reveals a significant contribution of water to the fluctuating forces. The slow component reflects disorder-induced inhomogeneous broadening.
Molecular couplings and energy exchange between DNA and water mapped by femtosecond infrared spectroscopy of backbone vibrations
Molecular couplings between DNA and water together with the accompanying processes of energy exchange are mapped via the ultrafast response of DNA backbone vibrations after OH stretch excitation of the water shell. Native salmon testes DNA is studied in femtosecond pump-probe experiments under conditions of full hydration and at a reduced hydration level with two water layers around the double helix. Independent of their local hydration patterns, all backbone vibrations in the frequency range from 940 to 1120 cm-1 display a quasi-instantaneous reshaping of the spectral envelopes of their fundamental absorption bands upon excitation of the water shell. The subsequent reshaping kinetics encompass a one-picosecond component, reflecting the formation of a hot ground state of the water shell, and a slower contribution on a time scale of tens of picoseconds. Such results are benchmarked by measurements with resonant excitation of the backbone modes, resulting in distinctly different absorption changes. We assign the fast changes of DNA absorption after OH stretch excitation to structural changes in the water shell which couple to DNA through the local electric fields. The second slower process is attributed to a flow of excess energy from the water shell into DNA, establishing a common heated ground state in the molecular ensemble. This interpretation is supported by theoretical calculations of the electric fields exerted by the water shell at different temperatures.