Photocatalytic
ammonia synthesis from N2 is a carbon-neutral
strategy, although its efficiency is impeded by the activation of
inert NN triple bonds. In N2 activation, the electron
acceptance process is often strongly coupled with the electron donation
process, leading to a high potential activation energy barrier and
low photocatalytic activity. Herein, we proposed a strategy to decouple
these two processes by bimetallic organic frameworks (BMOFs) for boosting
N2 activation. The rationally designed BMOFs are composed
of two functional metal nodes, in which the hard acid metal node with
a high ionization potential (I
n) accepts
the electron from N2 and the soft acid metal node with
a low I
n donates the electron to N2. Owing to the bimetal synergistic effect, the potential activation
energy barrier of N2 is reduced, as confirmed by the in situ Fourier transform infrared (FTIR) spectra and density
functional theory (DFT) calculations. Via testing six kinds of bimetal
combinations, it is found that, as the ionization potential difference
(ΔI
n) between the two metals is
≥6 eV and the proportion of high I
n metal reaches ∼20%, the bimetal synergistic effect becomes
dominant. In all the as-prepared BMOFs, the optimal BMOF(Sr)–0.2Fe
photocatalyst exhibits an NH3 evolution rate up to 780
μmol g–1 h–1. This work
may unveil a corner of the hidden mechanism for the chemical bond
activation in a broad range of catalytic processes.
The evolution of temperature and thermal stresses during friction stir welding of Al6061-T6 was investigated by means of in situ, time resolved neutron diffraction technique. A method was developed to deconvolute the temperature and stress from the lattice spacing changes measured by neutron diffraction. The deep penetration capability of neutrons made it possible for the first time to obtain the temperature and thermal stresses inside a friction stir weld.
Carbonization of nature-inspired polydopamine can yield thin films with high electrical conductivity. Understanding of the structure of carbonized PDA (cPDA) is therefore highly desired. In this study, neutron diffraction, Raman spectroscopy, and other techniques indicate that cPDA samples are mainly amorphous with some short-range ordering and graphite-like structure that emerges with increasing heat treatment temperature. The electrical conductivity and the Seebeck coefficient show different trends with heat treatment temperature, while the thermal conductivity remains insensitive. The largest room-temperature ZT of 2 × 10 was obtained on samples heat-treated at 800 °C, which is higher than that of reduced graphene oxide.
Rational manipulation of the photogenerated charge transfer inside the photocatalyst is key to enhancing the photocatalytic performance. Herein, inspired by the charge transport chain in natural photosynthesis, a novel multi-stepwise...
On Friday June 26, 2009, the neutron beam shutter for the VULCAN diffractometer at the SNS was opened for the first time. Initial measurements to characterize the instrument performance are reported. It is shown that the measurement results are by and large in agreement with design calculations. New research opportunities with VULCAN are discussed.
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