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1.
Dongshuang Wu Kohei Kusada Tomokazu Yamamoto Takaaki Toriyama Syo Matsumura Ibrahima Gueye Okkyun Seo Jaemyung Kim Satoshi Hiroi Osami Sakata Shogo Kawaguchi Yoshiki Kubota Hiroshi Kitagawa 《Chemical science》2020,11(47):12731
We report the synthesis of high-entropy-alloy (HEA) nanoparticles (NPs) consisting of five platinum group metals (Ru, Rh, Pd, Ir and Pt) through a facile one-pot polyol process. We investigated the electronic structure of HEA NPs using hard X-ray photoelectron spectroscopy, which is the first direct observation of the electronic structure of HEA NPs. Significantly, the HEA NPs possessed a broad valence band spectrum without any obvious peaks. This implies that the HEA NPs have random atomic configurations leading to a variety of local electronic structures. We examined the hydrogen evolution reaction (HER) and observed a remarkably high HER activity on HEA NPs. At an overpotential of 25 mV, the turnover frequencies of HEA NPs were 9.5 and 7.8 times higher than those of a commercial Pt catalyst in 0.05 M H2SO4 and 1.0 M KOH electrolytes, respectively. Moreover, the HEA NPs showed almost no loss during a cycling test and were much more stable than the commercial Pt catalyst. Our findings on HEA NPs may provide a new paradigm for the design of catalysts.RuRhPdIrPt high-entropy-alloy nanoparticles with a broad and featureless valence band spectrum show high hydrogen evolution reaction activity. 相似文献
2.
Direct Introduction of a Dimesitylboryl Group Using Base‐Mediated Substitution of Aryl Halides with Silyldimesitylborane 下载免费PDF全文
Dr. Eiji Yamamoto Kiyotaka Izumi Ryosuke Shishido Prof. Dr. Tomohiro Seki Noriaki Tokodai Prof. Dr. Hajime Ito 《Chemistry (Weinheim an der Bergstrasse, Germany)》2016,22(49):17547-17551
The first dimesitylboryl substitution of aryl halides with a silylborane bearing a dimesitylboryl group in the presence of alkali‐metal alkoxides is described. The reactions of aryl bromides or iodides with Ph2MeSi?BMes2 and Na(OtBu) afforded the desired aryl dimesitylboranes in good to high yields and with high borylation/silylation ratios. Selective reaction of the sterically less‐hindered C?Br bond of dibromoarenes provided monoborylated products. This reaction was used to rapidly construct a D‐π‐A aryl dimesityl borane with a non‐symmetrical biphenyl spacer. 相似文献
3.
4.
Funakawa Daiju Matsuzawa Yasumichi Sasaki Itaru Suzuki Akito Teranishi Noriaki 《Letters in Mathematical Physics》2020,110(9):2471-2490
Letters in Mathematical Physics - We study time operators for discrete-time quantum systems. Quantum walks are typical examples. We construct time operators for one-dimensional homogeneous quantum... 相似文献
5.
Genta Kawaguchi Prof. Dr. Mitsuhiko Maesato Dr. Tokutaro Komatsu Prof. Dr. Hiroshi Kitagawa Prof. Dr. Tatsuro Imakubo Dr. Andhika Kiswandhi Dr. David Graf Prof. Dr. James S. Brooks 《Angewandte Chemie (International ed. in English)》2015,54(35):10169-10172
Simultaneous manipulation of both spin and charge is a crucial issue in magnetic conductors. We report on a strong correlation between magnetism and conductivity in the iodine‐bonded molecular conductor (DIETSe)2FeBr2Cl2 [DIETSe=diiodo(ethylenedithio)tetraselenafulvalene], which is the first molecular conductor showing a large hysteresis in both magnetic moment and magnetoresistance associated with a spin‐flop transition. Utilizing a mixed‐anion approach and iodine bonding interactions, we tailored a molecular conductor with random exchange interactions exhibiting unforeseen physical properties. 相似文献
6.
Paola Zimmermann Crocomo Takahito Kaihara Soki Kawaguchi. Dr. Patrycja Stachelek Prof. Dr. Satoshi Minakata Prof. Dr. Piotr de Silva Prof. Dr. Przemyslaw Data Prof. Dr. Youhei Takeda 《Chemistry (Weinheim an der Bergstrasse, Germany)》2021,27(53):13390-13398
Novel electron donor–acceptor–donor (D-A-D) compounds comprising dibenzo[a,j]phenazine as the central acceptor core and two 7-membered diarylamines (iminodibenzyl and iminostilbene) as the donors have been designed and synthesized. Investigation of their physicochemical properties revealed the impact of C2 insertion into well-known carbazole electron donors on the properties of previously reported twisted dibenzo[a,j]phenazine-core D-A-D triads. Slight structural modification caused a drastic change in conformational preference, allowing unique photophysical behavior of dual emission derived from room-temperature phosphorescence and triplet–triplet annihilation. Furthermore, electrochemical analysis suggested sigma-dimer formation and electrochemical polymerization on the electrode. Quantum chemical calculations also rationalized the experimental results. 相似文献
7.
Keigo Kobayashi Prof. Hirokazu Kobayashi Prof. Mitsuhiko Maesato Dr. Mikihiro Hayashi Tomokazu Yamamoto Dr. Satoru Yoshioka Prof. Syo Matsumura Prof. Takeharu Sugiyama Dr. Shogo Kawaguchi Prof. Yoshiki Kubota Prof. Hiroshi Nakanishi Prof. Hiroshi Kitagawa 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2017,129(23):6678-6682
We report on hexagonal close-packed (hcp) palladium (Pd)–boron (B) nanocrystals (NCs) by heavy B doping into face-centered cubic (fcc) Pd NCs. Scanning transmission electron microscopy–electron energy loss spectroscopy and synchrotron powder X-ray diffraction measurements demonstrated that the B atoms are homogeneously distributed inside the hcp Pd lattice. The large paramagnetic susceptibility of Pd is significantly suppressed in Pd–B NCs in good agreement with the reduction of density of states at Fermi energy suggested by X-ray absorption near-edge structure and theoretical calculations. 相似文献
8.
Simultaneous measurements of velocity and temperature fluctuations in thermal boundary layer in a drag-reducing surfactant solution flow 总被引:6,自引:0,他引:6
The mechanism of turbulent heat transfer in the thermal boundary layer developing in the channel flow of a drag-reducing surfactant solution was studied experimentally. A two-component laser Doppler velocimetry and a fine-wire thermocouple probe were used to measure the velocity and temperature fluctuations simultaneously. Two layers of thermal field were found: a high heat resistance layer with a high temperature gradient, and a layer with a small or even zero temperature gradient. The peak value of
was larger for the flow with the drag-reducing additives than for the Newtonian flow, and the peak location was away from the wall. The profile of
was depressed in a similar manner to the depression of the profile of
in the flow of the surfactant solution, i.e., decorrelation between v and compared with decorrelation between u and v. The depression of the Reynolds shear stress resulted in drag reduction; similarly, it was conjectured that the heat transfer reduction is due to the decrease in the turbulent heat flux in the wall-normal direction for a flow with drag-reducing surfactant additives.List of symbols
ensemble averaged value
- (·)+
normalized by the inner wall variables
- (·)
root-mean-square value
-
C
concentration of cetyltrimethyl ammonium chloride (CTAC) solution
-
c
p
heat capacity
-
D
hydraulic diameter
-
f
friction factor
-
H
channel height
-
h
heat transfer coefficient
-
j
H
Colburn factor
-
l
length
-
Nu
Nusselt number, h
-
Pr
Prandtl number, c
p/
-
q
w
wall heated flux
-
Re
Reynolds number, U
b/
-
T
temperature
-
T
b
bulk temperature
-
T
i
inlet temperature
-
T
w
wall temperature
-
T
friction temperature, q
w
/c
p
u
-
U
local time-mean streamwise velocity
-
U
1
velocity signals from BSA1
-
U
2
velocity signals from BSA2
-
U
b
bulk velocity
-
u
streamwise velocity fluctuation
-
u1
velocity in abscissa direction in transformed coordinates
-
u
friction velocity,
-
v
wall-normal velocity fluctuation
-
v1
velocity in ordinate direction in transformed coordinates
- var(·)
variance
-
x
streamwise direction
-
y
wall-normal direction
-
z
spanwise direction
-
j
junction diameter of fine-wire TC
-
w
wire diameter of fine-wire TC
-
angle of principal axis of joint probability function p(u,v)
-
f
heat conduction of fluid
-
w
heat conduction of wire of fine-wire TC
-
kinematic viscosity
-
local time-mean temperature difference, T
w
–T
-
temperature fluctuation
-
standard deviation
-
density
-
w
wall shear stress 相似文献
9.
Yuki Sato Dr. Shin-ichi Kawaguchi Dr. Akihiro Nomoto Prof. Dr. Akiya Ogawa 《Chemistry (Weinheim an der Bergstrasse, Germany)》2019,25(9):2295-2302
Bis-phosphanated compounds are regarded as the most ubiquitous privileged ligand structures in transition-metal catalysis. The development of highly atom economical reactions is of great importance for their syntheses because less atom economical methods often require complicated purification procedures under inert atmospheres to remove excess starting materials and byproducts. Herein, the photoinduced addition reactions of diphosphane monosulfides bearing PV(S)−PIII single bonds to alkenes is disclosed. These reactions require only equimolar amounts of the diphosphane monosulfide relative to the alkene and facilitate highly selective introduction of two different types of phosphorus-containing groups, such as thiophosphoryl and phosphanyl groups, into a variety of alkenes without any catalyst, base, or additive. 相似文献
10.
Bo Huang Hirokazu Kobayashi Tomokazu Yamamoto Takaaki Toriyama Syo Matsumura Yoshihide Nishida Katsutoshi Sato Katsutoshi Nagaoka Masaaki Haneda Wei Xie Yusuke Nanba Michihisa Koyama Fenglong Wang Shogo Kawaguchi Yoshiki Kubota Hiroshi Kitagawa 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2019,131(8):2252-2257
Ru is an important catalyst in many types of reactions. Specifically, Ru is well known as the best monometallic catalyst for oxidation of carbon monoxide (CO) and has been practically used in residential fuel cell systems. However, Ru is a minor metal, and the supply risk often causes violent fluctuations in the price of Ru. Performance‐improved and cost‐reduced solid‐solution alloy nanoparticles of the Cu‐Ru system for CO oxidation are now presented. Over the whole composition range, all of the CuxRu1?x nanoparticles exhibit significantly enhanced CO oxidation activities, even at 70 at % of inexpensive Cu, compared to Ru nanoparticles. Only 5 at % replacement of Ru with Cu provided much better CO oxidation activity, and the maximum activity was achieved by 20 at % replacement of Ru by Cu. The origin of the high catalytic performance was found as CO site change by Cu substitution, which was investigated using in situ Fourier transform infrared spectra and theoretical calculations. 相似文献