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result(s) for
"Hu, Daqiao"
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Dual-quartet phosphorescent emission in the open-shell M1Ag13 (M = Pt, Pd) nanoclusters
2024
Dual emission (DE) in nanoclusters (NCs) is considerably significant in the research and application of ratiometric sensing, bioimaging, and novel optoelectronic devices. Exploring the DE mechanism in open-shell NCs with doublet or quartet emissions remains challenging because synthesizing open-shell NCs is difficult due to their inherent instability. Here, we synthesize two dual-emissive M
1
Ag
13
(PFBT)
6
(TPP)
7
(M = Pt, Pd; PFBT = pentafluorobenzenethiol; TPP = triphenylphosphine) NCs with a 7-electron open-shell configuration to reveal the DE mechanism. Both NCs comprise a crown-like M
1
Ag
11
kernel with Pt or Pd in the center surrounded by five PPh
3
ligands and two Ag(SR)
3
(PPh
3
) motifs. The combined experimental and theoretical studies revealed the origin of DE in Pt
1
Ag
13
and Pd
1
Ag
13
. Specifically, the high-energy visible emission and the low-energy near-infrared emission arise from two distinct quartet excited states: the core-shell charge transfer and core-based states, respectively. Moreover, PFBT ligands are found to play an important role in the existence of DE, as its low-lying
π
* levels result in energetically accessible core-shell transitions. This novel report on the dual-quartet phosphorescent emission in NCs with an open-shell electronic configuration advances insights into the origin of dual-emissive NCs and promotes their potential application in magnetoluminescence and novel optoelectronic devices.
Exploring the dual-emission mechanism in open-shell nanoclusters with doublet or quartet emissions remains challenging. Here, the authors reveal the origin of dual-quartet phosphorescent emission in the open-shell M1Ag13 (M = Pt, Pd) nanoclusters.
Journal Article
Interdependence between nanoclusters AuAg24 and Au2Ag41
2021
Whole series of nanoparticles have now been reported, but probing the competing or coexisting effects in their synthesis and growth remains challenging. Here, we report a bi-nanocluster system comprising two ultra-small, atomically precise nanoclusters, AuAg
24
(SR)
18
−
and Au
2
Ag
41
(SR)
26
(Dppm)
2
+
(SR = cyclohexyl mercaptan, Dppm = bis(diphenylphosphino)-methane). The mechanism by which these two nanoclusters coexist is elucidated, and found to entail formation of the unstable AuAg
24
(SR)
18
−
, followed by its partial conversion to Au
2
Ag
41
(SR)
26
(Dppm)
2
+
in the presence of di-phosphorus ligands, and an interdependent bi-nanocluster system is established, wherein the two oppositely charged nanoclusters protect each other from decomposition. AuAg
24
(SR)
18
and Au
2
Ag
41
(SR)
26
(Dppm)
2
are fully characterized by single crystal X-ray diffraction (SC-XRD) analysis – it is found that their co-crystallization results in single crystals comprising equimolar amounts of each. The findings highlight the interdependent relationship between two individual nanoclusters, which paves the way for new perspectives on nanocluster formation and stability.
Despite recent progress in individual nanocluster synthesis, understanding the competing or coexisting effects between particles in solution remains challenging. Here, the authors present the synthesis of a bi-nanocluster system comprising two atomically precise nanoclusters, and map out the interdependent relationship between them.
Journal Article
Active metal (cadmium) doping enhanced the stability of inert metal (gold) nanocluster under O2 atmosphere and the catalysis activity of benzyl alcohol oxidation
2015
Compared with the inert metal (gold), the active metal (Cd) is much more prone to oxidation, leading to its high oxidation state. In this work, we found that doping the homogold Au
25
(SR)
18
nanocluster with cadmium largely enhances its stability. The differential pulse voltammetry (DPV) analysis suggested that Cd doping raised the high occupied molecular orbital (HOMO) energy of homogold Au
25
nanocluster, which led to stronger retention of its valence electrons. Cd
1
Au
24
(SR)
18
nanocluster also exhibited much higher activity than homogold Au
25
nanocluster in aerobic benzyl alcohol oxidation.
Journal Article
Dual-quartet phosphorescent emission in the open-shell M 1 Ag 13 (M = Pt, Pd) nanoclusters
2024
Dual emission (DE) in nanoclusters (NCs) is considerably significant in the research and application of ratiometric sensing, bioimaging, and novel optoelectronic devices. Exploring the DE mechanism in open-shell NCs with doublet or quartet emissions remains challenging because synthesizing open-shell NCs is difficult due to their inherent instability. Here, we synthesize two dual-emissive M
Ag
(PFBT)
(TPP)
(M = Pt, Pd; PFBT = pentafluorobenzenethiol; TPP = triphenylphosphine) NCs with a 7-electron open-shell configuration to reveal the DE mechanism. Both NCs comprise a crown-like M
Ag
kernel with Pt or Pd in the center surrounded by five PPh
ligands and two Ag(SR)
(PPh
) motifs. The combined experimental and theoretical studies revealed the origin of DE in Pt
Ag
and Pd
Ag
. Specifically, the high-energy visible emission and the low-energy near-infrared emission arise from two distinct quartet excited states: the core-shell charge transfer and core-based states, respectively. Moreover, PFBT ligands are found to play an important role in the existence of DE, as its low-lying π* levels result in energetically accessible core-shell transitions. This novel report on the dual-quartet phosphorescent emission in NCs with an open-shell electronic configuration advances insights into the origin of dual-emissive NCs and promotes their potential application in magnetoluminescence and novel optoelectronic devices.
Journal Article
Interdependence between nanoclusters AuAg 24 and Au 2 Ag 41
2021
Whole series of nanoparticles have now been reported, but probing the competing or coexisting effects in their synthesis and growth remains challenging. Here, we report a bi-nanocluster system comprising two ultra-small, atomically precise nanoclusters, AuAg
(SR)
and Au
Ag
(SR)
(Dppm)
(SR = cyclohexyl mercaptan, Dppm = bis(diphenylphosphino)-methane). The mechanism by which these two nanoclusters coexist is elucidated, and found to entail formation of the unstable AuAg
(SR)
, followed by its partial conversion to Au
Ag
(SR)
(Dppm)
in the presence of di-phosphorus ligands, and an interdependent bi-nanocluster system is established, wherein the two oppositely charged nanoclusters protect each other from decomposition. AuAg
(SR)
and Au
Ag
(SR)
(Dppm)
are fully characterized by single crystal X-ray diffraction (SC-XRD) analysis - it is found that their co-crystallization results in single crystals comprising equimolar amounts of each. The findings highlight the interdependent relationship between two individual nanoclusters, which paves the way for new perspectives on nanocluster formation and stability.
Journal Article
Preparation and characterization of hydrogen-bonded P4VP-bisazobenzene complexes
by
Zhang, Qijin
,
Zou, Gang
,
Hu, Daqiao
in
Acetal resins
,
Azo compounds
,
Characterization and Evaluation of Materials
2012
Photoresponsive supramolecular complexes contain 4-hydroxyethyloxy-4′-(4-nitrophenylazo)azobenzene(BisAzo) molecule as a hydrogen bonding donor and poly(4-vinylpyridine) (P4VP) as a hydrogen bonding acceptor, and strong phenol pyridine hydrogen bonding is formed between them. FT-IR spectrum verifies the hydrogen bonding has formed between the phenol hydroxyl of BisAzo and pyridine ring of P4VP. The glass- transition temperature (
Tg
) is determined with differential-scanning calorimetry(DSC) and a decrease of complexes compared with pure P4VP is observed due to the attachment of BisAzo onto the backbone of P4VP. Polarized optical microscopy (POM) is performed to study the structure of supramolecular complexes,with a different texture observed which is different from both constituents alone. X-ray diffraction patterns are investigated with the same films already used for POM observation, indicating a lamellar structure with a periodic thickness of 4.1 nm. The supramolecular complexes P4VP/(BisAzo)
x
are prepared with the molar ratio of BisAzo to the pyridine group varied at
x
= 0.25, 0.5, 0.75 and 1.0, no mass aggregation is observed even at a high concentration of chromophore.
Journal Article
Active metal (cadmium) doping enhanced the stability of inert metal (gold) nanocluster under O sub(2) atmosphere and the catalysis activity of benzyl alcohol oxidation
2015
Compared with the inert metal (gold), the active metal (Cd) is much more prone to oxidation, leading to its high oxidation state. In this work, we found that doping the homogold Au sub(25)(SR) sub(18) nanocluster with cadmium largely enhances its stability. The differential pulse voltammetry (DPV) analysis suggested that Cd doping raised the high occupied molecular orbital (HOMO) energy of homogold Au sub(25) nanocluster, which led to stronger retention of its valence electrons. Cd sub(1)Au sub(24)(SR) sub(18) nanocluster also exhibited much higher activity than homogold Au sub(25) nanocluster in aerobic benzyl alcohol oxidation.
Journal Article
Flow Field Study of Sodium Aluminate Solution Slurry in an Unagitated Precipitation Tank by CFD Simulation
by
Hu, Da Qiao
,
Wang, Fan
,
Su, Xiang Dong
in
Computational fluid dynamics
,
Computer simulation
,
Mathematical models
2013
In order to explore the feasibility of remove agitation in gibbsite precipitation process, computational fluid dynamics method was carried out to study the flow field of sodium aluminate solution slurry in an unagitated precipitation tank. The solid content distribution is investigated by volume fraction of solid phase. The simulation results showed that little difference of solid content is found in the range between the tank bottom and the height position of 25 meters, which is the most zone of the tank, and there is a somewhat large difference in the top 5 meters zone, where the stratification occurs. With the inlet velocity increases, the zone of stratification shrinks to near the tank surface, which makes the solid content distribution in the whole tank seem uniform much more. Therefore, without agitation, the solid content would not concentrate to tank bottom completely in the normal work flow.
Journal Article
Activation and Disproportionation of Zr2Fe Alloy as Hydrogen Storage Material
2019
As a hydrogen storage material, Zr2Fe alloy has many advantages such as fast hydrogen absorption speed, high tritium recovery efficiency, strong anti-pulverization ability, and difficulty self-igniting in air. Zr2Fe alloy has lower hydrogen absorption pressure at room temperature than LaNi5 alloy. Compared with the ZrVFe alloy, the hydrogen release temperature of Zr2Fe is lower so that the material can recover hydrogen isotopes at lower hydrogen concentration efficiently. Unfortunately, the main problem of Zr2Fe alloy in application is that a disproportionation reaction is easy to occur after hydrogen absorption at high temperature. At present, there is little research on the generation and influencing factors of a disproportionation reaction in Zr2Fe alloy. In this paper, the effects of temperature and hydrogen pressure on the disproportionation of Zr2Fe alloy were studied systematically. The specific activation conditions and experimental parameters for reducing alloy disproportionation are given, which provide a reference for the specific application of Zr2Fe alloy.
Journal Article
Predictors and Treatments of Proglide-Related Complications in Percutaneous Endovascular Aortic Repair
2015
To investigate the predictors and treatment of the 6-Fr Perclose Proglide-related complications (PRC) in percutaneous endovascular aortic repair (pEVAR).
We retrospectively analyzed the PRC after pEVAR for the treatment of aortic aneurysm or dissection in our center from December 2012 to November 2013. Procedure success was defined as effective functioning of the two devices and local hemostasis. Access-related adverse events included vascular complications and device failures. Operative data and angiographic and computed tomography images were collected to assess the complications and treatment strategy.
A total of 198 patients with 275 puncture sites underwent pEVAR with the 6-Fr Perclose Proglide. The procedure was successful in 178 patients (89.9%), whereas PRC occurred in 20 cases (10.1%), including 10 device failures and 10 vascular complications. An extra manual ancillary compression was conducted in 7 patients, one more device was used in 8 patients, and surgical repair of the femoral artery was performed in 5 patients. PRC had a tendency to occur in patients with body mass index (BMI)>30 kg/m2 (p = 0.021), thoracic stent grafts (p = 0.038), common femoral artery (CFA) calcification (p = 0.001), CFA depth>4 cm (p = 0.001), and sheath size>20Fr (p = 0.005). Device failure-related mortality was zero. None of the access sites had complications during the midterm follow-up.
The pre-close technique with 6-Fr Perclose Proglide devices for pEVAR appears to be safe and effective with low technical failure and complication rates. Careful patient selection and proficiency in device manipulation might reduce the device related complications.
Journal Article