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result(s) for
"Wang, Liangbing"
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Atomic-level insights in optimizing reaction paths for hydroformylation reaction over Rh/CoO single-atom catalyst
2016
Rh-based heterogeneous catalysts generally have limited selectivity relative to their homogeneous counterparts in hydroformylation reactions despite of the convenience of catalyst separation in heterogeneous catalysis. Here, we develop CoO-supported Rh single-atom catalysts (Rh/CoO) with remarkable activity and selectivity towards propene hydroformylation. By increasing Rh mass loading, isolated Rh atoms switch to aggregated clusters of different atomicity. During the hydroformylation, Rh/CoO achieves the optimal selectivity of 94.4% for butyraldehyde and the highest turnover frequency number of 2,065 h
−1
among the obtained atomic-scale Rh-based catalysts. Mechanistic studies reveal that a structural reconstruction of Rh single atoms in Rh/CoO occurs during the catalytic process, facilitating the adsorption and activation of reactants. In kinetic view, linear products are determined as the dominating products by analysing reaction paths deriving from the two most stable co-adsorbed configurations. As a bridge of homogeneous and heterogeneous catalysis, single-atom catalysts can be potentially applied in other industrial reactions.
Despite the advantages of using heterogeneous catalysts, most successful rhodium hydrogenations are carried out with homogeneous catalysts. Here the authors report a supported single atom rhodium catalyst providing high activities and selectivities for propene hydroformylation.
Journal Article
Modulating oxygen coverage of Ti3C2Tx MXenes to boost catalytic activity for HCOOH dehydrogenation
2020
As a promising hydrogen carrier, formic acid (HCOOH) is renewable, safe and nontoxic. Although noble-metal-based catalysts have exhibited excellent activity in HCOOH dehydrogenation, developing non-noble-metal heterogeneous catalysts with high efficiency remains a great challenge. Here, we modulate oxygen coverage on the surface of Ti
3
C
2
T
x
MXenes to boost the catalytic activity toward HCOOH dehydrogenation. Impressively, Ti
3
C
2
T
x
MXenes after treating with air at 250 °C (Ti
3
C
2
T
x
-250) significantly increase the amount of surface oxygen atoms without the change of crystalline structure, exhibiting a mass activity of 365 mmol·g
−1
·h
−1
with 100% of selectivity for H
2
at 80 °C, which is 2.2 and 2.0 times that of commercial Pd/C and Pt/C, respectively. Further mechanistic studies demonstrate that HCOO* is the intermediate in HCOOH dehydrogenation over Ti
3
C
2
T
x
MXenes with different coverages of surface oxygen atoms. Increasing the oxygen coverage on the surface of Ti
3
C
2
T
x
MXenes not only promotes the conversion from HCOO* to CO
2
* by lowering the energy barrier, but also weakens the adsorption energy of CO
2
and H
2
, thus accelerating the dehydrogenation of HCOOH.
Developing non-noble-metal heterogeneous catalysts with high efficiency in HCOOH dehydrogenation is significant for the acquisition of hydrogen, but remains a great challenge. Here, the authors modulate oxygen coverage of Ti
3
C
2
T
x
MXenes to boost the catalytic activity toward HCOOH dehydrogenation.
Journal Article
Anchoring Pt Single Atoms on Te Nanowires for Plasmon‐Enhanced Dehydrogenation of Formic Acid at Room Temperature
2019
Formic acid (HCOOH), as a promising hydrogen carrier, is renewable, safe, and nontoxic. However, the catalytic dehydrogenation of HCOOH is typically conducted at elevated temperature. Here, HCOOH decomposition is successfully achieved for hydrogen production on the developed Pt single atoms modified Te nanowires with the Pt mass loading of 1.1% (1.1%Pt/Te) at room temperature via a plasmon‐enhanced catalytic process. Impressively, 1.1%Pt/Te delivers 100% selectivity for hydrogen and the highest turnover frequency number of 3070 h−1 at 25 °C, which is significantly higher than that of Pt single atoms and Pt nanoclusters coloaded Te nanowires, Pt nanocrystals decorated Te nanowires, and commercial Pt/C. A plasmonic hot‐electron driven mechanism rather than photothermal effect domains the enhancement of catalytic activity for 1.1%Pt/Te under light. The transformation of HCOO* to CO2δ −* on Pt atoms is proved to be the rate‐determining step by further mechanistic studies. 1.1%Pt/Te exhibits tremendous catalytic activity toward the decomposition of HCOOH owing to its plasmonic hot‐electron driven mechanism, which efficiently stimulates the rate‐determining step. In addition, hot electrons generated by the Te atoms nearby Pt single atoms are regarded to directly inject into the reactants adsorbed and activated on Pt single atoms. Pt single atoms modified Te nanowires with 1.1% Pt mass loading exhibit excellent catalytic activity and selectivity for hydrogen production from formic acid at room temperature via plasmonic catalysis. The HCOO*‐to‐CO2δ −* transformation on Pt single atoms is proved to be the rate‐determining step, which is efficiently stimulated by the plasmonic hot‐electron driven mechanism.
Journal Article
The Impacts of Enlarged Subarachnoid Space on Brain Growth and Cortex Maturation in Very Preterm Infants
2025
Objectives: The aim of this study is to investigate the changes in quantitative indices of brain volume and cortex development in preterm infants with enlarged subarachnoid space (ESS). Methods: A single-center retrospective cohort study was performed in Hong Kong University–Shenzhen Hospital from November 2014 to November 2023, involving 200 preterm infants whose brain MRI images were available. Parameters including the volume of cerebrospinal fluid (CSF), brain tissues, total intracranial cavity (ICC), and key indices of cortex maturation (surface area, cortical thickness, cortical volume, mean curvature) were compared between the groups with ESS and without ESS. The retrospective nature of this study may introduce selection bias in the process of enrolling preterm infants with ESS. Results: The groups with severe and mild ESS had a significantly greater ICC volume than the group without ESS (severe: 384.66 ± 30.33 [p < 0.001]; mild: 374.25 ± 26.45 [p < 0.001] vs. no ESS: 356.78 ± 26.03), and the difference was mostly due to the gap in extra-CSF volume among the three groups (severe: 74.20 ± 5.1 and mild: 55.36 ± 3.8 vs. no ESS: 40.54 ± 4.3, p ≤ 0.001). Only the volume of parenchyma of the severe-ESS group was significantly different (severe: 302.35 ± 26.43 vs. no ESS: 312.27 ± 20.75, p = 0.003). Regarding indices of cortex maturation, only the mean curvature showed a significant difference between the three groups, and most of the significant clusters were located around the parietal and temporal lobes. Conclusions: ESS may be associated with impaired early brain maturation in preterm infants after birth. A further neurodevelopmental follow-up study is needed.
Journal Article
Fetal Hyperthyroidism with Maternal Hypothyroidism: Two Cases of Intrauterine Therapy
by
Hong, Lu
,
Dai, Xiaoying
,
Cheung, Ka Wang
in
Cardiac arrhythmia
,
Case Report
,
Congenital diseases
2024
Fetal hyperthyroidism can occur secondary to maternal autoimmune hyperthyroidism. The thyroid-stimulating hormone receptor antibody (TRAb) transferred from the mother to the fetus stimulates the fetal thyroid and causes fetal thyrotoxicosis. Fetuses with this condition are difficult to detect, especially after maternal Graves disease therapy. Here, we present two cases of fetal hyperthyroidism with maternal hypothyroidism and review the assessment and intrauterine therapy for fetal hyperthyroidism. Both women were referred at 22+ and 23+ weeks of gestation with abnormal ultrasound findings, including fetal heart enlargement, pericardial effusion, and fetal tachycardia. Both women had a history of Graves disease while in a state of hypothyroidism with a high titer of TRAb. A sonographic examination showed a diffusely enlarged fetal thyroid with abundant blood flow. Invasive prenatal testing revealed no significant chromosomal aberration. Low fetal serum TSH and high TRAb levels were detected in the cord blood. Fetal hyperthyroidism was considered, and maternal oral methimazole (MMI) was administered as intrauterine therapy, with the slowing of fetal tachycardia, a reduction in fetal heart enlargement, and thyroid hyperemia. During therapy, maternal thyroid function was monitored, and the dosage of maternal levothyroxine was adjusted accordingly. Both women delivered spontaneously at 36+ weeks of gestation, and neonatal hyperthyroidism was confirmed in both newborns. After methimazole and propranolol drug treatment with levothyroxine for 8 and 12 months, both babies became euthyroid with normal growth and development.
Journal Article
Synergetic interaction between neighbouring platinum monomers in CO2 hydrogenation
2018
Exploring the interaction between two neighbouring monomers has great potential to significantly raise the performance and deepen the mechanistic understanding of heterogeneous catalysis. Herein, we demonstrate that the synergetic interaction between neighbouring Pt monomers on MoS2 greatly enhanced the CO2 hydrogenation catalytic activity and reduced the activation energy relative to isolated monomers. Neighbouring Pt monomers were achieved by increasing the Pt mass loading up to 7.5% while maintaining the atomic dispersion of Pt. Mechanistic studies reveal that neighbouring Pt monomers not only worked in synergy to vary the reaction barrier, but also underwent distinct reaction paths compared with isolated monomers. Isolated Pt monomers favour the conversion of CO2 into methanol without the formation of formic acid, whereas CO2 is hydrogenated stepwise into formic acid and methanol for neighbouring Pt monomers. The discovery of the synergetic interaction between neighbouring monomers may create a new path for manipulating catalytic properties.
Journal Article
Rhodium and Rhodium-Alloy Films and Nanoparticles: Part I
2024
Noble metals are key to various research fields and noble metal nanomaterials are directly relevant to optics, catalysis, medicine, sensing and many other applications. Rhodium-based nanomaterials have been less studied than metals such as gold, silver or platinum. There have been many improvements in characterisation tools over the years and knowledge about rhodium chemistry and nanomaterials is growing rapidly. Rhodium nanoparticles are widely used as catalysts for automotive emissions control and for hydrogen and oxygen precipitation reactions in electrolytic cells. Novel applications in electronics, anticancer drugs and aerospace are being revisited. In Part I of this two-part review, we cover different strategies for the synthesis of rhodium films and nanoparticles.
Journal Article
Rhodium and Rhodium-Alloy Films and Nanoparticles: Part II
2023
Part I of this review covered the synthesis methods for synthesis of rhodium films and nanoparticles (1). In Part II, we review the literature on the current and potential applications of rhodium and rhodium alloy films and nanoparticles in catalysis, components for the glass, chemical and electronic industries, thermal sensors and anticancer drugs.
Journal Article
Rhodium and Rhodium-Alloy Films and Nanoparticles: Part II
2024
Part I of this review covered the synthesis methods for synthesis of rhodium films and nanoparticles (). In Part II, we review the literature on the current and potential applications of rhodium and rhodium alloy films and nanoparticles in catalysis, components for the glass, chemical and electronic industries, thermal sensors and anticancer drugs.
Journal Article
Rhodium and Rhodium-Alloy Films and Nanoparticles: Part I
by
Zhou, Yicheng
,
Wang, Qinqin
,
Wang, Liangbing
in
Catalysis
,
Chemical elements
,
Chemical precipitation
2024
Noble metals are key to various research fields and noble metal nanomaterials are directly relevant to optics, catalysis, medicine, sensing and many other applications. Rhodium-based nanomaterials have been less studied than metals such as gold, silver or platinum. There have been many improvements in characterisation tools over the years and knowledge about rhodium chemistry and nanomaterials is growing rapidly. Rhodium nanoparticles are widely used as catalysts for automotive emissions control and for hydrogen and oxygen precipitation reactions in electrolytic cells. Novel applications in electronics, anticancer drugs and aerospace are being revisited. In Part I of this two-part review, we cover different strategies for the synthesis of rhodium films and nanoparticles.
Journal Article