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result(s) for
"Yan, Qixin"
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High Fe-Loading Single-Atom Catalyst Boosts ROS Production by Density Effect for Efficient Antibacterial Therapy
by
Yan, Qixin
,
Shi, Jianlin
,
Lu, Xiangyu
in
Antiinfectives and antibacterials
,
Atomic properties
,
Atomic structure
2025
Highlights
Fe single-atom catalysts (h
3
-FNCs) with high loading, high catalytic activity and high stability were synthesized via a method capable of increasing both the metal loading and mass-specific activity by exchanging zinc with iron.
The “density effect,” derived from the sufficiently high density of active sites, has been discovered for the first time, leading to a significant alteration in the intrinsic activity of single-atom metal sites.
The superior oxidase-like catalytic performance of h
3
-FNCs ensures highly effective bacterial eradication.
The current single-atom catalysts (SACs) for medicine still suffer from the limited active site density. Here, we develop a synthetic method capable of increasing both the metal loading and mass-specific activity of SACs by exchanging zinc with iron. The constructed iron SACs (h
3
-FNC) with a high metal loading of 6.27 wt% and an optimized adjacent Fe distance of ~ 4 Å exhibit excellent oxidase-like catalytic performance without significant activity decay after being stored for six months and promising antibacterial effects. Attractively, a “density effect” has been found at a high-enough metal doping amount, at which individual active sites become close enough to interact with each other and alter the electronic structure, resulting in significantly boosted intrinsic activity of single-atomic iron sites in h
3
-FNCs by 2.3 times compared to low- and medium-loading SACs. Consequently, the overall catalytic activity of h
3
-FNC is highly improved, with mass activity and metal mass-specific activity that are, respectively, 66 and 315 times higher than those of commercial Pt/C. In addition, h
3
-FNCs demonstrate efficiently enhanced capability in catalyzing oxygen reduction into superoxide anion (O
2
·
−
) and glutathione (GSH) depletion. Both in vitro and in vivo assays demonstrate the superior antibacterial efficacy of h
3
-FNCs in promoting wound healing. This work presents an intriguing activity-enhancement effect in catalysts and exhibits impressive therapeutic efficacy in combating bacterial infections.
Journal Article
CKB Promotes Mitochondrial ATP Production by Suppressing Permeability Transition Pore
by
Lin, Jianghua
,
Yan, Qixin
,
Shi, Yufeng
in
Adenosine Triphosphate - metabolism
,
aging
,
Animals
2024
Creatine kinases are essential for maintaining cellular energy balance by facilitating the reversible transfer of a phosphoryl group from ATP to creatine, however, their role in mitochondrial ATP production remains unknown. This study shows creatine kinases, including CKMT1A, CKMT1B, and CKB, are highly expressed in cells relying on the mitochondrial F1F0 ATP synthase for survival. Interestingly, silencing CKB, but not CKMT1A or CKMT1B, leads to a loss of sensitivity to the inhibition of F1F0 ATP synthase in these cells. Mechanistically, CKB promotes mitochondrial ATP but reduces glycolytic ATP production by suppressing mitochondrial calcium (mCa2+) levels, thereby preventing the activation of mitochondrial permeability transition pore (mPTP) and ensuring efficient mitochondrial ATP generation. Further, CKB achieves this regulation by suppressing mCa2+ levels through the inhibition of AKT activity. Notably, the CKB‐AKT signaling axis boosts mitochondrial ATP production in cancer cells growing in a mouse tumor model. Moreover, this study also uncovers a decline in CKB expression in peripheral blood mononuclear cells with aging, accompanied by an increase in AKT signaling in these cells. These findings thus shed light on a novel signaling pathway involving CKB that directly regulates mitochondrial ATP production, potentially playing a role in both pathological and physiological conditions. CKB is highly expressed and necessary for maintaining cell sensitivity to the blockage of F1F0 ATP synthase. CKB and phosphocreatine, suppress AKT activation. CKB‐AKT signaling inhibits mitochondrial calcium levels, which in turn inactivates the mPTP. CKB‐AKT signaling is involved in the mitochondrial energy metabolism of tumor progression. AKT activation resulting from declined CKB likely leads to dysregulated mitochondrial energy production in Aging.
Journal Article
BeautyREC: Robust, Efficient, and Content-preserving Makeup Transfer
2022
In this work, we propose a Robust, Efficient, and Component-specific makeup transfer method (abbreviated as BeautyREC). A unique departure from prior methods that leverage global attention, simply concatenate features, or implicitly manipulate features in latent space, we propose a component-specific correspondence to directly transfer the makeup style of a reference image to the corresponding components (e.g., skin, lips, eyes) of a source image, making elaborate and accurate local makeup transfer. As an auxiliary, the long-range visual dependencies of Transformer are introduced for effective global makeup transfer. Instead of the commonly used cycle structure that is complex and unstable, we employ a content consistency loss coupled with a content encoder to implement efficient single-path makeup transfer. The key insights of this study are modeling component-specific correspondence for local makeup transfer, capturing long-range dependencies for global makeup transfer, and enabling efficient makeup transfer via a single-path structure. We also contribute BeautyFace, a makeup transfer dataset to supplement existing datasets. This dataset contains 3,000 faces, covering more diverse makeup styles, face poses, and races. Each face has annotated parsing map. Extensive experiments demonstrate the effectiveness of our method against state-of-the-art methods. Besides, our method is appealing as it is with only 1M parameters, outperforming the state-of-the-art methods (BeautyGAN: 8.43M, PSGAN: 12.62M, SCGAN: 15.30M, CPM: 9.24M, SSAT: 10.48M).
Perylenetetracarboxylic acid nanosheets with internal electric fields and anisotropic charge migration for photocatalytic hydrogen evolution
Highly efficient hydrogen evolution reactions carried out via photocatalysis using solar light remain a formidable challenge. Herein, perylenetetracarboxylic acid nanosheets with a monolayer thickness of ~1.5 nm were synthesized and shown to be active hydrogen evolution photocatalysts with production rates of 118.9 mmol g
−1
h
−1
.
The carboxyl groups increased the intensity of the internal electric fields of perylenetetracarboxylic acid from the perylene center to the carboxyl border by 10.3 times to promote charge-carrier separation. The photogenerated electrons and holes migrated to the edge and plane, respectively, to weaken charge-carrier recombination. Moreover, the perylenetetracarboxylic acid reduction potential increases from −0.47 V to −1.13 V due to the decreased molecular conjugation and enhances the reduction ability. In addition, the carboxyl groups created hydrophilic sites. This work provides a strategy to engineer the molecular structures of future efficient photocatalysts.
While organic semiconductors provide a highly tailorable set of systems for solar-to-fuel conversion, such materials often show worse activities than inorganic materials. Here, authors prepare perylene-based nanosheets that demonstrate excellent performances for photocatalytic H
2
evolution.
Journal Article
Photocatalytic sacrificial H2 evolution dominated by micropore-confined exciton transfer in hydrogen-bonded organic frameworks
2023
Organic semiconductors are attractive photocatalysts, but their quantum yields are limited by the transfer of photogenerated charges to the surface. A promising strategy for low-loss charge transfer is to shorten the distance from the bulk exciton coupling region to the catalyst surface. Here we employ the hydrogen-bonded organic framework 1,3,6,8-tetrakis(
p
-benzoic acid)pyrene (HOF-H
4
TBAPy) with hydrophilic one-dimensional micropore channels as a proof of concept for this approach. Under irradiation, photogenerated excitons rapidly transfer to the inner surface of adjacent micropores, engendering a mere 1.88 nm transfer route, thus significantly improving exciton utilization. When the micropore channel length does not exceed 0.59 μm, the sacrificial photocatalytic H
2
evolution rate of HOF-H
4
TBAPy reaches 358 mmol h
−1
g
−1
and the apparent quantum yield at 420 nm is 28.6%. We further demonstrated a stable 1.03 mol day
−1
m
−2
H
2
evolution on a 0.5 m
2
HOF-H
4
TBAPy-loaded fibre under 1 Sun irradiation.
Organic semiconductors have potential for application as photocatalysts, but their efficiency is limited by recombination of charge carriers before they can reach the surface. Here hydrogen-bonded organic frameworks with designed micropores decrease the exciton transfer path to improve charge utilization in photocatalytic H
2
evolution.
Journal Article
Photogenerated outer electric field induced electrophoresis of organic nanocrystals for effective solid-solid photocatalysis
2024
Rapid mass transfer in solid-solid reactions is crucial for catalysis. Although phoretic nanoparticles offer potential for increased collision efficiency between solids, their implementation is hindered by limited interaction ranges. Here, we present a self-driven long-range electrophoresis of organic nanocrystals facilitated by a rationally designed photogenerated outer electric field (OEF) on their surface. Employing perylene-3,4,9,10-tetracarboxylic dianhydride (PTCDA) molecular nanocrystals as a model, we demonstrate that a directional OEF with an intensity of 13.6-0.4 kV m
−1
across a range of 25–200 μm. This OEF-driven targeted electrophoresis of PTCDA nanocrystals onto the microplastic surface enhances the activity for subsequent decomposition of microplastics (196.8 mg h
−1
) into CO
2
by solid-solid catalysis. As supported by operando characterizations and theoretical calculations, the OEF surrounds PTCDA nanocrystals initially, directing from the electron-rich (0 1 1) to the hole-rich
(
11
2
¯
)
surface. Upon surface charge modulation, the direction of OEF changes toward the solid substrate. The OEF-driven electrophoretic effect in organic nanocrystals with anisotropic charge enrichment characteristics indicates potential advancements in realizing effective solid-solid photocatalysis.
Charge accumulation in organic photocatalysts leads to an overlooked macroscopic particle migration, crucial for heterogeneous photocatalytic kinetics. Authors demonstrate self-driven electrophoresis of organic nanocrystals via rationally designed photogenerated outer electric field (OEF).
Journal Article
Analysis of double side ironless permanent magnet linear synchronous machine with low normal force
2025
An electromagnetic linear machine is an energy conversion device that can convert electrical energy into linear motion. Conventional study of electromagnetic linear machines mainly focuses on the axial thrust, because it can be used to act on external payloads directly. However, due to manufacturing error and mechanical deformation of mover, the double side permanent magnet linear synchronous machine (DPMLSM) often generates unbalanced normal force on mover. This unwanted force may aggravate the mover deformation and lead to unequal airgap, which increases the normal force further, consequently leading an increase of friction, vibration and noise of the system. Therefore, the normal force in also important that is ignored. The purpose of this article is to study the normal force of DPMLSM to provide theoretical support for the design. The normal force of DPMLSM is analysed systematically and the magnetic field distribution is formulated analytically. The normal force for different mover deformation and different number of Halbach segments are analysed. It is found that the offset of normal installation has a significant impact on the normal force, and the more segments there are, the smaller the normal force. The width of the pole is optimized and an experimental prototype is fabricated to verify the accuracy of analytical and numerical calculations through experiments.
Journal Article
Enhanced hydrogen peroxide photosynthesis via charge-complementary π-electron sites
Organic photocatalysts with porphyrin conjugated chromophore core are promising for artificial hydrogen peroxide (H
2
O
2
) photosynthesis, but the lack of bottom-up paradigm for oxygen (O
2
) adsorption sites hinders their activity. Here, we introduce imidazole groups as
π
-electron sites with charge-complementarity to the O
2
molecules, enhancing O
2
binding via sub-atomically mirrored electrostatic cooperative
π
-
π
dispersion forces. In situ spectroscopy and theory reveal that the ~2 Å linear δ
+
-δ
−
-δ
+
domain of the imidazole substituent exhibits 2.8-folds stronger O
2
adsorption than neutral
π
-electron substituents, accompanied by the generation of energetically peroxide intermediates. Consequently, imidazole-substituted porphyrin photocatalysts achieve a solar-to-chemical conversion efficiency of 1.85% using only H
2
O and O
2
. In scalable membranes with photocatalysts, enabling daily photosynthetic production of 80 L m
−2
of Fenton-applicable H
2
O
2
solution. This work offers a strategy to modulate the electrostatic distribution of oxygen photoreduction sites, providing insights into overcoming gas activation rate-limiting steps in photocatalytic processes.
Introducing imidazole groups into porphyrin structures creates charge-complementary π-electron sites for O
2
molecules which enhances binding force via electrostatic cooperative dispersion, thereby improving the efficiency of H
2
O
2
photosynthesis.
Journal Article
EDIL3 influenced the αvβ3‐FAK/MEK/ERK axis of endothelial cells in psoriasis
2022
One of the earliest events in the development of psoriatic lesion is a vascular network expansion. The abnormal vascular network is associated with increased endothelial cells (ECs) survival, proliferation, adhesion, migration, angiogenesis and permeability in psoriatic lesion. Our previous study demonstrated that epidermal growth factor‐like repeats and discoidin I‐like domains 3 (EDIL3) derived from psoriatic dermal mesenchymal stem cells (DMSCs) promoted cell–cell adhesion, migration and angiogenesis of ECs, but the molecular mechanism of upstream or downstream has not been explored. So, this study aimed to explore the association between EDIL3 derived from DMSCs (DMSCs‐derived EDIL3) and psoriasis‐associated angiogenesis. We injected recombinant EDIL3 protein to mouse model of psoriasis to confirm the roles of EDIL3 in psoriasis. Besides, we employed both short‐interference RNA (si‐RNA) and lentiviral vectors to explore the molecular mechanism of EDIL3 promoting angiogenesis in psoriasis. In vivo, this research found that after injected recombination EDIL3 protein, the epidermis thickness and microvessel density were both elevated. EDIL3 accelerated the process of psoriasis in the IMQ‐induced psoriasis‐like mouse model. Additionally, we confirmed that in vitro DMSCs‐derived EDIL3 is involved in the tube formation of ECs via αvβ3‐FAK/MEK/ERK signal pathway. This suggested that DMSCs‐derived EDIL3 and αvβ3‐FAK/MEK/ERK signal pathway in ECs play an important role in the pathogenesis of psoriasis. And the modification of DMSCs, EDIL3 and αvβ3‐FAK/MEK/ERK signal pathway will provide a valuable therapeutic target to control the angiogenesis in psoriasis.
Journal Article