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"Xu, Liang"
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Highly efficient eco-friendly X-ray scintillators based on an organic manganese halide
Scintillation based X-ray detection has received great attention for its application in a wide range of areas from security to healthcare. Here, we report highly efficient X-ray scintillators with state-of-the-art performance based on an organic metal halide, ethylenebis-triphenylphosphonium manganese (II) bromide ((C
38
H
34
P
2
)MnBr
4
), which can be prepared using a facile solution growth method at room temperature to form inch sized single crystals. This zero-dimensional organic metal halide hybrid exhibits green emission peaked at 517 nm with a photoluminescence quantum efficiency of ~ 95%. Its X-ray scintillation properties are characterized with an excellent linear response to X-ray dose rate, a high light yield of ~ 80,000 photon MeV
−1
, and a low detection limit of 72.8 nGy s
−1
. X-ray imaging tests show that scintillators based on (C
38
H
34
P
2
)MnBr
4
powders provide an excellent visualization tool for X-ray radiography, and high resolution flexible scintillators can be fabricated by blending (C
38
H
34
P
2
)MnBr
4
powders with polydimethylsiloxane.
Scintillation-based X-ray detection is promising for applications in various areas ranging from security to healthcare, and low-cost and eco-friendly scintillation materials would be beneficial. Here the authors report a facile solution growth of organic manganese halide for efficient X-ray scintillation.
Journal Article
In situ observation of thermal-driven degradation and safety concerns of lithiated graphite anode
Graphite, a robust host for reversible lithium storage, enabled the first commercially viable lithium-ion batteries. However, the thermal degradation pathway and the safety hazards of lithiated graphite remain elusive. Here, solid-electrolyte interphase (SEI) decomposition, lithium leaching, and gas release of the lithiated graphite anode during heating were examined by in situ synchrotron X-ray techniques and in situ mass spectroscopy. The source of flammable gas such as H
2
was identified and quantitively analyzed. Also, the existence of highly reactive residual lithium on the graphite surface was identified at high temperatures. Our results emphasized the critical role of the SEI in anode thermal stability and uncovered the potential safety hazards of the flammable gases and leached lithium. The anode thermal degradation mechanism revealed in the present work will stimulate more efforts in the rational design of anodes to enable safe energy storage.
The role of the lithiated graphite anode in battery thermal runaway failure remains under intense investigation. In this work, with multiple in situ synchrotron X-ray characterizations, the phase evolution, gas release, and lithium leaching of lithiated graphite anode are illustrated in detail.
Journal Article
Suppressing electrolyte-lithium metal reactivity via Li+-desolvation in uniform nano-porous separator
Lithium reactivity with electrolytes leads to their continuous consumption and dendrite growth, which constitute major obstacles to harnessing the tremendous energy of lithium-metal anode in a reversible manner. Considerable attention has been focused on inhibiting dendrite via interface and electrolyte engineering, while admitting electrolyte-lithium metal reactivity as a thermodynamic inevitability. Here, we report the effective suppression of such reactivity through a nano-porous separator. Calculation assisted by diversified characterizations reveals that the separator partially desolvates Li
+
in confinement created by its uniform nanopores, and deactivates solvents for electrochemical reduction before Li
0
-deposition occurs. The consequence of such deactivation is realizing dendrite-free lithium-metal electrode, which even retaining its metallic lustre after long-term cycling in both Li-symmetric cell and high-voltage Li-metal battery with LiNi
0.6
Mn
0.2
Co
0.2
O
2
as cathode. The discovery that a nano-structured separator alters both bulk and interfacial behaviors of electrolytes points us toward a new direction to harness lithium-metal as the most promising anode.
Lithium dendrite and parasitic reactions are two major challenges for lithium metal anode. Here, the authors show suppression of lithium-dendrite and elimination of continuous parasitic reactions by tuning the reduction kinetics of lithium-ion through a uniform nano-porous separator.
Journal Article
Reversal of nucleobase methylation by dioxygenases
The repertoire of nucleobase methylation in DNA and RNA, introduced by chemical agents or enzymes, is large. Most methylation can be reversed either directly by restoration of the original nucleobase or indirectly by replacement of the methylated nucleobase with an unmodified nucleobase. In many direct and indirect demethylation reactions, ALKBH (AlkB homolog) and TET (ten eleven translocation) hydroxylases play a role. Here, we suggest a chemical classification of methylation types. We then discuss pathways for removal, emphasizing oxidation reactions. We highlight the recently expanded repertoire of ALKBH- and TET-catalyzed reactions and describe the discovery of a TET-like protein that resembles the hydroxylases but uses an alternative co-factor and catalyzes glyceryl transfer rather than hydroxylation.
This Review summarizes the chemical and physical properties of methylated nucleobases in DNA and RNA, proposes a chemical classification of methylation types, and discusses recent advance in demethylation reactions mediated by dioxygenases.
Journal Article
Entropy and crystal-facet modulation of P2-type layered cathodes for long-lasting sodium-based batteries
P2-type sodium manganese-rich layered oxides are promising cathode candidates for sodium-based batteries because of their appealing cost-effective and capacity features. However, the structural distortion and cationic rearrangement induced by irreversible phase transition and anionic redox reaction at high cell voltage (i.e., >4.0 V) cause sluggish Na-ion kinetics and severe capacity decay. To circumvent these issues, here, we report a strategy to develop P2-type layered cathodes via configurational entropy and ion-diffusion structural tuning. In situ synchrotron X-ray diffraction combined with electrochemical kinetic tests and microstructural characterizations reveal that the entropy-tuned Na
0.62
Mn
0.67
Ni
0.23
Cu
0.05
Mg
0.07
Ti
0.01
O
2
(CuMgTi-571) cathode possesses more {010} active facet, improved structural and thermal stability and faster anionic redox kinetics compared to Na
0.62
Mn
0.67
Ni
0.37
O
2
. When tested in combination with a Na metal anode and a non-aqueous NaClO
4
-based electrolyte solution in coin cell configuration, the CuMgTi-571-based positive electrode enables an 87% capacity retention after 500 cycles at 120 mA g
−1
and about 75% capacity retention after 2000 cycles at 1.2 A g
−1
.
The use of Mn-rich layered cathodes in Na-based batteries is hindered by inadequate cycling reversibility and sluggish anionic redox kinetics. Here, the authors report a strategy to stabilize the structure and promote anionic redox via configurational entropy and ion-diffusion structural tuning.
Journal Article
Quantifying electron-transfer in liquid-solid contact electrification and the formation of electric double-layer
Contact electrification (CE) has been known for more than 2600 years but the nature of charge carriers and their transfer mechanisms still remain poorly understood, especially for the cases of liquid–solid CE. Here, we study the CE between liquids and solids and investigate the decay of CE charges on the solid surfaces after liquid–solid CE at different thermal conditions. The contribution of electron transfer is distinguished from that of ion transfer on the charged surfaces by using the theory of electron thermionic emission. Our study shows that there are both electron transfer and ion transfer in the liquid–solid CE. We reveal that solutes in the solution, pH value of the solution and the hydrophilicity of the solid affect the ratio of electron transfers to ion transfers. Further, we propose a two-step model of electron or/and ion transfer and demonstrate the formation of electric double-layer in liquid–solid CE.
The identity of charge carriers (electron or ion) in contact electrification has been discussed for many years. Here, the authors demonstrate that the electron transfer paly an important role in liquid-solid contact electrification and the formation mechanism of electric double-layer is proposed.
Journal Article
H19 activates Wnt signaling and promotes osteoblast differentiation by functioning as a competing endogenous RNA
Bone homeostasis is tightly orchestrated and maintained by the balance between osteoblasts and osteoclasts. Recent studies have greatly expanded our understanding of the molecular mechanisms of cellular differentiation. However, the functional roles of non-coding RNAs particularly lncRNAs in remodeling bone architecture remain elusive. In our study, lncRNA H19 was found to be upregulated during osteogenesis in hMSCs. Stable expression of H19 significantly accelerated
in vivo
and
in vitro
osteoblast differentiation. Meanwhile, by using bioinformatic investigations and RIP assays combined with luciferase reporter assays, we demonstrated that H19 functioned as an miRNA sponge for miR-141 and miR-22, both of which were negative regulators of osteogenesis and Wnt/β-catenin pathway. Further investigations revealed that H19 antagonized the functions of these two miRNAs and led to de-repression of their shared target gene β-catenin, which eventually activated Wnt/β-catenin pathway and hence potentiated osteogenesis. In addition, we also identified a novel regulatory feedback loop between H19 and its encoded miR-675-5p. And miR-675-5p was found to directly target H19 and counteracted osteoblast differentiation. To sum up, these observations indicate that the lncRNA H19 modulates Wnt/β-catenin pathway by acting as a competing endogenous RNA, which may shed light on the functional role of lncRNAs in coordinating osteogenesis.
Journal Article
Native lattice strain induced structural earthquake in sodium layered oxide cathodes
High-voltage operation is essential for the energy and power densities of battery cathode materials, but its stabilization remains a universal challenge. To date, the degradation origin has been mostly attributed to cycling-initiated structural deformation while the effect of native crystallographic defects induced during the sophisticated synthesis process has been significantly overlooked. Here, using in situ synchrotron X-ray probes and advanced transmission electron microscopy to probe the solid-state synthesis and charge/discharge process of sodium layered oxide cathodes, we reveal that quenching-induced native lattice strain plays an overwhelming role in the catastrophic capacity degradation of sodium layered cathodes, which runs counter to conventional perception—phase transition and cathode interfacial reactions. We observe that the spontaneous relaxation of native lattice strain is responsible for the structural earthquake (e.g., dislocation, stacking faults and fragmentation) of sodium layered cathodes during cycling, which is unexpectedly not regulated by the voltage window but is strongly coupled with charge/discharge temperature and rate. Our findings resolve the controversial understanding on the degradation origin of cathode materials and highlight the importance of eliminating intrinsic crystallographic defects to guarantee superior cycling stability at high voltages.
Native crystallographic defects are often introduced during synthesis of battery materials, but has been overlooked. Here, using in situ synchrotron X-ray probes and electron microscopy, the authors have revealed their adverse effect during battery operation.
Journal Article
Profiling of Phenolic Compounds and Antioxidant Activity of 12 Cruciferous Vegetables
The phenolic profiles of 12 cruciferous vegetables (pakchoi, choysum, Chinese cabbage, kailan, Brussels sprout, cabbage, cauliflower, broccoli, rocket salad, red cherry radish, daikon radish, and watercress) were studied with UHPLC-MS/MS. Antioxidant activity and total phenolic content (TPC) were also evaluated. A total of 74 phenolic compounds were identified, including 16 hydroxycinnamic acids and derivatives, and 58 flavonoids and derivatives. The main flavonoids identified were glycosylated quercetin, kaempferol and isorhamnetin, and the main hydroxycinnamic acids were ferulic, sinapic, caffeic and p-coumaric acids. Principal component analysis (PCA) revealed that the distribution of phenolic compounds in different genera of cruciferous vegetables was in accordance with their conventional taxonomy. The DPPH, ORAC and TPC values ranged from 1.11 to 9.54 µmoles Trolox equivalent/g FW, 5.34 to 32.92 µmoles Trolox equivalent/g FW, and 0.16 to 1.93 mg gallic acid equivalent/g FW respectively. Spearman’s correlation showed significant (p < 0.05) positive correlations between TPC, flavonoids and antioxidant activity.
Journal Article