Solid-state color centers with manipulatable spin qubits and telecom-ranged fluorescence are ideal platforms for quantum communications and distributed quantum computations. In this work, we ...coherently control the nitrogen-vacancy (NV) center spins in silicon carbide at room temperature, in which telecom-wavelength emission is detected. We increase the NV concentration sixfold through optimization of implantation conditions. Hence, coherent control of NV center spins is achieved at room temperature, and the coherence time T2 can be reached to around 17.1 μs. Furthermore, an investigation of fluorescence properties of single NV centers shows that they are room-temperature photostable single-photon sources at telecom range. Taking advantage of technologically mature materials, the experiment demonstrates that the NV centers in silicon carbide are promising platforms for large-scale integrated quantum photonics and long-distance quantum networks.
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CMK, CTK, FMFMET, IJS, NUK, PNG, UL, UM
Many in vitro studies have shown that tea catechins had vevarious health beneficial effects. However, inconsistent results between in vitro and in vivo studies or between laboratory tests and ...epidemical studies are observed. Low bioavailability of tea catechins was an important factor leading to these inconsistencies. Research advances in bioavailability studies involving absorption and metabolic biotransformation of tea catechins were reviewed in the present paper. Related techniques for improving their bioavailability such as nanostructure-based drug delivery system, molecular modification, and co-administration of catechins with other bioactives were also discussed.
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IZUM, KILJ, NUK, PILJ, PNG, SAZU, UL, UM, UPUK
Photocatalysts based on g-C3N4 by loading cocatalysts or constructing heterojunctions have shown great potential in solar-driven water oxidation. However, the intrinsic drawbacks of g-C3N4, such as ...poor mass diffusion and charge separation efficiency, remain as the bottleneck to achieve highly efficient water oxidation. Here we report a simple protonation method to improve the activity of g-C3N4. Studies using valence band X-ray photoelectron spectra and steady-state and time-resolved spectroscopy reveal that the promotion of catalytic ability originates from the higher thermodynamical driving force and longer-lived charge separation state, which may provide guidance in designing efficient polymeric semiconductor photocatalysts with desirable kinetics for water oxidation.
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IJS, KILJ, NUK, PNG, UL, UM
Semiconducting quantum dots (QDs) have recently triggered a huge interest in constructing efficient hydrogen production systems. It is well established that a large fraction of surface atoms of QDs ...need ligands to stabilize and avoid them from aggregating. However, the influence of the surface property of QDs on photocatalysis is rather elusive. Here, the surface regulation of CdSe QDs is investigated by surface sulfide ions (S2−) for photocatalytic hydrogen evolution. Structural and spectroscopic study shows that with gradual addition of S2−, S2− first grows into the lattice and later works as ligands on the surface of CdSe QDs. In‐depth transient spectroscopy reveals that the initial lattice S2− accelerates electron transfer from QDs to cocatalyst, and the following ligand S2− mainly facilitates hole transfer from QDs to the sacrificial agent. As a result, a turnover frequency (TOF) of 7950 h−1 can be achieved by the S2− modified CdSe QDs, fourfold higher than that of original mercaptopropionic acid (MPA) capped CdSe QDs. Clearly, the simple surface S2− modification of QDs greatly increases the photocatalytic efficiency, which provides subtle methods to design new QD material for advanced photocatalysis.
To unravel how surface sulfide ions (S2−)regulate photocatalytic hydrogen evolution of CdSe quantum dots (QDs), the different roles of introduced S2− on QDs are revealed. The results show that S2− at an earlier stage grows into the lattice and accelerates electron transfer, while afterward the S2− works as ligands and promotes hole transfer, and thus greatly improves the photocatalytic hydrogen evolution efficiency.
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BFBNIB, FZAB, GIS, IJS, KILJ, NLZOH, NUK, OILJ, SBCE, SBMB, UL, UM, UPUK
Liver transplantation is the ultimate method for treating end-stage liver disease. With the increasing prevalence of obesity, the number of patients with non-alcoholic fatty liver, a common cause of ...chronic liver disease, is on the rise and may become the main cause of liver transplantation in the future. With the increasing gap between the number of donor livers and patients waiting for liver transplantation and the increasing prevalence of non-alcoholic fatty liver, the proportion of steatosis livers among non-standard donor organs is also increasing. Ischemia-reperfusion injury has historically been the focus of attention in the liver transplantation process, and severe ischemia-reperfusion injury leads to adverse outcomes of liver transplantation. Studies have shown that the production of reactive oxygen species and subsequent oxidative stress play a key role in the pathogenesis of hepatic ischemia and reperfusion injury and non-alcoholic fatty liver. Furthermore, the sensitivity of fatty liver transplantation to ischemia-reperfusion injury has been suggested to be related to the production of reactive oxygen species (ROS) and oxidative stress. In ischemia-reperfusion injury, Kupffer cell and macrophage activation along with mitochondrial damage and the xanthine/xanthine oxidase system promote marked reactive oxygen species production and the inflammatory response and apoptosis, resulting in liver tissue injury. The increased levels of ROS and lipid peroxidation products, vicious circle of ROS and oxidative stress along with mitochondrial dysfunction promoted the progress of non-alcoholic fatty liver. In contrast to the non-fatty liver, a non-alcoholic fatty liver produces more reactive oxygen species and suffers more serious oxidative stress when subjected to ischemia-reperfusion injury. We herein review the effects of reactive oxygen species on ischemia-reperfusion injury and non-alcoholic fatty liver injury as well as highlight several treatment approaches.
A three-component protocol involving enantiopure Δ-Ir(ppy)2(MeCN)2(PF6) (ppy is 2-phenylpyridine) and salicylaldehyde as chiral auxiliaries was successfully applied to discriminate the absolute ...configuration and determine the enantiopurity of primary amines and amine alcohols via 1H NMR spectroscopy. The assembly reaction is rapid and quantitative, generating a pair of diastereomers that can be determined directly without physical separation. Single crystal structural analyses indicate that the shielding effects on the ligands imposed by a pair of diastereomers are different and generate sufficient resolution NMR signals for identification. The enhancement of stability via chelating coordination to Ir(III) ion and more than one pair of diastereotopic resonances in different detection regions of the three-component protocol ensure a high degree of accuracy in quantifying the ee value of chiral amines. The absolute errors in the ee determinations by 1H NMR spectroscopy in different detection windows are within 2.0%. The linear relationship between the experimentally measured ee values and the gravimetrically prepared samples is found to be excellent. This finding would provide a complementary method for the discrimination and determination of the enantiopurity of chiral primary amines and amine alcohols in the screening of asymmetric reactions.
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IJS, KILJ, NUK, PNG, UL, UM
Necroptosis is a necrotic programmed cell death with potent immunogenicity. Due to the dual effects of necroptosis on tumor growth, metastasis and immunosuppression, we evaluated the prognostic value ...of necroptosis-related genes (NRGs) in hepatocellular carcinoma (HCC).
We first analyzed RNA sequencing and clinical HCC patient data obtained to develop an NRG prognostic signature based on the TCGA dataset. Differentially expressed NRGs were further evaluated by GO and KEGG pathway analyses. Next, we conducted univariate and multivariate Cox regression analyses to build a prognostic model. We also used the dataset obtained from the International Cancer Genome Consortium (ICGC) database to verify the signature. The Tumor Immune Dysfunction and Exclusion (TIDE) algorithm was used to investigate the immunotherapy response. Furthermore, we investigated the relationship between the prediction signature and chemotherapy treatment response in HCC.
We first identified 36 differentially expressed genes out of 159 NRGs in hepatocellular carcinoma. Enrichment analysis showed that they were mainly enriched in the necroptosis pathway. Four NRGs were screened by Cox regression analysis to establish a prognostic model. The survival analysis revealed that the overall survival of patients with high-risk scores was significantly shorter than that of patients with low-risk scores. The nomogram demonstrated satisfactory discrimination and calibration. The calibration curves validated a fine concordance between the nomogram prediction and actual observation. The efficacy of the necroptosis-related signature was also validated by an independent dataset and immunohistochemistry experiments. TIDE analysis revealed that patients in the high-risk group were possibly more susceptible to immunotherapy. Furthermore, high-risk patients were found to be more sensitive to conventional chemotherapeutic medicines such as bleomycin, bortezomib, and imatinib.
We identified 4 necroptosis-related genes and established a prognostic risk model that could potentially predict prognosis and response to chemotherapy and immunotherapy in HCC patients in the future.
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DOBA, IZUM, KILJ, NUK, PILJ, PNG, SAZU, SIK, UILJ, UKNU, UL, UM, UPUK
With 2-phenylquinoline (pq) as a cyclometalated ligand, a series of cationic Ir(III) complexes Ir(pq)2(L1)2(PF6) (L1 is pyridine (1a), 4-methoxypyridine (1b), 4-dimethylaminopyridine (1c), and ...4-acetylpyridine (1d)) and Ir(pq)2(L2)(PF6) (L2 is 2,2′-bipyridine (1e), 2,2′-bipyrimidyl (1f), 4,4′-dimethyl-2,2′-bipyridine (1g), and 4,4′-dimethoxy-2,2′-bipyridine (1h)) were synthesized and characterized. The influence of the metal-based highest occupied molecular orbital on triplet-state lifetime, triplet-state quantum yield, and 1O2 generation quantum yield as well as aerobic photo-oxidation of sulfide into sulfoxide was evaluated via tuning the ancillary ligand of Ir(pq)2 complexes. The results revealed that 1h with chelate ancillary ligand bearing electron-donating group possesses a high 1O2 generation quantum yield (0.90) and photocatalytic activity for sulfide oxidation with high chemoselectivity and a low catalyst loading (0.5 mol %) under mild conditions. Moreover, one-pot two-step procedure for preparation of enantiopure sulfoxides, including aerobic photo-oxidation of sulfide using 1h as a photosensitizer and chiral resolution of sulfoxide via a chiral-at-metal strategy, was also developed.
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A diastereoselective photooxidation of α-amino acid (AA) complexes into imino acid complexes using a chiral iridium(III) complex as a photosensitizer and stereo-controller under visible light ...irradiation and oxygen was developed. It was found that the oxidative rate of Δ-Ir(pq)2(L-AA) (pq is 2-phenylquinoline) diastereomer is significantly higher than that of the corresponding Δ-Ir(pq)2(D-AA) diastereomer, providing a new protocol for kinetic resolution of AAs via a nonenzymatic pathway. Moreover, the thermodynamic controlled strategy offered a complemental method for the diastereoselective hydrogenation of imine bonds using NaBH4 as a reductant under the chiral Ir(III) complex as a stereo-controller. The combination of diastereoselective photooxidation and reduction processes results in a new protocol for deracemization of α-amino acids under mild conditions. Mechanism study strongly indicates that singlet oxygen is a key participant in the reaction and the α-C–H bond cleavage of AAs is the rate-determining step.
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IJS, KILJ, NUK, PNG, UL, UM
The tumor microenvironment (TME) is essential for immune escape by tumor cells. It plays essential roles in tumor development and metastasis. The clinical outcomes of tumors are often closely related ...to individual differences in the patient TME. Therefore, reprogramming TME cells and their intercellular communication is an attractive and promising strategy for cancer therapy. TME cells consist of immune and nonimmune cells. These cells need to be manipulated precisely and safely to improve cancer therapy. Furthermore, it is encouraging that this field has rapidly developed in recent years with the advent and development of gene editing technologies. In this review, we briefly introduce gene editing technologies and systematically summarize their applications in the TME for precision cancer therapy, including the reprogramming of TME cells and their intercellular communication. TME cell reprogramming can regulate cell differentiation, proliferation, and function. Moreover, reprogramming the intercellular communication of TME cells can optimize immune infiltration and the specific recognition of tumor cells by immune cells. Thus, gene editing will pave the way for further breakthroughs in precision cancer therapy.
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DOBA, IZUM, KILJ, NUK, PILJ, PNG, SAZU, SIK, UILJ, UKNU, UL, UM, UPUK
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