Nature Communications
·
2023
·Vol. 14
·期 1
·1-12
·
IF 16.6
Jung Sinyeong,Cheung Wai-Lung,Li Si-jie,Wang Min,Li Wansi,Wang Cangyu,Song Xiaoge,Wei Guodan,Song Qinghua,Chen Season Si,Cai Wanqing,Ng Maggie,Tang Wai Kit,Tang Man-Chung
The realization of operationally stable blue organic light-emitting diodes is a challenging issue across the field. While device optimization has been a focus to effectively prolong device lifetime, strategies based on molecular engineering of chemical structures, particularly at the subatomic level, remains little. Herein, we explore the effect of targeted deuteration on donor and/or acceptor units of thermally activated delayed fluorescence emitters and investigate the structure-property relationship between intrinsic molecular stability, based on isotopic effect, and device operational stability. We show that the deuteration of the acceptor unit is critical to enhance the photostability of thermally activated delayed fluorescence compounds and hence device lifetime in addition to that of the donor units, which is commonly neglected due to the limited availability and synthetic complexity of deuterated acceptors. Based on these isotopic analogues, we observe a gradual increase in the device operational stability and achieve the long-lifetime time to 90% of the initial luminance of 23.4 h at the luminance of 1000 cd m −2 for thermally activated delayed fluorescence-sensitized organic light-emitting diodes. We anticipate our strategic deuteration approach provides insights and demonstrates the importance on structural modification materials at a subatomic level towards prolonging the device operational stability.
研究领域:
材料科学
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化学工程
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光学工程
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产品关联
DOI
PubMed
高影响因子
ACS Applied Energy Materials
·
2021
·
IF 6.024
Juemin Yan,Nanlin He,Xiaojun Chen,Chengjian Xiao,LinJie Zhao,Tao Gao
A tetralithium titanium (Li4TiO4) compound is a tritium breeder material that deserves serious consideration for the fusion reactor blanket concept because of its high lithium density. In the current research, an experimental investigation was conducted for the first time to verify the calculated simulation results. First, the lattice parameters, energy band structures, and thermodynamic properties of Li4TiO4 are investigated by means of first-principles density functional theory. Then, the Li4TiO4 powder was synthesized via a solid-state reaction. Subsequently, the samples were systematically characterized using various measurement techniques. The products of the ultraviolet diffuse reflection spectrum, Raman spectroscopy, and laser thermal conductivity are consistent with the theoretical calculations.
研究领域:
材料科学
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核能工程
✓ 已验证
DOI
高影响因子
JOURNAL OF NUCLEAR MATERIALS
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2020
·
IF 2.485
Meifang Liu,Yueqing Zheng,Qiang Chen,Yuguang Wang,Yiyang Liu,Jing Li,Jie Li,Yawen Huang,Qiang Yin
Deuterated polymer beads with specifications on their size and structure are needed for preparing the targets in the inertial confined fusion experiments. Driven by the need to fabricate these beads meeting physical design, the coflow microfluidic device composed of glass round capillaries were fabricated. The formation mechanism of the droplets of the polymer solution (O droplets), the vacuole formation in the polymer beads and the size relationship between the O droplets and the resulting polymer beads were also investigated. The diameter of the O droplets can be controlled by designing microfluidic device with appropriate capillaries and tuning the flow rate of the polymer solution and aqueous solution. Residual solvent in polymer beads was reduced by optimizing the solidifying and drying process, leading to the decrease of the vacuoles. The size relationship between the initial O droplets and the resulting beads was revealed and confirmed. Consequently, monodisperse polymer beads such as ∼480 μm and ∼700 μm poly (α-methylstyrene), ∼700 μm polystyrene and ∼800 μm deuterated polystyrene beads meeting physical design were successfully prepared, which can be used to prepare the target in the inertial confined fusion experiments. It demonstrated the technical feasibility of controlling the bead size, providing a promising approach to fabricate the polymer beads meeting size requirement.
研究领域:
材料科学
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核物理
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化学工程
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产品关联
DOI
高影响因子
JOURNAL OF LABELLED COMPOUNDS & RADIOPHARMACEUTICALS
·
2018
·Vol. 61
·期 14
·1043-1047
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IF 1.423
Wulian Chen,Chaomin Zhao,Xiaojun Deng
An efficient and simple synthetic route of deuterium-labeled 2-quinoxalinecarboxylic acid- d 4 (QCA- d 4 ) and 3-methylquinoxaline-2-carboxylic acid- d 4 (MQCA- d 4 ) is presented with 99.9% and 99.6% isotopic enrichment using aniline- d 5 as labeled starting material. Their chemical structures were confirmed by 1 H NMR, and their isotopic abundance was determined by mass spectrometry analysis.
研究领域:
有机化学
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药物化学
✓ 已验证
DOI
高影响因子
Advanced Optical Materials
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2024
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IF 8
Cangyu Wang,Xiaoge Song,Wansi Li,Xiongkai Tang,Maggie Ng,Season Si Chen,Wai Kit Tang,Wen-Cheng Chen,Yanping Huo,Man-Chung Tang
Multiple-resonance thermally activated delayed fluorescence (MR-TADF) emitters have garnered significant attention in recent years due to their remarkable properties, such as high luminescent quantum yield, robustness, and their compliance with the Broadcast Television 2020 standard for the new generation of ultrahigh-definition. Despite these advancements, the operational lifetimes of organic light-emitting diodes (OLEDs) relying on MR-TADF emitters still fall short for practical application. It is believed that the enhancement of the intrinsic molecular stability of t Bu-DABNA , a fundamental backbone of MR-TADF emitters, holds great promise to be a universal strategy for all MR-TADF emitters improving the operational lifetimes of OLEDs. Herein, the design and synthesis of targeted deuteration are reported on donor and/or backbone of MR-TADF emitters, where the structure-property relationship between intrinsic molecular stability upon isotopic effect and device operational stability are examined. The isotopic analogs show a gradual increase in the device operational stability and achieve long-lifetime LT 80 (80% of the initial luminance of 1000 cd m −2 ) of 24.3 h for TADF-sensitized fluorescence OLED, representing a sevenfold enhancement when compared with the undeuterated counterpart. This strategic deuteration approach underlines the importance of structural modification on materials toward device operational stability.
研究领域:
材料科学
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光学工程
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2020
·Vol. 9
·期 7
·3985-3994
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IF 11.301
Ruidi Wang,Bei-Bei Xu,Jiachen Wang,Xue Lu Wang,Ye-Feng Yao
The relationship between the structural characteristics and photocatalytic reaction mechanisms of graphitic carbon nitride (g-C3N4) still remains unclarified at the molecular level, which severely hinders the further development of this field. The present study addresses this issue by employing an innovative strategy to investigate the relationship between the H-containing structures of g-C3N4 and its water splitting properties. The exchangeable and unexchangeable protons of the H-containing groups of g-C3N4 were differentiated by selective deuteration, providing a way to distinguish the hydrophilic and relatively non-hydrophilic H-containing groups of g-C3N4. A combination of advanced solid-state NMR approaches reveals that amino group defects (CN2(NHx)) on the C–N skeleton of the photocatalyst likely serve as hydrophilic active sites for facilitating the photocatalytic hydrogen evolution reaction. Accordingly, the newly synthesized g-C3N4 sample having a high concentration of CN2(NHx) by design demonstrates an enhanced H2 yield by a factor of 17 compared to that of pure g-C3N4.
研究领域:
材料化学
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光催化
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固体核磁共振
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表面科学
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能源材料
✓ 已验证
DOI
高影响因子
Matter and Radiation at Extremes
·
2021
·Vol. 6
·期 2
·
IF 2.845
Liu Meifang,Ai Xing,Liu Yiyang,Chen Qiang,Zhang Shuai,He Zhibing,Huang Yawen,Yin Qiang
Deuterated polymer microspheres can be used as a neutron source in conjunction with lasers because thermonuclear fusion neutrons can be produced efficiently by collisions of the resulting energetic deuterium ions. A new type of solid deuterated polymer microsphere with a carbon hydrogen–carbon deuterium (CH-CD) multilayer has been designed for preparing the target for inertial confinement fusion (ICF) experiments. To fabricate these solid CH-CD multilayer microspheres, CH beads are first fabricated by a microfluidic technique, and the CD coating layer is prepared by a plasma polymerization method. Both polystyrene (PS) and poly( α -methylstyrene) (PAMS) are used as the material sources for the CH beads. The effects of the PS and PAMS materials on the quality of the solid CH beads and the resulting CH-CD multilayer polymer microspheres are investigated. The solid PS beads have better sphericity and a smoother surface, but large vacuoles are observed in solid PS-CD multilayer microspheres owing to the presence of residual fluorobenzene in the beads and a glass transition temperature of the solid PS beads that is lower than the temperature of plasma polymerization. Therefore, solid PAMS beads are more suitable as a mandrel for fabricating solid CH-CD multilayer polymer microspheres. Solid CH-CD multilayer microspheres with specified size have been successfully prepared by controlling the droplet size and the CD deposition rate and deposition time. Compared with the design value, the diameter deviation of the inner CH beads and the thickness deviation of the CD layer can be controlled within 20 µ m and 2 µ m, respectively. Thus, an approach has been developed to fabricate solid CH-CD multilayer microspheres that meet the physical design requirements for ICF.
研究领域:
材料科学
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核物理
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Shubin Cheng,Qian Lei,Coner Deng,Weixin Lei,Honglin Chen
A green protocol for refining industrial chemicals containing formaldehyde (FA) impurities is presented here for the first time. FA, as an unreactant or a byproduct, causes separation problems in many industrial processes. It can be removed to a level of less than 1 ppm with easily separable methanol formation using commercial Cu/ZnO/Al 2 O 3 catalyst at atmospheric pressure in the absence of external hydrogen. The formation of methanol is achieved by the transfer of hydrogen species generated with the assistance of water to free FA, affording high methanol selectivity (62 %). By investigating potential intermediates and implementing deuterium labeling experiments, together with carbon and hydrogen balance calculations, a plausible pathway of water-assisted FA removal is proposed. Moreover, the in situ generated hydrogen species can be transferred directly into unsaturated compounds for selective reduction.
研究领域:
化学工程
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催化
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环境化学
✓ 已验证
产品关联
DOI
高影响因子
ENERGY & FUELS
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2024
·
IF 5.2
Zhong Chen,Qiao Chen,Dongyuan Li,Yi Zhong,Hongzhen Chen,Wei Peng
Conversion of heavy oil is urgent as most of the explored fossil oil reserves and renewable raw biodiesel can be categorized as heavy oil. Supercritical water upgrading (SCWU) is a green and promising technology for heavy oil conversion, but the hydrogen-donating capacity of pure water is inadequate. This study adopts transition-metal hydroxide (M–OH) to enhance the in situ hydrogen-donating capacity of water for the first time. Both M–OH and the corresponding metal oxide nanoparticle (MOn) of one post-transition metal (Al) and five transition metals (Cr, Cu, Fe, Ni, Zn) are tested. The SCWU conditions are selected as 425 °C, 60 min, water-to-oil ratio of 4:1, catalyst-to-oil ratio of 1:10, and water density of 308 kg m–3. Deuterium oxide (D2O) instead of H2O is used as the reaction medium for a deuterium tracing study. Results indicate that the different metal-based MOn nanoparticles display various effects on heavy hydrocarbon cracking, gasification, coke suppression, and D addition reactions. The overall performance is found to be on the order of NiO > Cr2O3 > Fe2O3 > CuO > Al2O3 > ZnO. Compared to MOn, M–OH can generally improve the oil yield and H/C ratio and reduce the coke yield simultaneously. The mechanism analysis suggests that the M–OH decomposition behavior under hydrothermal conditions is the primary cause by which MOn and lattice H2O are generated in the oil-rich phase. The lattice H2O can not only take part in SCWU reactions but also suppress coke formation. In conclusion, M–OH is a promising catalyst as it combines the good dispersibility and catalytic activity of MOn nanoparticles and the low cost of water-soluble inorganic metal salts (M-IAc) but does not result in any corrosive species, such as inorganic acid from M-IAc.
研究领域:
化学工程
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能源技术
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环境科学
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材料科学
✓ 已验证
DOI
高影响因子
Energy Storage Materials
·
2023
·
IF 20.4
Zhewen Ma,Zhongyuan Huang,Zhao Li,Guojie Chen,Yinghui Li,Wen Zhu,Wenguang Zhao,Haocheng Ji,Hui Fang,Wen Wen,Wen Yin,Jianxin Zou,Yinguo Xiao
In this study, ultrafine Mg(In) solid-solution particles were successfully prepared through an arc plasma method and their deuterium uptake/release performances were systematically estimated with respect to the identically processed pure Mg particles. Thermodynamic destabilization and kinetic enhancement of Mg-In-D system were achieved simultaneously with lower deuterium ab/desorption enthalpies and decreased desorption temperatures. For the first time, an in-situ synchrotron X-ray diffraction (ISXRD) coupled with neutron powder diffraction (NPD) technique and density functional theory (DFT) calculations clearly substantiated that an indium diffusion-dominated phase transition is the driving force for the evolution from mixture of MgD 2 and Mg-In intermetallic to Mg-based solid solution during the deuterium release (DR). The ISXRD results clarified the real-time phase transition from MgIn to Mg 3 In at 515 K and the interreaction of MgD 2 and Mg 3 In at 640 K, by which the matrix could be destabilized to trigger an indium-diffusion governed DR reaction in deuteride. Moreover, with the aid of NPD experiment, the microstructure evolution of Mg-In-D system demonstrated the continuous diffusion of indium into Mg/MgD 2 upon desorption. The solubilized indium in MgD 2 effectively reduced the D -migration energy barrier and stabilized the lattice structure to restrain the constriction of Mg-D bonds, through which the noticeable improvement on both thermodynamic and kinetic performances of the Mg-In system was achieved. The combination of synchrotron X-ray and neutron diffraction offers a high-efficiency strategy to fathom the hydrogen discharging mechanism from the viewpoint of real-time phase transitions and crystalline structure evolutions.
研究领域:
材料科学
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物理化学
✓ 已验证
DOI
高影响因子
NUCLEIC ACIDS RESEARCH
·
2022
·Vol. 50
·期 10
·5850-5863
·
IF 19.16
Lei Yixuan,Fei Panyu,Song Bin,Shi Wenjia,Luo Cheng,Luo Dahai,Li Dan,Chen Wei,Zheng Jie
DDX58 encodes RIG-I, a cytosolic RNA sensor that ensures immune surveillance of nonself RNAs. Individuals with RIG-IE510V and RIG-IQ517H mutations have increased susceptibility to Singleton-Merten syndrome (SMS) defects, resulting in tissue-specific (mild) and classic (severe) phenotypes. The coupling between RNA recognition and conformational changes is central to RIG-I RNA proofreading, but the molecular determinants leading to dissociated disease phenotypes remain unknown. Herein, we employed hydrogen/deuterium exchange mass spectrometry (HDX-MS) and single molecule magnetic tweezers (MT) to precisely examine how subtle conformational changes in the helicase insertion domain (HEL2i) promote impaired ATPase and erroneous RNA proofreading activities. We showed that the mutations cause a loosened latch-gate engagement in apo RIG-I, which in turn gradually dampens its self RNA (Cap2 moiety:m7G cap and N1-2-2′-O-methylation RNA) proofreading ability, leading to increased immunopathy. These results reveal HEL2i as a unique checkpoint directing two specialized functions, i.e. stabilizing the CARD2-HEL2i interface and gating the helicase from incoming self RNAs; thus, these findings add new insights into the role of HEL2i in the control of antiviral innate immunity and autoimmunity diseases.
研究领域:
免疫学
·
分子生物学
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遗传学
·
生物化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Crystals
·
2020
·Vol. 10
·期 6
·511
·
IF 2.404
Xueni Liu,Yan Ren,Cheng Qian Zhang,Bo Wang,Sheng Qing Xia
Single-crystalline fibers have distinct structures and optical properties comparing with the bulk crystals. In this article, two types of single-crystalline fibers of deuterated potassium dihydrogen phosphate (K(H1−xDx)2PO4,DKDP) are obtained by rapid growth in room-temperature supersaturated solution. X-ray diffraction analysis reveals that these DKDP single-crystalline fibers belong to tetragonal (I-42d) and monoclinic (P21/c) phases, respectively. The crystal structure of the tetragonal DKDP single-crystalline fiber is identical to that of the bulk DKDP tetragonal crystal reported. The lattice parameters of the monoclinic DKDP fiber (with the deuterium content of 55%) are a = 14.6571 Å, b = 4.5187 Å, c = 18.6962 Å, and β = 108.030°, which is a new crystal phase of DKDP. The monoclinic DKDP single-crystalline fiber is metastable at the present experimental condition and readily transit to the corresponding DKDP tetragonal phase in solution and in solid by grinding. The optical experiment shows that the highly deuterated tetragonal DKDP single-crystalline fiber possesses excellent optical guided-wave and effective second-harmonic generation properties. DKDP single-crystalline fibers are expected to be the suitable candidates for fabrication of the miniaturized nonlinear optical devices.
研究领域:
材料科学
·
光学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）