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Journal of Physical Chemistry C · 2023 · IF 3.7

Inducing Ferroelectricity in NH4I and NH4Br via Partial Replacement of Protons by Deuterons

Miao Miao Zhao,Lei Meng,Yi Yang Xu,Na Du,Fei Yen

While all of the polymorphs of NH4I and NH4Br are nonpolar, a reversible electric polarization is established in the ordered γ phases of (NH4)0.73(ND4)0.27I and (NH4)0.84(ND4)0.16Br (where D is 2H) via dc electric fields. The presence of two groups of orbital magnetic moments appears to be responsible for the asymmetric lattice distortions. Our findings provide an alternative pathway for hydrogen-based materials to potentially add a ferroelectric functionality.

研究领域: 材料科学 · 物理学
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ORGANIC ELECTRONICS · 2024 · IF 2.7

Enhancing the operational stability of OLED devices through the utilization of deuterated TTU host materials

Cangyu Wang,Xiaoge Song,Sinyeong Jung,Wansi Li,Maggie Ng,Season Si Chen,Man-Chung Tang

Recent research on anthracene-based hydrocarbon (PNA) as the emissive layer host found that deuteration mediated the formation of these adduct species, presumably quenchers, and thus improved the device lifetime. Meanwhile, studies on deuterium in PNA host materials with stepwise deuteration are scarce. In this work, we report a systematic study of isotopic effects through independent deuteration of the phenyl or/and the dibenzofuran unit on a series of PNA materials polyaromatic dibenzofuran ( PAF , PAF- d 5 , PAF- d 7 and PAF- d 12 ). We fabricated fluorescent OLED based on this triplet-triplet up-conversion active host materials for conventional MR-TADF emitter. A short-lived excited delayed lifetime of less than 2 μs has been observed in their electroluminescence decay studies. In addition, LT 80 of up to 12.7 h has been observed in PAF- d 12 at the brightness of 1000 cd m −2 , corresponding to a 4-fold enhancement of OLED stability compared to the non-deuterated counterpart. We hope the current research can provide insights for further device improvement.

CAS / MDL: 89827-45-2 127-08-2
研究领域: 材料科学 · 有机电子学
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EUROPEAN JOURNAL OF ORGANIC CHEMISTRY · 2023 ·Vol. 26 ·期 20 ·e202300278 · IF 2.8

Gram-Scale Synthesis of Chain-Deuterated Sphingosine and Its Derivatization to Produce Ceramide, Sphinganine and Sphingosine-1-phosphate

Yonghang Mu,Zi Wang,Linhua Song,Kun Ma,Yao Chen,Peixun Li,Zifeng Yan

Graphical We report a gram-scale synthesis of sphingosines with different deuterated chains. The synthesis of highly stereoselective chain deuterated sphingosine was accomplished in five steps which started from hydrothermal platinum-catalyzed hydrogen/deuterium (H/D) exchange of protiated fatty acids. The subsequent synthesis of the deuterated-chain derivatives are also described. They were all characterized with deuterated content above 94 %. Sphingosine plays crucial roles in various cellular functions. Deuterated molecules are widely used as the important tools to explore the structure, property, and function of biochemical materials. We here report a gram-scale synthesis of sphingosines with different deuterated chains. The synthesis started from different protiated fatty acids, which underwent hydrothermal platinum-catalyzed hydrogen/deuterium (H/D) exchange to produce the deuterated chains with different length. The Horner–Wadsworth–Emmons (HWE) coupling of a chiral amino acid derivative with the deuterated chains generated the unsaturated ketone precursors. The following stereoselective reduction via cyclic Felkin–Anh transition led to the desired anti- amino alcohol geometry. This efficient protocol enabled the gram-scale synthesis of the chain-deuterated sphingosines. The subsequent synthesis of the chain-deuterated derivatives, i. e. ceramide, sphinganine and sphingosine-1-phosphate, is also described. Their deuterium content was simultaneously characterized by 1 H NMR and high-resolution mass spectrum (HRMS).

研究领域: 有机化学 · 生物化学 · 药学
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JOURNAL OF ORGANIC CHEMISTRY · 2023 · IF 3.6

Difluoromethylation–Carboxylation and −Deuteration of Alkenes Triggered by Electroreduction of Difluoromethyltriphenylphosphonium Bromide

Fenfen Xie,Fen Han,Yunying Yan,Haiqiong Li,Jianjun Hao,Linhai Jing,Pan Han

It is significant to develop novel difluoromethylation methods because of the important roles of difluoromethyl groups in the medicinal chemistry and material industries. Here, we developed a novel difluoromethylation–carboxylation and difluoromethylation–deuteration method triggered by a difluoromethyl radical generated by electroreduction of stable and easily available difluoromethyltriphenylphosphonium bromide. Various molecules containing difluoromethyl and carboxyl or deuterium groups can be synthesized through this method. The establishment of this method will provide an alternative to radical difluoromethylation reactions.

研究领域: 有机化学 · 药物化学
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Journal of Materials Chemistry C · 2023 ·Vol. 11 ·期 23 ·7611-7618 · IF 6.4

Valence state control of Cr4+-activated Li2SrGeO4 for NIR-II light source to distinguish deuterium and non-deuterium reagents

Xiaoxuan Guo,Bomei Liu,Rongyi Kuang,Weijiang Gan,Lin Huang,Jing Wang

Cr-activated phosphor-converted light sources have attracted widespread attention in various applications based on near-infrared (NIR) spectroscopy. Unfortunately, Cr ions usually face the issue of multivalence and typically exist in the valence of +3, which gives the emission mainly at NIR-I (700–1000 nm) and greatly limits its potential application. In this study, we propose the control strategies of site occupancy confinement and sintering atmosphere to synthesize Cr4+-activated Li2SrGeO4 (LSGO:Cr4+) phosphors. Interestingly, the as-optimized LSGO:Cr4+ achieves a NIR broadband emission peak at 1170 nm with an FWHM of 208 nm upon excitation at 680 nm and exhibits excellent thermal stability and high efficiency with the external quantum efficiency of 30.0%. Furthermore, the as-fabricated LSGO:Cr NIR phosphor-converted light emitting diode (NIR pc-LED) device shows a high power of up to 69.1 mW at 550 mA. Furthermore, as NIR-II (1000–1700 nm) light source, the phosphor successfully distinguishes deuterium and non-deuterium reagents. For example, the quantitative detection of H2O in heavy water (D2O) is demonstrated by NIR spectroscopy with a limit of detection (LOD) of 0.47 vol%. Our findings will open up a new avenue to develop novel Cr4+-activated NIR-II phosphors and NIR-II light sources.

研究领域: 材料科学 · 光学工程 · 分析化学
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Science Bulletin · 2020 · IF 9.511

Electrocatalytic water-splitting for the controllable and sustainable synthesis of deuterated chemicals

Bing Zhang,Chuntian Qiu,Shan Wang,Hua Gao,Kunyi Yu,Zhaofei Zhang,Xiang Ling,Wei Ou,Chenliang Su

Tandem water electrolysis for the transformation of universal feedstock to value-added chemicals integrated with hydrogen generation and in situ utilization is a promising approach to address the economic challenges of electrochemical hydrogen evolution and storage. Herein, we present the controllable electrocatalytic deuteration of halides using inexpensive and reusable heavy water (D 2 O) as a D-source for the preparation of valuable D-labelled chemicals and pharmaceuticals under mild conditions. This electrochemical deuteration method with high efficiency and selectivity furnishes a series of D-labelled chemicals and pharmaceuticals in high yields with excellent D-incorporation. The reaction efficiency and selectivity, that is, the precise substitution of deuterium atoms at different halogen positions, can be tuned by varying the applied voltages . The results show the great potential of green and economical electrocatalytic methods for producing value-added fine chemicals in addition to hydrogen evolution.

研究领域: 化学工程 · 电化学
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JOURNAL OF ORGANIC CHEMISTRY · 2023 · IF 3.6

Pd-Catalyzed Regioselective Deuteration of Indole’s C4-Position with Transient Directing Groups

Chenxu Zheng,Zhi-Jiang Jiang,Ke Jin,Qian Wang,Jian-Fei Bai,Gang Xu,Zhanghua Gao

As a representative scaffold of alkaloids, indoles have been extensively subjected to deuteration, but the regioselective C4 labeling has not been achieved due to its low reactivity. In this work, a Pd-catalyzed deuterium labeling at the indole’s C4 position has been developed under the strategy of transient directing, using D2O as a deuterium source. The substituent effect is found to be crucial in facilitating this H/D exchange process, where the reversing C–D bond formation favors an electron-enriched ligation contrary to its C–H halogenation counterpart.

研究领域: 有机化学 · 药物化学
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Advanced Science · 2024 ·Vol. 11 ·期 29 ·2308523 · IF 14.3

Deuteration-Induced Energy Level Structure Reconstruction of Carbon Dots for Enhancing Photoluminescence

Zimin Yao,Xiaokun Wen,Xia Hong,Ran Tao,Feifei Yin,Shuo Cao,Jiayi Yan,Kexin Wang,Jiwei Wang

Constrained by a limited understanding of the structure and luminescence mechanisms of carbon dots (CDs), achieving precise enhancement of their photoluminescence (PL) performance without altering the emission wavelength and color remains a challenge. In this work, a deuterated CD is first achieved by simply replacing the reaction solvent from H 2 O to D 2 O. The substitution of D atoms for H atoms is not limited on the surface but also within the internal structure of CDs. Deuteration affects the formation of the π -conjugated network structure by altering the content of sp 2 carbon and sp 3 carbon, ultimately inducing a reconstruction for energy level structure of CDs. Both the intrinsic state and surface state emission, including quantum yield, emission intensity and lifetime, are significantly enhanced after deuteration. It benefits from the reduction in non-radiative transitions, since the lowered vibrational frequencies of D atoms and optimized local energy level distribution in CDs structure. The deuterated CDs are applied in the fabrication of white-light-emitting diodes to show their application potential. This work provides a highly versatile route for improving and controlling photoluminescence performance of CDs and has opportunities to guide the development of CDs for practical applications.

研究领域: 材料科学 · 光学
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Nature Communications · 2025 ·Vol. 16 ·期 1 ·1-9 · IF 15.7

Boosted high-throughput D⁺ transfer from D₂O to unsaturated bonds via Pdδ+ cathode for solvent-free deuteration

Zhang Xiu-Feng,Zhang Shi-Nan,Zhang Zhao,Leng Bing-Liang,Lu Kai-Yuan,Chen Jie-Sheng,Li Xin-Hao

Deuterated organic compounds have gained significant attention due to their diverse applications, including reaction mechanism studies, probes for metabolism and pharmacokinetics, and raw materials for labeled compounds and polymers. Conventional reductive deuteration methods are limited by the high cost of deuterium sources (e.g., D₂ gas) and challenges in product separation and D₂O recycling. Electrochemical deuteration using D₂O is promising, but existing methods still suffer from low Faradaic efficiency (FE) and high separation costs. Herein, we report a deuterium ion diffusion-based all-solid electrolyser, featuring a RuO₂ anode for D + generation from pure D 2 O and a Pd/nitrogen-doped carbon-based liquid diffusion cathode (Pd δ+ /NC LDC) with tunable electron deficiencies Pd δ+ /NC to enhance selective deuteration. This system achieves over 99% selectivity for deuterated benzyl alcohol with a FE of 72%, and demonstrates broad applicability for the deuteration of aldehydes, ketones, imines, and alkenes with high FE and selectivity. Moreover, the Pd δ+ /NC-based electrolyser can achieve ten-gram-scale production of deuterated benzyl alcohol over 500 hours, showcasing its potential for high-throughput, solvent-free deuteration reactions in practical applications.

研究领域: 有机化学 · 药物化学 · 合成化学
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Nuclear Materials and Energy · 2021 · IF 2.32

Analytical approach for description of deuterium content in deuterium-beryllium co-deposited layers

S. Krat,Yu. Gasparyan,Ya. Vasina,A. Prishvitsyn,G.De Temmerman,A. Pisarev

Available literature data for beryllium content in D-Be co-deposited layers was modeled using newly developed model. It was shown that the model adequately describes the experimental results. An empirical scaling for the available trap concentrations as a function of deuteron energy was introduced in order to improve the agreement between the experimental data and model predictions. The limited recombination rate describes the co-deposition better than the unlimited one. Assuming two types of traps in the film with detrapping energies of 0.8–0.9 and 1.2–1.3 eV and trap concentrations of 10 at. % and 1 at. %, respectively, and the deuterium implantation energy of 15.6 eV, the average relative deviation between experimental and predicted D/Be values of 1.9 was observed, which is better than the empirical D/Be scalings.

研究领域: 核物理学 · 材料科学
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JOURNAL OF CHROMATOGRAPHY B-ANALYTICAL TECHNOLOGIES IN THE BIOMEDICAL AND LIFE SCIENCES · 2019 · IF 2.813

Simultaneous determination of deuterated vortioxetine and its major metabolite in human plasma by UPLC-MS/MS and application to a pharmacokinetic study in healthy volunteers

Yingyue Yi,Guanghui Ren,Ming Zheng,Di Zhao,Ning Li,Xijng Chen,Yang Lu

JJH201501, a deuterated modification for multi-target antidepressant vortioxetine, is currently in phase I clinical trial. This study aimed to establish a sensitive and rapid UPLC-MS/MS method that was capable of simultaneously detecting JJH201501 and its major metabolite JJH201501-01 quantitatively in human plasma. The pretreatment was achieved by protein precipitation using 4-fold(v:v) acetonitrile with 5 ng/mL fluoxetine as internal standard precipitant. For method validation, the method was investigated in terms of the selectivity, inter- and intra-run precision and accuracy, carryover, matrix effect, extraction recovery and stability. The total running time was 3 min, and the retention time of JJH201501 and JJH201501-01 was 1.17 min and 1.05 min, respectively. The linear concentration range for JJH201501 and JJH201501-01 was 0.2 to 50 ng/mL and 0.4 to 100 ng/mL, respectively. The results showed that this method was in line with the guidelines for bioanalytical method proposed by FDA. In addition, the method was successfully applied to a plasma pharmacokinetic study of JJH201501 tablets in healthy volunteers which was part of the phase I trial.

研究领域: 药物分析 · 临床药理学 · 分析化学
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Radiation Effects and Defects in Solids · 2024 · IF 1.1

Damage caused by He and D plasma exposure in Mo/Zr-added W-Y2O3 composites

X.L. Ren,G. Yao,L.M. Luo,Y. Xu,A. Yabuuchi,Q. Xu

In the present study, we developed Mo- and Zr-added W-Y2O3 composites, and investigated their surface damage, including commercially available W induced by He and D as well as He and D mixture plasmas. Blistering was not observed in the D-plasma-irradiated W and W composites. The thickness of the damaged surface layer due to He plasma exposure of the W-Mo-Y2O3 composite was similar to that of W. However, the thickness of the damaged surface layer of the W-Y2O3 composite was half that of W. In addition, the thickness of the damaged surface layer of the W-Zr-Y2O3 composite was further improved by 5 times. Y2O3 nanoparticles, especially refined Zr-Y-O nanoparticles, act as He trap sites to suppress the formation and growth of He bubbles. Furthermore, the W-O-Y and W-O-Zr-Y nanoparticles increased the solubility of He and delayed He diffusion, hindering the formation of He bubbles.

CAS / MDL: 12054-85-2
研究领域: 材料科学 · 核能工程
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