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JOURNAL OF MOLECULAR STRUCTURE · 2025 · IF 4.7

Rigid clusteroluminogens of p(C3O2)n polyesters for detection of deuterated water

Huiling Yuan,Qihang Sun,Jinming Chang,Hejun Gao,Juan Zhang,Fang Liao,Hongquan Fu,Yunwen Liao

The rapid expansion of nuclear energy confronts ecological challenges, especially the analysis of heavy water (D 2 O) in radioactive wastewater. The unique red carbon (C 3 O 2 ) molecule spontaneously polymerizes into highly conjugated fluorescent structures, p(C 3 O 2 ) n , enabling us to deeply investigate their recognition mechanism for D 2 O, as aggregation-induced emission luminogens. Density functional theory calculations and experiments reveal the π–π stacking crystal structure of p(C 3 O 2 ) n nanosheets in an aggregated state, enhancing their fluorescence properties in solution. This allows for highly sensitive, fast (< 0.2 s), and stable detection of D 2 O, with a minimum detection limit of 2.91×10 −5 %, unaffected by external factors. The fluorescence quenching is attributed to hydrogen bond formation between -C=O groups and D 2 O's D atoms (static quenching) and intramolecular electron transfer (dynamic quenching). Thus, p(C 3 O 2 ) n polyesters serve as an effective luminescent probe for D 2 O sensing, offering a novel approach for designing conjugated fluorescent polyesters.

研究领域: 材料科学 · 环境科学 · 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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ANALYTICAL CHEMISTRY · 2022 · IF 8.008

Highly Facile Strategy for Detecting D2O in H2O by Porphyrin-Based Luminescent Probes

Zhengang Han,Juxia Wang,Peiyao Du,Jing Chen,Shuhui Huo,Huixia Guo,Xiaoquan Lu

Owing to their almost similarities in size, shape, and chemical reactivity, effectively distinguishing deuteroxide (D2O) in water (H2O) remains an ongoing challenge, and the examples of a D2O probe are still quite scarce. Herein, since H2O can decrease the lifetime of a singlet oxygen as a vital intermediate and an H/D exchange in the luminescence process of porphyrins, we systematically investigated the enhanced ultraviolet–visible (UV–vis), photoluminescence (PL), and electrochemiluminescence (ECL) of water-soluble tetrakis(carboxphenyl)porphyrin (TCPP) in D2O. The findings showed that these luminescent properties had been greatly enhanced with the increase of the D2O fraction in water. Consequently, we first developed the highly facile methods of detecting D2O in H2O by the UV–vis, PL, and ECL of TCPP, respectively. Impressively, the ECL analysis exhibited a great superiority with a lower detection limit of 0.29 nM. The work not only achieves the challenging task of distinguishing between H2O and D2O but also provides a unique strategy to enhance the luminescent performance of porphyrin.

研究领域: 分析化学 · 光化学 · 材料科学
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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

Self-preservation effect exceeding 273.2 K by introducing deuterium oxide to form methane hydrate

Jun Chen,Jianjian Wu,Yaosong Zeng,Zhikai Liang,Guangjin Chen,Bei Liu,Zhi Li,Bin Deng

Self-preservation effect of hydrate is an advantage for gas storage by using hydrate-based technology. Unlike focusing on guest molecules in previous publications, deuterium   oxides (D 2 O) were introduced as one of host molecules to form methane hydrate. Methane hydrate dissociated percentage was 92.2% after 12 h of dissociation at 273.7 K without the addition of D 2 O, while the methane hydrate dissociated percentage decreased to 55.2 % with the addition of 30 wt% D 2 O. The methane hydrate dissociated percentage reduced to 15.7% when methane hydrate formed in D 2 O system. The results suggested that the self-preservation effect of methane hydrate was improved to above 273.2 K for the first time since this abnormal phenomenon was found in 1986. The temperature of self-preservation effect for (CH 4  + D 2 O) hydrate was improved at least 3.5 K higher than that for (CH 4  + H 2 O) hydrate. From the simulation results, some (D 2 O + H 2 O) mixed cages with different D 2 O and H 2 O molecules formed, and CH 4 inserted into the mixed cages to form CH 4 hydrate as sI structure. The (D 2 O + H 2 O) mixed cages may explain the self-preservation effect of (CH 4  + D 2 O + H 2 O) hydrate above 273.2 K to some extent. Finally, it was also found from the simulation results that (CH 4  + D 2 O + H 2 O) hydrate not only formed from hydrate/(D 2 O + H 2 O) contact, but also nucleated independently.

CAS / MDL: 7789-20-0
研究领域: 化学工程 · 材料科学
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ADVANCED MATERIALS · 2022 ·Vol. 34 ·期 49 ·2206524 · IF 32.086

Macroscopic Heterostructure Membrane of Graphene Oxide/Porous Graphene/Graphene Oxide for Selective Separation of Deuterium Water from Natural Water

Jing Liang,Xin Zhang,Tian-qi Liu,Xu-dong Gao,Wen-bin Liang,Wei Qi,Li-juan Qian,Zhan Li,Xi-meng Chen

Deuterium water (D 2 O) is a strategic material that is widely used in and scientific research and has applications in fields such as nuclear energy generation. However, its content in natural water is extremely low. Therefore, the development of a room-temperature technology for achieving simple, efficient, and low-cost separation of D 2 O from natural water is challenging. In this study, porous graphene (PG) nanosheets with “crater-like” pores are sandwiched between two layers of graphene oxide (GO) membranes to prepare a GO/PG/GO membrane with a macroscopic heterostructure, which can be used to separate D 2 O and H 2 O by pressure-driven filtration. At 25 °C, the rejection rate of D 2 O is ≈97%, the selectivity of H 2 O/D 2 O is ≈35.2, and the excellent performance can be attributed to the difference of transmembrane resistance and flow state of H 2 O and D 2 O in the confinement state. In addition, the D 2 O concentration in natural water is successfully enriched from 0.013% to 0.059% using only one stage, and the membrane exhibits excellent structural and cycling stability. Therefore, this method does not require ultralow temperatures, high energy supplies, complex separation equipment, or the introduction of toxic chemicals. Thus, it can be directly applied to the large-scale industrial production and removal of D 2 O.

CAS / MDL: 7732-18-5 7647-01-0
研究领域: 材料科学 · 化学工程 · 能源技术
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CRYSTENGCOMM · 2025 ·Vol. 27 ·期 16 ·2591-2599 · IF 2.6

A flexible molecular organic crystal with π–π bonding for the highly selective recognition of hydrogen isotopes

Min Lei,Lisha Jiang,Chunhui Wang,Jianxin Song,Wei Liu,Jie Qiu

Deuterium oxide (D2O) is widely used in diverse fields, notably as a moderator in heavy water reactors, for electrolytic extraction of deuterium gas, and in nuclear magnetic resonance (NMR) research. However, it exhibits a high susceptibility to H2O contamination. Herein, a fluorescent hydrogen-bonded molecular organic crystal (ASP-101) with robust π–π interactions was synthesized by using 5,5′-(9,10-anthracene diphenyl dicarboxylic acid) (H4ADIP) and dimethyl sulfoxide (DMSO). Distinct fluorescence quenching phenomena were observed when ASP-101 was soaked in H2O and D2O. Based on these phenomena, subsequent studies demonstrated that ASP-101 is capable of detecting trace amounts of H2O in D2O, with a KSV value of 6 × 10−2 M−1 and a detection limit of 6.5 × 10−3 M (0.117 ppm). Batch experiments proved that the DMSO molecules within ASP-101 undergo exchange with H2O and D2O after soaking in aqueous solution. Previous research had found that deuteration can affect the emission properties of organic molecules. Thus, ASP-101's ability to detect H2O in D2O may be attributed to the fluorescent difference arising from the incorporation of H2O and D2O into its structure via solvent exchange. This study presents an authentic scenario for advancing isotopic identification based on alterations in fluorescence induced by solvent exchange.

CAS / MDL: 7789-20-0
研究领域: 材料科学 · 有机化学 · 分析化学 · 核工程 · 荧光光谱学
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APPLIED MICROBIOLOGY AND BIOTECHNOLOGY · 2018 ·Vol. 103 ·期 3 ·1455-1464 · IF 3.34

Heavy water-labeled Raman spectroscopy reveals carboxymethylcellulose-degrading bacteria and degradation activity at the single-cell level

Olaniyi Oladipo Oladiti,Yang Kai,Zhu Yong-Guan,Cui Li

Biodegradation of cellulose-rich substrates is an indispensable process for soil carbon replenishment in various ecological niches. Biodegradation of cellulose has been studied extensively via an enzyme assay to quantify the amount of cellulase with a view to identify effective cellulose degraders. However, a bulk enzyme assay undermines the role of physiological heterogeneity between cells; it is therefore imperative to opt out for a more effective method such as single-cell Raman spectroscopy combined with heavy water (D 2 O) to reveal active cellulose degraders. Cellular incorporation of D 2 O-derived D produces a new C-D Raman band which can act as a quantitative indicator of microbial activity. In this study, metabolic responses of seven cellulose-degrading bacteria to carboxymethylcellulose (CMC) and glucose were evaluated via the C-D Raman band. On the basis of % C-D, CMC was demonstrated to be most efficiently metabolized by Bacillus velezensis 2a-9 and Providencia vermicola 5a-9(b). Metabolic activity between individual cells of B . velezensis and P . vermicola towards CMC ranged from approximately 8 to 27% and 6 to 16%, respectively, clearly indicating heterogeneous degradation activities among isogenic populations. Linear correlation between % C-D and specific endoglucanase activity validated Raman results on CMC-degrading activity. Also, % C-D obtained from bacteria cultivated with only glucose was around 60% higher than that obtained from CMC, indicating the preference of bacteria for simple sugar glucose than CMC. In conclusion, Raman spectroscopy combined with heavy water is a sensitive analytical technique to reveal cellulose degraders and their degrading activities.

研究领域: 微生物学 · 环境科学 · 光谱学
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