SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Li Xu,Qiye Ju,Haiyan Jiang,Na Geng,Jianze Xiao,Ziqian Xue,Tingyu Zhu,Yangyang Guo
Heavy water (D 2 O) electrolysis is the primary technology for D 2 production, playing an irreplaceable role in fields such as nuclear fusion research and isotope tracing. However, the inherent similarity in chemical properties between H 2 O and D 2 O (with only a 1.4 °C difference in boiling points) poses significant challenges to their separation. Furthermore, the extremely low natural abundance of D 2 O (0.015 %) increases the difficulty and cost of separation, while traditional electrolysis and distillation techniques are highly energy intensive. Therefore, there is an urgent need to develop novel adsorbents for efficient and environmentally sustainable H 2 O/D 2 O separation. Herein, we used polydentate ligand 2, 5-dihydroxyterephthalic acid (DOBDC) and its derivatives 4,4́-(anthracene-9,10-diyl) bis (2-hydroxybenzoic acid (ABHB) as raw materials to prepare two novel high coordination Sr-MOFs namely IPE-1 and IPE-2, respectively. These MOFs were applied for efficient separation of H 2 O and D 2 O at room temperature. X-ray diffraction results reveal that one Sr atom in IPE-1 is coordinated with 9 oxygen atoms. This high coordination number results in the formation of ultra-small rectangular pores of approximately 2.5 Å. Adsorption isotherms of N 2 , CO 2 , H 2 O, and D 2 O indicate that the ultramicroporous structure of IPE-1 precludes efficient diffusion of CO 2 and H 2 O molecules into the MOF channels. In contrast, the activated IPE-2 exhibits good CO 2 , H 2 O, and D 2 O uptake capacities of 3 mmol/g, 8.38 mmol/g, and 6.51 mmol/g at 298 K, respectively. The Q st values and K sap values of H 2 O and D 2 O indicate that the adsorption rates of H 2 O were much higher than D 2 O under 0.2 < P/P 0 < 0.7, with a calculated ratio of approximately 1.26. This study not only provides appealing MOFs materials for efficient H 2 O/D 2 O separation at room temperature but also provides a new avenue for preparing adsorbents with high stability and high separation performance.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
Nature Communications
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2024
·Vol. 15
·期 1
·1-10
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IF 14.7
He Meng,Li Rui,Cheng Chuanqi,Liu Cuibo,Zhang Bin
The high Faradaic efficiency (FE) of the electrocatalytic deuteration of organics with D 2 O at a large current density is significant for deuterated electrosynthesis. However, the FE and current density are the two ends of a seesaw because of the severe D 2 evolution side reaction at nearly industrial current densities. Herein, we report a combined scenario of a nanotip-enhanced electric field and surfactant-modified interface microenvironment to enable the electrocatalytic deuteration of arylacetonitrile in D 2 O with an 80% FE at −100 mA cm −2 . The increased concentration with low activation energy of arylacetonitrile due to the large electric field along the tips and the accelerated arylacetonitrile transfer and suppressed D 2 evolution by the surfactant-created deuterophobic microenvironment contribute to breaking the trade-off between a high FE and large current density. Furthermore, the application of our strategy in other deuteration reactions with improved Faradaic efficiencies at −100 mA cm −2 rationalizes the design concept.
研究领域:
化学工程
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电化学
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催化科学
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DOI
PubMed
高影响因子
TALANTA
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2024
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IF 5.6
Shengdi Tai,Chengjian Zhang,Shuaibo Shi,Kang Yang,Shaolong Han,Jinyu Wu,Shishen Zhang,Kun Zhang
The increasing demands in fields of anti-counterfeiting, fluorescence analysis, clinical therapy and LED illumination are urgently eager for more excellent optically switchable luminescent materials with the stable and multimodal fluorescence in single-component matrix. Herein, the lanthanide-disalicylaldehyde coordination hybrid H 2 Q j4 /Tb x Eu y is proposed as an efficient luminescent matrix to connect terbium sensibilization with ESIPT (excited-state intramolecular proton transfer) effects, and three multi-emission hybrids are finally designed and synthesized by regulating Tb 3+ and Eu 3+ ratios. Surprisingly, the H 2 Q j4 /Tb 0.91 Eu 0.09 shows the excitation wavelength-dependent luminescence in solution which originates from two energy transfer ways of terbium sensibilization effect. It exhibits green and red lights under the 369 and 394 nm UV lamp, respectively. Three hybrids are further used as lab-on-a-molecule fluorescent probes to perform multianalyte detection for various solvents by selected fluorescent sensing channels. By means of PCA (principal component analysis) and HCA (hierarchical cluster analysis), all of them can successfully detect and discriminate17 common solvents, especially the H 2 O and D 2 O. Moreover, the H 2 Q j4 /Tb 0.91 Eu 0.09 also shows the wide linear responses of H 2 O content in D 2 O, discrimination of two-component solvent mixtures , hygroscopicity evaluation of D 2 O and information encryption which will advance the progress of multimodal luminescent materials and multianalyte chemosensors .
研究领域:
材料科学
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光学
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分析化学
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DOI
PubMed
高影响因子
ANALYTICAL CHEMISTRY
·
2019
·
IF 6.35
Hong-Zhe Li,Qing-fang Bi,Kai Yang,Bang-Xiao Zheng,Qiang Pu,Li Cui
Increasing the bioavailability of immobilized phosphorus (P) in soil by phosphate-solubilizing bacteria (PSB) is an effective strategy for sustainable agronomic use of P and for mitigating the P crisis. Here, D2O isotope labeling combined with single-cell Raman spectroscopy (Raman–D2O) was developed as an efficient activity-based approach to characterizing the presence and activity of PSB in a culture-independent way. On the basis of the finding that PSB were significantly more active than non-PSB in the presence of insoluble P, a C–D Raman band from active assimilation of D2O-derived D was established as a biomarker for both inorganic-phosphate-solubilizing bacteria and organic-phosphate-solubilizing bacteria. C–D ratios (intensities of C–D bands as percentages of the intensities of both the C–D and C–H bands) were further established as semiquantitative indicators of P-releasing activities because of the consistency between the C–D ratio and the concentration of solubilized phosphate or acid phosphatase activity as measured by conventional bulk assays. By applying Raman imaging, single-cell Raman–D2O clearly discerned PSB in a mixed-soil bacterial culture and even in complex soil communities. Remarkable heterogeneity of microbial activity, ranging from 2 to 30% (close to that in medium without P and that in medium with sufficient soluble P, respectively), was revealed at the single-cell level and clearly illustrated the subpopulation of soil bacteria active in solubilizing P. This work not only enables probing PSB and their P-releasing activities but also opens a window to explore more diverse microbial resources when obtaining related isotope-labeled substrates is prohibitive.
研究领域:
微生物学
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土壤科学
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环境生物学
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DOI
PubMed
高影响因子
ANALYTICAL CHEMISTRY
·
2020
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IF 6.785
Hong-Zhe Li,DanDan Zhang,Kai Yang,Xin-Li An,Qiang Pu,Shao-Min Lin,Jian-Qiang Su,Li Cui
The rapid spread of antibiotic resistance threatens our fight against bacterial infections. Environments are an abundant reservoir of potentially transferable resistance to pathogens. However, the trajectory of antibiotic resistance genes (ARGs) spreading from environment to clinic and the associated risk remain poorly understood. Here, single-cell Raman spectroscopy combined with reverse D2O labeling (Raman-rD2O) was developed as a sensitive and rapid phenotypic tool to track the spread of plasmid-borne ARGs from soil to clinical bacteria via transformation. Based on the activity of bacteria in assimilating H to substitute prelabeled D under antibiotic treatment, Raman-rD2O sensitively discerned a small minority of phenotypically resistant transformants from a large pool of recipient cells. Its single-cell level detection greatly facilitated the direct calculation of spread efficiency. Raman-rD2O was further employed to study the transfer of complex soil resistant plasmids to pathogenic bacteria. Soil plasmid ARG-dependent transformability against five clinically relevant antibiotics was revealed and used to assess the spreading risk of different soil ARGs, i.e., ampicillin > cefradine and ciprofloxacin > meropenem and vancomycin. The developed single-cell phenotypic method can track the fate and risk of environmental ARGs to pathogenic bacteria and may guide developing new strategies to prevent the spread of high-risk ARGs.
研究领域:
微生物学
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分子生物学
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环境科学
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生物技术
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DOI
PubMed
高影响因子
JOURNAL OF ORGANIC CHEMISTRY
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2023
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IF 3.6
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
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药物化学
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DOI
PubMed
高影响因子
JOURNAL OF CATALYSIS
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2026
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IF 6
Wei Huang,Fangjun Shao,Zhanpeng Xu,Jiale Zhang,Shaokang Zheng,Xu Zhang,Zhongzhe Wei,Jianguo Wang
Sustainable deuteration of monohydric alcohols with D 2 O under mild conditions remains challenging because of the intrinsic inertness of aliphatic sp 3 C–H bonds. Herein, a Ru catalyst supported on Ni-doped MCM-41 was developed to construct Lewis acid-modulated metal-support interfaces for efficient heterogeneous hydrogen isotope exchange. Under mild conditions (40 ℃, 0.1 MPa H 2 ), the catalyst afforded up to 99% deuterium incorporation for 1-hexanol, whereas Ru/MCM-41 gave only ∼ 24%. The enhanced performance is attributed to the combined effects of high Ru dispersion and Ni-derived interfacial acidity. Spectroscopic results indicated that Ni-O-Si motifs electronically modified interfacial Ru sites. Mechanistic studies indicated that D 2 O is the dominant deuterium source under the present conditions and showed that deuteration proceeds through rapid hydroxyl exchange followed by rate-limiting C–H activation at the Ru-Lewis acid interface (k H /k D = 2.22), consistent with a radical-mediated pathway. The catalyst also showed broad substrate scope and good durability, retaining > 90% deuterium incorporation after 14 cycles. These results identify Lewis acid-modulated metal-support interfaces as an effective motif for heterogeneous deuteration with D 2 O under mild conditions. Download: Download high-res image (67KB) Download: Download full-size image
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DOI
高影响因子
JOURNAL OF ORGANIC CHEMISTRY
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2024
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IF 3.3
Hui Xu,Zhi-Jiang Jiang,Yun Jia,Yuhang Su,Jian-Fei Bai,Zhanghua Gao,Jia Chen,Kun Gao
Aromatic sulfones are the prevailing scaffolds in pharmaceutical and material sciences. However, compared to their widespread application, the selective deuterium labeling of these structures is restricted due to their electron-deficient properties. This study presents two comprehensive strategies for the deuteration of aromatic sulfones. The base-promoted deuteration uses DMSO-d6 as the deuterium source, resulting in a rapid H/D exchange within 2 h. Meanwhile, a silver-catalyzed protocol offers a much milder option by using economical D2O to furnish the labeled sulfones.
研究领域:
药物化学
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材料科学
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有机合成
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DOI
PubMed
高影响因子
JOURNAL OF MOLECULAR LIQUIDS
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2012
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IF 1.58
Jinshou Wang,Yan Chen,Boan Shi,Yan Xie,Yu Cao,Yingxuan Liu,Shenghui Zhang
We have measured the rate of S N 1 hydrolysis reaction of 2-bromo-2-methylpropane in triethylamine + D 2 O near and far away from its critical point by electrical conductivity experiment. We report the observation of critical slowing down in the rate of reaction in the one-phase region near the consolute point of triethylamine + D 2 O, in contrast to Kim and Baird, J. Phys. Chem. A 107, 8435 (2003), who reported speeding up in the one-phase region of triethylamine + H 2 O. Like them, however, we observed slowing down in the rate of reaction in the two-phase region near the consolute point.
研究领域:
物理化学
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溶液化学
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反应动力学
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临界现象
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溶剂效应
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DOI
高影响因子
JOURNAL OF ORGANIC CHEMISTRY
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2026
·
IF 3.3
Yu Meng,Zhi-Jiang Jiang,Jiawei Han,Kenan Wang,Mengtao Zhu,Jian-Fei Bai,Jia Chen,Zhanghua Gao
Hydrogen isotope exchange is an atom-economical strategy for accessing deuterium-labeled molecules, but its synthetic utility is often limited by slow exchange kinetics and poor reactivity of π-extended arenes. Herein, we report a palladium-catalyzed nondirected hydrogen isotope exchange (HIE) enabled by a dual-ligand combination of a monoprotected aminoethyl thioether (MPAThio) and an N-heteroarene ligand. This system exhibits faster HIE kinetics, reaching isotopic equilibrium within 30 min at 105 °C (and within 60 min at 90 °C), and enables efficient deuterium incorporation under mild conditions using D2O as the deuterium source. The protocol enables efficient deuteration of a broad range of mono- and multisubstituted arenes. For poorly soluble substrates relevant to organic light-emitting diode materials, a cosolvent strategy addresses solubility limitations, affording high deuterium incorporation. Mechanistic studies indicate that the MPAThio ligand lowers the barrier of accessing the reactive C-H activation manifold, thereby favoring efficient reversible HIE.
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DOI
高影响因子
ANALYTICAL CHEMISTRY
·
2022
·
IF 8.008
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
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光化学
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材料科学
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产品关联
DOI
PubMed
高影响因子
TALANTA
·
2024
·
IF 5.6
Jingyun Huang,Qingning Zuo,Xiaoliang Wang,Xiaoping Bai,Qiming Wei,Junnan Zhang,Xiaoshuang Geng,Zitao Yan,Zhen Li,Bo Yang,Lu Li
The real-time detection of gaseous H 2 O and its typical isotopic molecules, e.g., H 2 18 O, D 2 O, HDO, and HTO, is highly desirable in many fundamental scientific studies and practical monitoring, such as mechanistic studies of H 2 O-involved chemical reactions and radiation risk warning of abnormal HTO emissions. However, ionization methods for mass spectrometry (MS) to directly measure isotopic water molecules are limited, and the discrimination of those with similar molecular weights (MWs) usually requires the use of high-resolution mass spectrometers. In this study, we present a highly efficient ionization method for water vapor based on a photoinduced associative ionization (PAI) reaction, where one excited-state CH 2 Cl 2 ∗ reacts with two H 2 O molecules to transfer a proton from one H 2 O molecule to another (i.e., the analyte). Benefit to the distinctive ionization pathway, different featured ions of H 2 O, D 2 O, and H 2 18 O were observed. Surprisingly, each isotopic water molecule has its own unique PAI mass spectrum pattern according to the same ionization principle, which offers a convenient method for distinguishing isotopic water molecules with similar MWs, such as D 2 O, H 2 18 O, and HTO (20 Da), without the need for high-resolution mass spectrometers. The measured detection sensitivities of a laboratory-built PAI time-of-flight mass spectrometer towards D 2 O and H 2 18 O were 1465.1 ± 37.0 and 1324.4 ± 86.4 counts ppbv −1 , respectively, in a detection time of 10 s. The corresponding 3σ LODs were 0.10 and 0.11 ppbv, respectively. This study provides a novel ionization method for the direct detection and discrimination of isotopic water molecules, which has potential to combine with portable MS for on-site measurements.
研究领域:
分析化学
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环境科学
·
放射化学
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产品关联
DOI
PubMed
高影响因子
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