EUROPEAN JOURNAL OF INORGANIC CHEMISTRY
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2015
·Vol. 2015
·期 13
·2229-2236
·
IF 2.942
Long Zhang,Shulin Zhao,Yafei Li,Yaqian Lan,Min Han,Zhihui Dai,Jianchun Bao
Graphical Monoclinic Cu 2 Se nanocrystals and Cu 2 Se/Pd heterostructures have been synthesized by simple and facile methods. Owing to strong synergistic effects and phase-dependent characteristics, the surface-enhanced Raman scattering performance of the Cu 2 Se/Pd heterostructure is superior to those of Cu 2 Se, Pd, CuSe/Pd, and Cu 2– x Se/Pd. We have developed a simple and facile approach to the fabrication of monoclinic Cu 2 Se nanocrystals and Cu 2 Se/Pd heterostructures. [(C 2 H 5 ) 4 N] 2 [CuCl 4 ] was chosen as the copper source and SeO 2 /terpineol was used as the Se –II precursor for the generation of hexagonal CuSe and cubic Cu 2– x Se through the “hot-injection” and “one-pot” methods, respectively. Both CuSe and Cu 2– x Se could be further transformed into monoclinic Cu 2 Se through heat treatment with trioctylphosphine (TOP) at 220 °C. Cu 2 Se/Pd as well as CuSe/Pd and Cu 2– x Se/Pd were readily obtained by simply mixing copper selenides and Pd(NO 3 ) 2 in a 2-propanol solution. The Pd nanoparticles were distributed on the surface of the copper selenides. The effect of certain reaction parameters on the formation of copper selenides was studied. The amount of terpineol used played an important role in the phase-selective synthesis of CuSe and Cu 2– x Se. The surface-enhanced Raman scattering (SERS) performance of the heterostructures was investigated with 4-mercaptopyridine (4-Mpy) as a probe molecule. Owing to the strong synergistic effects between Cu 2 Se and Pd, Cu 2 Se/Pd showed greater SERS performance than pure Pd or Cu 2 Se. Moreover, compared to those of CuSe/Pd and Cu 2– x Se/Pd, Cu 2 Se/Pd exhibited the highest SERS sensitivity to 4-Mpy with a detection limit as low as 1.0 × 10 –9 M , which revealed its phase- and composition-dependent characteristics. This Cu 2 Se/Pd heterostructure exhibits potential applications in the chemical and biological sensing fields.
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Journal of the American Chemical Society
·
2015
·
IF 12.113
Xiao-Li Pei,Yang Yang,Zhen Lei,Shan-Shan Chang,Zong-Jie Guan,Xian-Kai Wan,Ting-Bin Wen,Quan-Ming Wang
The activation of C(sp3)–H bonds is challenging, due to their high bond dissociation energy, low proton acidity, and highly nonpolar character. Herein we report a unique gold(I)–silver(I) oxo cluster protected by hemilabile phosphine ligands [OAu3Ag3(PPhpy2)3](BF4)4 (1), which can activate C(sp3)–H bonds under mild conditions for a broad scope of methyl ketones (RCOCH3, R = methyl, phenyl, 2-methylphenyl, 2-aminophenyl, 2-hydroxylphenyl, 2-pyridyl, 2-thiazolyl, tert-butyl, ethyl, isopropyl). Activation happens via triple deprotonation of the methyl group, leading to formation of heterometallic Au(I)–Ag(I) clusters with formula RCOCAu4Ag4(PPhpy2)4(BF4)5 (PPhpy2 = bis(2-pyridyl)phenylphosphine). Cluster 1 can be generated in situ via the reaction of [OAu3Ag(PPhpy2)3](BF4)2 with 2 equiv of AgBF4. The oxo ion and the metal centers are found to be essential in the cleavage of sp3 C–H bonds of methyl ketones. Interestingly, cluster 1 selectively activates the C–H bonds in −CH3 rather than the N–H bonds in −NH2 or the O–H bond in −OH which is traditionally thought to be more reactive than C–H bonds. Control experiments with butanone, 3-methylbutanone, and cyclopentanone as substrates show that the auration of the C–H bond of the terminal methyl group is preferred over secondary or tertiary sp3 C–H bonds; in other words, the C–H bond activation is influenced by steric effect. This work highlights the powerful reactivity of metal clusters toward C–H activation and sheds new light on gold(I)-mediated catalysis.
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PubMed
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2017
·
IF 2.536
Yu-Feng Zhu,Yong-Sheng Wang,Bin Zhou,Yan-Qin Huang,Xue-Jiao Li,Si-Han Chen,Xiao-Feng Wang,Xian Tang
We for the first time confirmed that the low concentrations of Ag(I) could induce a silver specific aptamer probe (SAP) from a random coil sequence form to G-quadruplex structure. Thereby, a novel highly sensitive fluorescence strategy for silver(I) assay was established. The designed multifunctional SAP could act as a recognition element for Ag(I) and a signal reporter. The use of such a SAP can ultrasensitively and selectively detect Ag(I), giving a detection limit down to 0.64 nM. This is much lower than those reported by related literatures. This strategy has been applied successfully for the detection of Ag(I) in real samples, further proving its reliability. Taken together, the designed SAP is not only a useful recognition and signal probe for silver, but also gives a platform to study the interaction of monovalent cations with DNA .
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高影响因子
Chemistry-Switzerland
·
2025
·Vol. 7
·期 3
·75
·
IF 2.4
Jing Zhang,Xiaoxing Ji,Qingxiu Yu,Xixi Zhang,Chuanlin Li,Na Li,Mengzhen Kong,Dingzheng Li,Wenjie Liu,Chenggang Wang,Xijin Xu
Zinc-halogen batteries are usually based on two-electron transfer reactions from X−to X2. However, the halogen is capable of being further oxidized to higher valence states, thereby achieving the higher capacity of zinc- halogen batteries. Here, a six-electron reaction based on I−/I+and Br−/Br0is activated successfully by introducing KI into the electrolyte. ZIF-8-derived porous carbon (ZPC), serving as the host of halogen, effectively suppresses polybromide/polyiodide shuttle owing to the chemisorption/physical adsorption. Additionally, the adsorption of I−on the surface of the zinc anode effectively inhibits the growth of dendrites and the formation of by-products. Consequently, zinc-bromine batteries exhibit outstanding electrochemical performance, including a specific capacity of 345 mAh g−1at 1 A g−1and an excellent capacity retention of 80% after 3000 cycles at 2 A g−1. This strategy provides a novel way for enhancing the electrochemical performance of zinc-halogen batteries.
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TALANTA
·
2025
·
IF 6.1
Yafang Shen,Xingyue Tang,Jiangqi Wang,Huang Dai,Yanna Cui,Qiuyue Hu,Yuxin Wu,Fei Jia,Guijie Hao
Recent years have witnessed the flourishing of CRISPR/Cas-based biosensors in various fields. However, most of them were developed for nucleic acid detection because non-nucleic acid targets are unable to unleash the cleavage activity of the CRISPR/Cas system directly. To circumvent this problem, activator DNA and deoxyribonuclease I (DNase I) were introduced in this research to render the CRISPR/Cas12a system as a new powerful tool for the detection of enrofloxacin (ENR), a common veterinary drug. In this biosensor, target ENR competed with DNase I- and bovine serum albumin-ENR composite-modified gold nanoparticles (DNase I-AuNPs-BSA-ENR) for the binding sites on the surface of antibody-modified magnetic nanoparticles (immuno-MNPs). Then, the captured DNase I-AuNPs-BSA-ENR degraded the activator DNA in the solution, which inhibited the activation of the CRISPR/Cas12a system. Finally, the fluorescence released by the activated CRISPR/Cas12a system was measured for the quantitative detection of ENR. The ingenious use of activator DNA and DNase I helped transduce the target recognition event into the cleavage activity of the CRISPR/Cas12a system. Moreover, the dual enzymatic amplification from DNase I and the CRISPR/Cas12a system guaranteed the sensitivity of this method with a low detection limit of 0.04 ng/mL. The developed biosensor extended the application of the CRISPR/Cas12a system for the sensitive detection of non-nucleic acid targets, providing a powerful tool in various fields such as environmental monitoring, food safety and clinical diagnosis.
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JOURNAL OF THE MECHANICS AND PHYSICS OF SOLIDS
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2023
·
IF 5.3
Xingjian Sun,Ping Rao,Xitao He,Canhui Yang,Wei Hong
Do materials prepared from identical compositions of constituting ingredients always exhibit similar mechanical properties? The answer is negative for most structural materials, as has been demonstrated by extensive studies on various factors such as the effects of processing and microstructures. However, the same question has seldom been addressed in the case of polymeric gels. In this work, by using a simple chemically crosslinked hydrogel as a model system, the mechanical properties, including elastic stiffness , fracture toughness , and fatigue threshold, of gels with identical chemical compositions are systematically investigated. The distinct material properties are then rationalized and quantitatively correlated to synthesis conditions and manufacture processes through scaling laws derived from basic physics. Different scaling laws are identified between samples prepared from swelling and deswelling. Extreme mechanical properties, such as the remarkable fracture energy of hydrogels prepared by deswelling from highly swollen samples, are observed and attributed to the structural characteristics of the polymer network , and further correlated to the synthesis processes. This study provides insights into the synthesis-property correlations of polymeric gels, which may have profound influences on the design of new polymeric materials and their applications in various fields.
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JOURNAL OF ORGANIC CHEMISTRY
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2023
·
IF 3.6
Ming Huang,Changsheng Zhou,Ke-Fang Yang,Ze Li,Guo-Qiao Lai,Pinglu Zhang
An effective (NHC)AgCl catalysis was developed in the hydroborylation of cyclopropenes with B2pin2, delivering a variety of cyclopylboronates in a stereoselective manner, which could be easily transformed for the construction of versatile cyclopropanes. This protocol works effectively under mild reaction conditions in an open-air atmosphere, and it was easy to apply on a gram scale. This novel method in detail was also explored by control experiments, providing a number of key insights. The kinetic process followed by 1H NMR indicated that the reaction was finished in 15 min. Furthermore, the mechanism of silver(I)-catalyzed hydroborylation of cyclopropenes was proposed, with the protonation by methanol as the rate-determining step.
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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
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2026
·
IF 6.7
Zhang Huang,Weijie Zhou,Jiani Dong,Lin Zhu,Yayang Xu,Xuesong Chang,Lei Ye,Weibin Bai
Abstract The crude anthocyanin extract isolated from cranberry (Vaccinium macrocarpon Aiton) was enzymatically acylated with fatty acids of varying chain lengths using Novozyme 435 (Candida antarctica lipase B immobilized on acrylic resin). After optimization, the highest acylation rates of 65.72% and 70.64% for cyanidin-3-O-galactoside and peonidin-3-O-galactoside, respectively, were obtained by acylating with octanoic acid under the conditions of lipase dosage of 10 mg/mL, molar ratio of 1:418, at 50 °C for 30 h in 2-methyl-2-butanol. Acylated anthocyanins with high purity (>97%) were obtained through liquid–liquid extraction and medium-pressure liquid chromatography and identified as cyanidin-3-O-(6″-octanoyl) galactoside and peonidin-3-O-(6″-octanoyl) galactoside by MS/MS and 2D NMR. The acylated cranberry anthocyanins exhibited enhanced lipophilicity, photostability, thermostability, and excellent antioxidant activity in both aqueous and lipid systems. These findings demonstrate enzymatic acylation in a crude anthocyanin matrix and provide insights into acylation-induced structure–property relationships, supporting the rational development of functionalized anthocyanins from natural extracts.
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ACS Applied Polymer Materials
·
2026
·
IF 5.2
Jiru Jia,Fangqing Ge,Xiaotian Chen,Zhihe Zhang,Lvyi Yang,Jing Qu,Jun Peng,Qi Xiao,Ya Yang,Wei Ma,Jie Chen
Abstract To address the challenge of balancing high-water content with structural stability in hydrogels, gelatin methacryloyl (GelMA) was introduced into a poly(acrylic acid-co-hydroxyethyl acrylate) system. GelMA/PAH composite hydrogels (Gel-PAH) were then prepared through one-step ultraviolet (UV) photocuring, and their network formation and overall properties were tuned by varying the glycerol dimethacrylate (GDMA) content. The Gel-PAH hydrogels exhibited higher hydration capacity and greater surface wettability than the corresponding PAH hydrogels. As the GDMA content increased, the gel fraction and tensile strength of both the PAH and Gel-PAH series generally increased. The tensile strength of the Gel-PAH hydrogels ranged from approximately 1.6 to 2.5 MPa. Gel-PAH-0.15 exhibited an equilibrium water content of 82.55%, a water contact angle of approximately 39°, and a relative cellular metabolic activity of approximately 84% after 24 h. Overall, Gel-PAH-0.15 achieved a favorable balance among network stability, hydration capacity, mechanical performance, and preliminary direct contact cytocompatibility. These results show that a compositionally simple AA/HEA-GelMA system provides a straightforward route to tune hydration and mechanical performance through one-step UV photocuring and adjustment of GDMA content, without introducing additional reinforcing fillers or sequential cross-linking processes.
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ACS Synthetic Biology
·
2026
·
IF 4.5
Jiao Liu,Niling He,Yi Zhang,Bin Zhang,Jie Bao
Abstract Achieving highly coordinated metabolism and efficient conversion of lignocellulose-derived non-glucose sugars remains a major challenge for biorefinery microbial cell factories. Herein, we report an evolutionary rewiring of an engineered lactic acid bacterium Pediococcus acidilactici G1 with enhanced co-utilization of glucose, xylose, arabinose, mannose, and galactose for l-lactic acid generation. Transcriptomic analysis revealed the extraordinary upregulation of a unique sugar transporter gene cluster, manXYZ, while genome re-sequencing identified two convergent mutations in the transcriptional regulators CcpA (T65I) and LevR (E159G). Back mutation, reverse metabolic engineering, and electrophoretic mobility shift assays (EMSA) were then employed to investigate the regulation of manXYZ expression by CcpA T65I and LevR E159G. Collectively, our findings demonstrate that recurrent mutations in transcriptional regulators CcpA and LevR drove the significant upregulation of the manXYZ sugar transporter cluster during adaptive evolution, highlighting the importance of sugar transport in improving non-glucose sugar metabolism. This study not only develops a promising strain for practical biorefinery applications but also provides a new sugar transporter solution, rather than regular intracellular metabolic pathway engineering, for highly efficient non-glucose sugars utilization in P. acidilactici.
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ACS Sustainable Chemistry & Engineering
·
2026
·
IF 7.6
Changliu He,Chengye Li,Yuan Fang,Xi Zhao,Tianwei Tan,Huimin Yun,Xu Zhang
Abstract Efficient fractionation of lignocellulosic biomass is essential for maximizing carbon utilization and enabling integrated biorefinery processes. We developed a three-stage countercurrent recycling process using a fermentation compatible deep eutectic solvent (DES) for Pennisetum × sinese. In this process, regenerated DES contacted the partially fractionated solids in the final stage, while the lignin-rich DES stream was used for the initial treatment of fresh biomass. This countercurrent arrangement improved the use of the remaining solvent capacity. Lignin and hemicellulose removals remained at approximately 90 and 95%, respectively, over 12 recycling cycles. The glucose yield remained at 34.28–37.26 g per 100 g of dry biomass, with fluctuations between cycles being smaller than those observed in conventional batch cycles. In addition, 10–14 g of low-molecular-weight lignin was recovered per 100 g of dry biomass, with limited structural variation during recycling. The DES recovered remained suitable for microbial fermentation and showed high glycerol utilization, demonstrating its potential for further biological conversion. Overall, the three-stage countercurrent recycling process provides a practical strategy for extending DES reuse and integrating biomass fractionation, fermentable-sugar production, lignin recovery, and further valorization of the solvent within a lignocellulosic biorefinery.
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Journal of the American Chemical Society
·
2026
·
IF 16.6
Wei Tan,Xueqing Liu,Jiawei Yang,Xiaoyu Ji,Kailong Ye,Shaohua Xie,Ge Yao,Chuanzhi Sun,Fudong Liu,Lin Dong
Abstract The catalytic conversion of gaseous NO to NH3 offers a promising dual-benefit strategy for environmental remediation and sustainable chemical synthesis. Herein, CuO/Al2O3 catalysts with varied CuO loadings (x wt %, xCu/Al) were developed for the possible NH3 production from NO reduction by CO with the assistance of H2O. While increasing CuO loading (1–12 wt %) monotonically improved NO conversion to N2 under dry conditions, the introduction of H2O dramatically boosted NO conversion on 5Cu/Al with highly dispersed CuOx clusters, raising its NO conversion comparable to that of 12Cu/Al. Further analysis revealed that NH3 was generated on xCu/Al catalysts under wet conditions, with NH3 generation on 5Cu/Al initiating at the lowest temperature (275 °C) and being the most vigorous. Combined experimental and theoretical analysis suggested that, on CuOx clusters, H2O facilitated the conversion of the NCO* intermediate to NH3 with a much lower activation barrier compared to its CO-mediated pathway to N2, well explaining the boosted NO conversion and NH3 yield on the 5Cu/Al catalyst upon H2O addition to NO + CO flow. This work highlights that a simple, earth-abundant Cu catalyst enabled the efficient and cost-effective synthesis of NH3 from air pollutants of NO and CO under mild conditions, underscoring a sustainable strategy that simultaneously addresses pollution abatement and resource recovery.
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