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MATERIALS LETTERS · 2018 · IF 2.687

A low-cost, high-efficiency and durable homogeneous system for molecular hydrogen

Qifeng Liu,Bingrui Liu,Qian Zhang,Jianping Gao,Jingjun Ma

High-efficiency hydrogen evolution is obtained from a novel fluorescein homogeneous system, comprising a noble metal free fluorescein as the photosensitizer, Pt nanoparticle as the cocatalyst and TEOA as the holes scavenger in an aqueous solution under visible light irradiation. The highest H 2 production rate is 491.40 μmol/h (λ > 420 nm) and quantum efficiencies of our system are among the highest reported for the molecular hydrogen systems in the visible light range. Unlike many reported molecular hydrogen systems are either unstable under illumination and expensive, or have weak photocatalytic performances, our low-cost system exhibits excellent activity and endurance. We believe that this low-cost, high-efficiency and durable homogeneous system for molecular hydrogen may result in new breakthroughs for the hydrogen energy and solar energy utilization.

CAS / MDL: 2321-07-5
研究领域: 能源科学 · 光化学 · 材料科学
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APPLIED CATALYSIS A-GENERAL · 2019 · IF 4.63

Cobalt in N-doped carbon matrix catalyst for chemoselective hydrogenation of nitroarenes

Yihu Dai,Chunyang Jiang,Min Xu,Bo Bian,Di Lu,Yanhui Yang

Anilines as important intermediates for both organic synthesis and industrial manufactory are densely substituted with a variety of functional moieties, and the transformation of nitroarenes into corresponding anilines requires catalytically selective hydrogenation catalyst. Herein, we describe a simple pyrolysis strategy to prepare cobalt catalysts in nitrogen-doped carbon matrix applied in the selective hydrogenation of nitroarenes with molecular hydrogen. The Co/NC catalysts are obtained through thermal treatment of mixed precursors of cobalt phthalocyanine and melamine . The surface-modified Co particles with Co 3 O 4 and CoN x sites are surrounded by N-doped carbon layers according to a series of structural characterization results. These Co/NC catalysts are capable of efficiently selective hydrogenation of nitrobenzene and various substituted nitroarenes into corresponding anilines under relatively mild reaction conditions. The optimal catalytic hydrogenation performance is contributed to the fast rate of H 2 dissociated activation on the CoN x active sites and the facile adsorption of the reactant substances, which is verified by the isotopic H 2 -D 2 exchange experiments, reactant adsorption and the ORR reaction tests. Furthermore, the heterogeneous Co/NC catalyst is highly stable without the Co leaching and deactivation issues during the recycling reaction runs.

CAS / MDL: 108-78-1
研究领域: 催化化学 · 材料科学
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2023 · IF 8.2

Exploration of the structural mechanism of hydrogen (H2)-promoted horseradish peroxidase (HRP) activity via multiple spectroscopic and molecular dynamics simulation techniques

Chuang Zhu,Fenfen Wei,Huibin Jiang,Zihan Lin,Lingyue Zhong,Yan Wu,Xiangjun Sun,Lihua Song

Horseradish peroxidase (HRP) is an enzyme that is widely used in various fields. In this study, the effects of molecular hydrogen (H 2 ) on the activity and structural characteristics of HRP were investigated by employing multiple spectroscopic techniques , atomic force microscopy (AFM) and molecular dynamics (MD) simulations. The results demonstrated that H 2 could enhance HRP activity, especially in 1.5 mg/L hydrogen-rich water (HRW). The structural analysis results showed that H 2 might alter HRP activity by affecting the active sites, secondary structure , hydrogen bonding network, C S groups, and morphological characteristics . The MD results also confirmed that H 2 could increase the Fe N bond distance in the active site, affect the secondary structure, and increase the number of hydrogen bonds . The MD results further suggested that H 2 could increase the number of salt bridges, and lengthen the S S bonds in HRP. This study primarily revealed the mechanism by which H 2 enhances the HRP activity, providing insight into the interactions between gas and macromolecular proteins. However, some of the results obtained via MD simulations still need to be verified experimentally. In addition, our study also provided a new convenient strategy to enhance enzyme activity .

研究领域: 生物化学 · 酶学 · 计算生物学
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Applied Sciences-Basel · 2017 ·Vol. 7 ·期 5 ·475 · IF 1.679

A Fast and Cost-Effective Detection of Melamine by Surface Enhanced Raman Spectroscopy Using a Novel Hydrogen Bonding-Assisted Supramolecular Matrix and Gold-Coated Magnetic Nanoparticles

Jing Neng,Jiayuan Tan,Kan Jia,Peilong Sun

A fast and cost-effective melamine detection approach has been developed based on surface enhanced Raman spectroscopy (SERS) using a novel hydrogen bonding-assisted supramolecular matrix. The detection utilizes Fe3O4/Au magnetic nanoparticles coated with 5-aminoorotic acid (AOA) as a SERS active substrate (Fe3O4/Au–AOA), and Rhodamine B (RhB) conjugated AOA as a Raman reporter (AOA–RhB). Upon mixing the reagents with melamine, a supramolecular complex [Fe3O4/Au–AOA•••melamine•••AOA–RhB] was formed due to the strong multiple hydrogen bonding interactions between AOA and melamine. The complex was separated and concentrated to a pellet by an external magnet and used as a supramolecular matrix for the melamine detection. Laser excitation of the complex pellet produced a strong SERS signal diagnostic for RhB. The logarithmic intensity of the characteristic RhB peaks was found to be proportional to the concentration of melamine with a limit of detection of 2.5 µg/mL and a detection linearity range of 2.5~15.0 µg/mL in milk. As Fe3O4nanoparticles and AOA are thousands of times less expensive than the monoclonal antibody used in a traditional sandwich immunoassay, the current assay drastically cut down the cost of melamine detection. The current approach affords promise as a biosensor platform that cuts down sample pre-treatment steps and measurement expense.Keywords:surface enhanced Raman spectroscopy (SERS);Fe3O4magnetic nanoparticles;melamine;detection;supramolecular hydrogen bonding;matrix

研究领域: 分析化学 · 食品安全
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ACS Applied Polymer Materials · 2023 · IF 5

Design of a Low-Temperature Ring-Opening Benzoxazine System Using a Supramolecular Hydrogen-Bond Structure

Jingkai Liu,Liyue Zhang,Xinbei Zhu,Qing Chen,Kan Zhang,Xiaoqing Liu

Phenolic derivatives capable of reducing the ring-opening temperature of benzoxazine resin have gradually emerged as valuable modules for benzoxazine chemistry, not to mention their good compatibility, coreactivity, and network modifiability. However, the previously reported unsatisfactory promotion effects, unclear reaction mechanisms, and unstable structure have severely limited the development of benzoxazine/phenol systems. Herein, a supramolecular hydrogen-bonded system consisting of resorcinol and 2-aminopyridine benzoxazine (PH-2a) was developed. The PH-2a/resorcinol mixture system with an equivalence ratio of 1:1 exhibited a dramatic reduction in ring-opening peak temperature (Tp) from 283 to 110 °C. Experimental combined with computational investigations supported its supramolecular H-bond behavior. Based on the cross-comparison of PH-2a analogues and other diphenols, the critical roles of H-bonding interactions both in activating reactants and inducing a directional reaction were revealed. These H-bonds with appropriate strengths can self-assembly form and close the distance between potential reaction sites, facilitating the direct production of an adduct. In addition, the application potential of the PH-2a/resorcinol system was also prospected, which can promise network tailoring and low-temperature cross-linking by the design flexibility of PH-2a and resorcinol derivatives, opening up possibilities for the preparation of advanced polybenzoxazine resins at low temperature.

研究领域: 材料科学 · 高分子化学 · 超分子化学
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2022 · IF 24.319

Topologically and chemically engineered conjugated polymer with synergistically intensified electron generation, transfer and utilization for photocatalytic nicotinamide cofactor regeneration

Shihao Li,Yuqing Cheng,Yu Chen,Jing Li,Yiying Sun,Jiafu Shi,Zhongyi Jiang

Electron generation, transfer and utilization in photocatalytic reduction reactions jointly govern the solar-to-chemical conversion efficiency. In natural photosynthesis, the ultrathin thylakoid membrane loads numerous pigments and proteins for light harvesting and electron transfer, which also integrates ferredoxin-NADP + reductase bearing molecule hydrides for electron utilization in NADPH regeneration. Inspired by this, herein, conjugated polymer nanolayer coordinated with (Cp*RhCl 2 ) 2 (CPNL-Rh) is developed through a topological and chemical engineering strategy to synergistically intensify electron generation, transfer and utilization for NADH regeneration. Specifically, the triazine moieties well distributed in CPNL-Rh largely harvest visible light to generate electrons. The electrons are rapidly transferred to Rh cocatalyst through CPNL. Rh cocatalyst finally accepts electrons and protons in solution to form molecule hydrides for implementing NADH regeneration. The turnover frequency of CPNL-Rh for NADH regeneration reaches 44.8 h −1 , among the highest value ever reported and ~346% higher than that of bulk CP with free Rh cocatalyst.

研究领域: 材料科学 · 化学工程 · 光化学 · 催化
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