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FOOD RESEARCH INTERNATIONAL · 2022 · IF 7.425

Trapping of reactive carbonyl species by fiber-bound polyphenols from whole grains under simulated physiological conditions

Jinxin Li,Hao Zhang,Xijuan Yang,Ling Zhu,Gangcheng Wu,Xiguang Qi,Hui Zhang

The carbonyl trapping activity of bound-polyphenol rich insoluble dietary fiber (BP-IDF) from different whole grains and underlying mechanism of these BP-IDF actions were studied under simulated physiological conditions. We found that the black highland barley BP-IDF exhibited the most pronounced effect in scavenging carbonyls by trapping 88.7%, 72.2%, 95.7%, and 31.4% for methylglyoxal, glyoxal, acrolein, and malondialdehyde within 24 h, respectively. After vitro gastrointestinal digestion, the black highland barley BP-IDF still retained considerable trapping activity for carbonyls. The carbonyl scavenging capacity was reduced by up to 93% after removing bound polyphenols from the black highland barley BP-IDF, which was consistent with the reduction in its total phenolic content. Moreover, the formation of adducts between reactive carbonyl species (RCS) and polyphenols bound to insoluble dietary fiber (IDF) was also detected. Overall, these findings confirmed that IDF-bound polyphenols were still active to trap RCS, indicating the potential benefits of BP-IDF from whole grains as functional ingredients to limit carbonyl stress across the gastrointestinal tract.

研究领域: 食品科学 · 营养学 · 生物化学
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Catalysis Science & Technology · 2024 · IF 4.4

“Honeycomb catalytic strategy” for carbonylation reaction based on the structural evolution of cobalt species

Peng Zhang,Liying An,Chunqiu Zhao,Qiang Chang,Fei Wang,Chenghua Zhang,Yulei Zhu,Yong Yang,Yongwang Li

For catalytic carbonylation reactions, the high-cost catalyst recovery process is a huge challenge in industrial applications. Herein, the “honeycomb catalytic strategy” based on the structural evolution of supported cobalt catalysts successfully implements a facile and efficient catalyst recovery in the methoxycarbonylation of propylene oxide. In this strategy, cobalt species mainly exist in the form of homogeneous cobalt carbonyl species and supported cobalt nanoparticles in the reaction and product/catalyst separation stage, respectively, for reconciling catalytic efficiency and metal recovery. Our results demonstrate that catalytic behaviors of supported cobalt catalysts strongly depend on the support materials and the in situ generated cobalt carbonyls. And higher CO partial pressure and lower temperature are conducive to the conversion of metallic cobalt into cobalt carbonyls, while additional post-treatment procedures (removing CO and introducing high temperature) can recover the dissolved cobalt species in the product mixture onto the support. ICP testing proved that the optimal post-treatment process can increase the Co retention ratio of the Co/C catalyst from 45.3% to 98.9%. After four honeycomb catalytic cycles, the Co retention ratio remained at 95.2% with a slight loss of productivity. Meanwhile, for the cobalt-based catalysts with different supports and higher loadings, the post-treatment process also significantly enhanced the Co retention ratio, thereby demonstrating the effectiveness and universality of the “honeycomb catalytic strategy”.

研究领域: 化学工程 · 催化化学
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RESEARCH ON CHEMICAL INTERMEDIATES · 2020 ·Vol. 47 ·期 2 ·663-682 · IF 2.262

Experimental and theoretical investigation on the effect of N-substituent position on the inhibition performance of l-lysine derivatives for carbon steel in H2SO4 solution

Zhu Lin,Zheng Xingwen,Zeng Xianguang,Gong Min,Guo Lei

The inhibitive effect and inhibition mechanism of l -lysine derivatives, namely α- N -benzyloxycarbonyl- l -lysine (α-NL) and ε- N -benzyloxycarbonyl- l -lysine (ε-NL), on the corrosion of carbon steel in 0.5 M H 2 SO 4 solution were investigated by electrochemical technique, weightlessness test, scanning electron microscope, atomic force microscope, infrared attenuated reflectance spectroscopy and quantum chemical calculation. The results showed that α-NL and ε-NL as moderate cathodic inhibitors mainly inhibited the cathodic reaction of carbon steel in 0.5 M H 2 SO 4 solution, and the terminal substituted ε-NL showed better corrosion inhibition than the α- N -benzyloxycarbonyl protected α-NL. Their inhibition efficiencies increased with the increase in inhibitor concentration, and the inhibition efficiency of α-NL and ε-NL with concentration of 10 mmol can reach 53.4% and 61.5%, respectively, but decreased with rising temperature. The adsorption of investigated inhibitors on the surface of carbon steel obeyed the modified Langmuir isotherm and El-Awady thermodynamic-kinetic model, and the thermodynamic and kinetic parameters were determined to discuss the mechanism of inhibition of α-NL and ε-NL. Moreover, Quantum chemical calculation gave further insight into the inhibition mechanism of α-NL and ε-NL and was employed to reveal the reasons for their differences in inhibition performance.

研究领域: 材料科学 · 电化学 · 量子化学
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Catalysts · 2020 ·Vol. 10 ·期 11 ·1304 · IF 3.52

Vapor-Phase Furfural Decarbonylation over a High-Performance Catalyst of 1%Pt/SBA-15

Qiang Yuan,Jifeng Pang,Wenguang Yu,Mingyuan Zheng

A high-performance Pt catalyst supported on SBA-15 was developed for furfural decarbonylation. Compared to Pt catalysts loaded on microporous DeAl-Hbeta zeolite and hierarchical micro-mesoporous MFI nanosheet (NS) materials, the 1%Pt/SBA-15 catalyst afforded notably higher activity, furan selectivity and stability owing to the negligible acid sites and proper mesopores on the SBA-15 support. Among a set of 1%Pt/SBA-15 catalysts bearing Pt nanoparticles (NPs) with sizes of 2.4–4.3 nm, the catalyst with 3.7 nm Pt NPs afforded the highest furan selectivity. Over the optimal catalyst, 88.6% furan selectivity and ca. 90% furfural conversion were obtained at 573 K and a high weight hourly space velocity (WHSV) of 16.5 h−1. Moreover, the reaction temperatures at 440–573 K and the ratios of H2to furfural at 0.79–9.44 did not affect the reaction selectivity notably, showing that the reaction over 1%Pt/SBA-15 can be conducted over a wide range of conditions. The catalyst was stable under the harsh reaction conditions and lasted for 90 h without significant deactivation, demonstrating the superior property of SBA-15 as a catalyst support for furfural decarbonylation.Keywords:decarbonylation;furfural;furan;platinum;SBA-15

研究领域: 催化化学 · 能源化学 · 材料科学
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Materials · 2020 ·Vol. 13 ·期 18 ·4026 · IF 3.057

Study on Rh(I)/Ru(III) Bimetallic Catalyst Catalyzed Carbonylation of Methanol to Acetic Acid

Shasha Zhang,Wenxin Ji,Ning Feng,Liping Lan,Yuanyuan Li,Yulong Ma

In this study, a Rh(I)/Ru(III) catalyst with a bimetallic space structure was designed and synthesized. The interaction between the metals of the bimetallic catalyst and the structure of the bridged dimer can effectively reduce the steric hindrance effect and help speed up the reaction rate while ensuring the stability of the catalyst. X-ray photoelectron spectroscopy (XPS) results show that rhodium accepts electrons from chlorine, thereby increasing the electron-rich nature of rhodium and improving the catalytic activity. This promotes the nucleophilic reaction of the catalyst with methyl iodide and reduces the reaction energy barrier. The methanol carbonylation performance of the Rh/Ru catalyst was evaluated, and the results show that the conversion rate of methyl acetate and the yield of acetic acid are 96.0% under certain conditions. Furthermore, during the catalysis, no precipitate is formed and the amount of water is greatly reduced. It can be seen that the catalyst has good stability and activity.Keywords:carbonylation;acetic acid;bimetallic catalyst

CAS / MDL: 64-19-7 67-56-1 497-19-8
研究领域: 化学工程 · 催化化学
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Energy Storage Materials · 2023 · IF 20.4

Double-chain conjugated carbonyl polymer cathode for rechargeable magnesium batteries: Constructing active sites for reversible storage of bivalent magnesium cations

Xin Ren,Donggang Tao,Shuai Cui,Ting Li,Yuliang Cao,Fei Xu

Rechargeable Mg batteries are advantageous substitutes for lithium-ion batteries in large-scale energy storage with low cost and high safety, but the lack of cathode materials is blocking the development. Organic polymers are promising Mg-storage materials, and the construction of suitable Mg-storage active sites is of great significance for the performance. In the present study, a double-chain conjugated carbonyl polymer is designed and investigated as cathode material of rechargeable Mg batteries. The double-chain structure builds favorable active sites for reversible storage of bivalent Mg 2+ cation by means of immobilization of the two adjacent carbonyls. This double-chain polymer shows a higher Mg-storage capacity (194 mAg –1 ) than the corresponding single-chain polymer (116 mAg –1 ). The Mg-storage capacity of this double-chain polymer also exceeds the Li-storage capacity (106 mAg –1 ) significantly. A mechanism study demonstrates the reversible carbonyl enolization in Mg-storage reactions. A theoretical computation demonstrates the magnesiation structure has a higher HOMO and a lower LUMO energy level, as well as a smaller HOMO–LUMO gap. This is favorable for the Mg-storage reaction reversibility and stability of the magnesiation structure, thus improving the capacities and cycling stabilities. The principle revealed in the present study provides an important insight to design organic conjugated polymers with favorable Mg-storage active sites, which would assist the development of high-performance Mg-storage materials.

研究领域: 材料科学 · 储能 · 电化学 · 聚合物化学
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JOURNAL OF ORGANIC CHEMISTRY · 2022 · IF 4.198

Nickel-Catalyzed Decarbonylative Thioetherification of Carboxylic Acids with Thiols

Tianhao Xu,Xingyu Zhou,Xiong Xiao,Yan Yuan,Long Liu,Tianzeng Huang,Chunya Li,Zhi Tang,Tieqiao Chen

A nickel-catalyzed decarbonylative thioetherification of carboxylic acids with thiols was developed. Under the reaction conditions, benzoic acids, cinnamic acids, and benzyl carboxylic acids coupled with various thiols including both aromatic and aliphatic ones produce the corresponding thioethers in up to 99% yields. Moreover, this reaction was applicable to the modification of bioactive molecules such as 3-methylflavone-8-carboxylic acid, probenecid, and flufenamic acid, and the synthesis of acaricide chlorbenside. These results well demonstrated the potential synthetic value of this new reaction in organic synthesis.

研究领域: 有机化学 · 合成化学
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES · 2025 · IF 8.5

Enhancement of antioxidant, carbonyl scavenging and anti-glycation activities of polysaccharide-based hydrocolloids by covalent grafting with gallic acid

Mianzhang Zhang,Hongliang Li,Fu Liu,Shiyi Ou,Pengzhan Liu,Jie Zheng

Carbonyl stress contributes to pathological disorders leading to the progression of a variety of chronic diseases. Exploration of food ingredients with carbonyl scavenging capacities became one of the most potential strategies for the prevention of these diseases. Polysaccharide-based hydrocolloids have wide application approaches in the food industry. However, the carbonyl scavenging capacity of some natural polysaccharide-based hydrocolloids is unsatisfactory due to structural limitations. In this research, gallic acid (GA) was grafted onto different hydrocolloids (xanthan gum, carrageenan, carboxymethylcellulose, carboxymethyl chitosan (CMCS), and sodium alginate) by a free radical-mediated reaction to improve their antioxidant, carbonyl scavenging, and anti-glycation activities. The antioxidant activity of hydrocolloids was significantly improved after GA grafting. Among them, CMCS-GA (graft ratio 15.45 mg GA/g) exhibited the same ABTS scavenging ability as the equivalent amount of free GA and Vc. The carbonyl scavenging capacity, and the inhibitory effects on the fluorescent advanced glycation end products (AGEs) and protein oxidation products of some hydrocolloids also increased significantly GA grafting. The scavenging capacity of CMCS-GA on MGO, GO, ACR, and MDA in the model reaction increased by 220 %, 100 %, 6 %, and 58 %, respectively. Overall, CMCS-GA showed the best performance in radical scavenging, carbonyl scavenging, and AGEs inhibition compared to all the other hydrocolloids investigated. The findings showed that grafting GA onto hydrocolloids is a viable strategy to enhance the carbonyl scavenging capacity and anti-glycation activity of hydrocolloids.

研究领域: 食品科学 · 生物化学
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JOURNAL OF HAZARDOUS MATERIALS · 2022 · IF 14.224

Graphite (GP) induced activation of ferrate(VI) for degradation of micropollutants: The crucial reduction role of carbonyl groups on GP surface

Mengfan Luo,Heng Zhang,Peng Zhou,Jiali Peng,Ye Du,Zhaokun Xiong,Bo Lai

The sluggish oxidation kinetics of ferrate (Fe(VI)) at neutral and slightly alkaline pH impedes its rapid abatement of micropollutants in practical application. This work discovers that graphite (GP), a metal-free carbonaceous material , can be a promising material to improve the reactivity of Fe(VI) in the pH range of 7.0 − 9.0. The performance of the GP/Fe(VI) process for sulfamethoxazole (SMX) removal was further evaluated via altering the dosages of Fe(VI), GP, and SMX. Probe analysis and quenching experiments identified Fe(IV) and Fe(V) as the primary active species responsible for the removal of organic compounds in the GP/Fe(VI) system. The detailed activation mechanism of GP is discussed via analyzing the surface chemical changes of GP exposed to Fe(VI). It is found that the carbonyl groups on GP surface execute a critical role in Fe(VI) activation. The GP/Fe(VI) system shows powerful anti-interference ability to environmental background substances. Therefore, the new oxidation process proposed in this work holds a great application prospect for contamination remediation. Finally, we discuss the underlying degradation pathways of SMX by the GP/Fe(VI) system. This study not only develops a promising system for the removal of micropollutants but also provides an in-depth insight into the activation mechanism of metal-free carbonaceous material in Fe(VI) oxidation process.

研究领域: 环境科学 · 化学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

An improvement for enrichment and purification of germanium using carbonyl acid extractants

Xilin Geng,Qionghua Xie,Yundong Zhu,Guocheng Yao,Liangshi Wang

Germanium is a strategic metal that is challenging to enrich and purify without any side effects, especially stability and selectivity. Here the role of carbonyl acid in selective separation of germanium from complex industrial liquids was highlighted. Integrating theoretical and experimental analyses, carbonyl acids exhibit strong binding ability and high selectivity to germanium was demonstrated. The first set of carbonyl acid extractant (CAE) for germanium extraction was successfully synthesized with a solubility of less than 50 mg/L at pH = 0. The process analysis exhibits the extraction rate of germanium in a single stage by CAEs exceeds 99.9 %, while the separation factor surpasses 10 3 , far beyond 10 1 of hydroxamic acids. Furthermore, the stripping rate for germanium in a single stage exceeds 83.0 %, with germanium accounting for over 99.9 % of the total metal content in the stripping solution. The CAE extraction process is straightforward and characterized by high germanium separation efficiency. The development of CAE not only realises the stable, green, low-carbon, and high-efficiency purification of germanium, but also the universality and inspiration of CAE make it highly significant and valuable in both theoretical research and practical applications.

CAS / MDL: 126-73-8 1116-76-3
研究领域: 冶金学 · 化学工程 · 材料科学
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SURFACE & COATINGS TECHNOLOGY · 2022 · IF 4.865

Enhancement of oxidation and corrosion resistance of flaky carbonyl‑iron powder via SiO2/KH560/PDMS coating applied with sol-gel

Linbo Zhang,Weihong Wan,Xianyu Jiang,Bo Wang,Liangjun Yin,Simeon Agathopoulos,Jiangliang Xie,Li Zhang,Haipeng Lu,Longjiang Deng

The popular magnetic material of flaky carbonyl iron (FCI) is unfortunately vulnerable to electrochemical corrosion when exposed to a salty and foggy environment. This work reports on a sol-gel method that successfully modifies FCI particles, using lithium silicate (Li 2 SiO 3 ), poly dimethyl siloxane (PDMS), and γ-(2,3-epoxypropoxy) propytrimethoxysilane (KH560), to synthesize Fe@SiO 2 @KH560@PDMS hybrid composite, related to its organic–inorganic hybrid coatings. The favorable hydrophobicity of organic–inorganic hybrid coatings with the static contact angle of 120° impeded the contact between corrosive medium and FCI core. The results of electrochemical experiments also confirmed its excellent corrosion resistance , since the corrosion potential E corr was positively shifted to 0.01 V, and the corrosion current I corr was three orders of magnitude lower than that of the unmodified FCI particles. Thermogravimetric (TG) analysis indicates that the presence of hybrid coatings also improved the thermal stability of the produced material towards oxidation . Furthermore, the results of molecular dynamics simulation reveal that the hybrid layer inhibits the diffusion of corrosive medium.

CAS / MDL: 7664-38-2
研究领域: 材料科学 · 电化学 · 表面工程
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ACS Sustainable Chemistry & Engineering · 2022 · IF 9.224

Synthesis of Oxygen-Containing Precursors of Aviation Fuel via Carbonylation of the Aqueous Bio-oil Fraction Followed by C–C Coupling

Jiayuan Sun,Shanshan Shao,Xinggang Hu,Xiaohua Li,Huiyan Zhang

The aqueous fraction of bio-oil from biomass fast pyrolysis mainly contains low-molecular-weight oxygenates such as carboxylic acids, ketones, aldehydes, phenols, and furans. In this study, the full components of aqueous bio-oil are directionally converted into carbonyl groups such as aldehydes and ketones, and then the oxygen-containing precursors of aviation fuel are prepared through coupling, focusing on exploring the mechanism of carbonylation and C–C coupling. Studies have revealed that propionic acid, furfural, and phenol can be directionally converted into ketones, in which reaction 3-pentanone, cyclopentanone, and cyclohexanone were formed via ketonization and hydrogenation in the aqueous phase. Then the two components of 3-pentanone, cyclopentanone, cyclohexanone, acetone, and acetaldehyde were subjected to aldol condensation to explore the C–C coupling mechanism in the preparation of the C7–C18 precursor of aviation fuel. The mechanism in the high-quality utilization of all components of the aqueous phase bio-oil fraction was explored, which was favorable for the synthesis of biomass-based aviation fuel.

研究领域: 化学工程 · 可再生能源 · 生物质转化
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