CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Liangdong Hu,Lian-hua Xu,Chenjun Yang,Longfei Hong,Kai Wu,Sheng Chu,Longlong Ma,Shurong Wang,Rui Xiao,Huiyan Zhang
Lewis acid sites (LASs) are essential for the photocatalytic isomerization of biomass into high-value platform compounds. However, transient changes in the number of LASs in a photocatalytic system have not been clearly documented, often resulting in an inaccurate understanding of their role in isomerization. To address this challenge, in this study, the molecular probes glyceraldehyde was isomerized to 1,3-dihydroxyacetone (DHA, 63.5 % yield , 3 h) and fructose (47.9 % yield , 3 h) on Pt–KC 3 N 4 , with concurrent production of H 2 (233.8 μmol g −1 ). The results of in situ NH 3 –temperature-programmed desorption (TPD) characterization demonstrated that light irradiation induced the formation of transient LASs on Pt–KC 3 N 4 , and the density of acid sites observed in this study differed significantly from that observed in offline data. Furthermore, theoretical calculations demonstrated that photothermal electron redistribution on Pt–KC 3 N 4 is the main factor driving this transient LAS formation. This report describes a unique methodology to explore transient acid sites in isomerization reactions and provides insight into potential applications in the field of photocatalytic biomass valorization.
研究领域:
化学
·
可再生能源
·
生物质转化
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DOI
高影响因子
BIOORGANIC CHEMISTRY
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2020
·
IF 4.831
Ibrahim Khalifa,Du Xia,Kunal Dutta,Jinmeng Peng,Yangyang Jia,Chunmei Li
Advanced glycation end-products (AGEs), which instigate many disorders, are mostly mediated by dicarbonyl rearrangements. We studied the corresponding mechanisms of the anti-glycation effects of two anthocyanins purified from mulberry fruits, namely cyanidin 3-glucoside (C3G) and cyanidin 3-rutinoside (C3R), on glycated β-lactoglobulins (β-Lg). Both mulberry anthocyanins (MAs) inhibited the AGEs-formation in a dose-dependent manner, but the effect of C3R was significantly stronger than that of C3G (p < 0.05). MAs inhibited AGEs-formation by selectively trapping dicarbonyls, especially glyoxal. The UPLC-ESI-Q-TOF-MS results characterized that C3R formed mono- and di-glyoxal adducts, where C3G only created di-glyoxal adducts. Additionally, C3R could directly interact with some of the glycation sites of β-Lg. Overall, GO-trapping and β-Lg-MAs covalent/noncovalent binding are disclosed as the key mechanisms of the anti-AGEs activity of MAs on β-Lg, which could be valorised as effectual AGEs inhibitors in proteins-rich matrices.
研究领域:
食品科学
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生物化学
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DOI
高影响因子
Journal of Environmental Sciences
·
2025
·
IF 6.3
Kun Liu,Tao Wang,Guohua Zhang,Wei Sun,Ye Yang,Mingjin Tang,Xinming Wang,Xinhui Bi
Aqueous-phase reactions between carbonyls and reduced nitrogen compounds play a considerable role in the formation of secondary organic aerosols and brown carbon in the atmosphere. However, the reported reaction rate constants for these reactions have largely been limited to bulk aqueous-phase simulations, which may not accurately represent the real state of atmospheric cloud droplets. We employed an integration of optical tweezers and Raman spectroscopy to manipulate and analyze simulated cloud droplets (size range 8000-10000 nm), comprising a mixture of glyoxal and ammonium sulfate. This approach enabled us to delve into the intricate realm of their reaction kinetics at individual droplet level mimicking cloud droplets. Raman spectroscopy provided high temporal resolution (20 s) measurements of the changes in the amount of nitrogen-containing organics (or NOCs as represented by the C-N bond) within the droplets. The results indicate that the reaction follows first-order kinetics throughout the monitoring over 80-400 minutes. The average reaction rate constant for the formation of NOCs within the single droplet was determined to be (6.77 ± 0.98) × 10 -5 s -1 , up to three orders of magnitude higher than those through the bulk aqueous-phase simulations, especially at lower pH levels. Additionally, the reaction rate constant in single droplet increases with increasing pH, consistent with the trend previously reported for the aqueous-phase simulations. The results highlight the difference of the reaction rate constant between bulk aqueous phase and droplets, which would improve our understanding on the formation and impacts of secondary organic aerosols and brown carbon in atmospheric aqueous phase.
研究领域:
大气科学
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化学动力学
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产品关联
DOI
PubMed
高影响因子
FOOD CHEMISTRY
·
2020
·
IF 6.306
Xiao-Yuan Wang,Yun-Jiao Ma,Yu Guo,Xiao-Lin Luo,Ming Du,Liang Dong,Pei Yu,Xian-Bing Xu
2-Acetylthiazole possesses a nutty, cereal-like and popcorn-like aroma and a low odor threshold, and this compound has been identified in some processed foods, while the formation pathway of 2-acetylthiazole has not been clearly elucidated. Here, a model reaction of d -glucose and l -cysteine was constructed to investigate the formation pathway of 2-acetylthiazole. l -Cysteine, d -glucose and the corresponding intermediates, namely, dicarbonyl compounds (DCs), were involved in the formation of 2-acetylthiazole and detected by high-performance liquid chromatography with tandem mass spectrometry (HPLC-MS/MS), high-performance ion chromatography (HPIC) and HPLC, respectively. The carbon module labeling (CAMOLA) technique revealed that the C-4 and C-5 of 2-acetylthiazole were derived from the carbons of glucose. The potential of glyoxal, which is degraded by glucose, to form 2-acetylthiazole was revealed for the first time. A novel route to form 2-acetylthiazole by the reaction of glyoxal and methylglyoxal produced by d -glucose with H 2 S and NH 3 produced by l -cysteine was proposed.
研究领域:
食品科学
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生物化学
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DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2014
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IF 4.331
Bo Li,Lijian Ma,Yin Tian,Xiaodan Yang,Juan Li,Chiyao Bai,Xiaoyu Yang,Shuang Zhang,Shoujian Li,Yongdong Jin
We proposed a new approach for preparing an efficient uranium-selective solid phase extractant (HTC-btg) by choosing bayberry tannin as the main building block and especially glyoxal as crosslinking agent via a simple, economic, and green one-pot hydrothermal synthesis. The results of characterization and analysis show that after addition of glyoxal into only bayberry tannin-based hydrothermal reaction system, the as-synthesized HTC-btg displayed higher thermal stability, larger specific surface area and more than doubled surface phenolic hydroxyl groups. The sorption behavior of the sorbents toward uranium under various conditions was investigated in detail and the results indicated that the process is fast, endothermic, spontaneous, and pseudo-second-order chemisorption. The U(VI) sorption capacity reached up to 307.3 mg g −1 under the current experimental conditions. The selective sorption in a specially designed multi-ion solution containing 12 co-existing cations over the range of pH 1.0–4.5 shown that the amount of uranium sorbed accounts for about 53% of the total sorption amount at pH 4.5 and distinctively about 85%, unreported so far to our knowledge, at pH 2.0. Finally, a possible mechanism involving interaction between uranyl ions and phenolic hydroxyl groups on HTC-btg was proposed.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
PubMed
高影响因子
Journal of Physical Chemistry C
·
2023
·
IF 3.7
Ernest Pahuyo Delmo,Yian Wang,Shangqian Zhu,Tiehuai Li,Yinuo Wang,Juhee Jang,Qinglan Zhao,Alexander Perez Roxas,Gabriel Sikukuu Nambafu,Zhengtang Luo,Lu-Tao Weng,Minhua Shao
The C2 product formation mechanism in the electrochemical reduction reaction of CO2 (CO2RR) is still poorly understood. This work aims to analyze the copper-catalyzed electroreduction of aqueous glyoxal to understand its role as a potential reaction intermediate during CO2RR. Multiple reaction pathways are observed during glyoxal reduction, including its electroreduction to ethanol and ethylene glycol, disproportionation to glycolate and formate, and further coupling toward the formation of C4 compounds and graphitic carbon. A significantly high ethylene glycol to ethanol ratio indicates that glyoxal may not be the main intermediate toward ethanol production in CO2RR on Cu, contradicting previous hypotheses. Density functional theory calculations show that the hydration of aldehyde functional groups can shift the ethylene glycol vs ethanol selectivity, in which the former is preferred when the carbonyl groups remain unhydrated. A CO2-to-glycolate pathway is also possible as a consequence of the base-catalyzed internal Cannizzaro disproportionation of glyoxal. Finally, C–C coupling during glyoxal reduction may open up a CO2RR pathway toward C4 products such as tetroses and 1,4-butanediol that have not been previously observed in electrochemical CO2RR. The formation of graphitic carbon also suggests that the carbon deposits usually observed during CO2RR may originate from glyoxal-derived C–C coupling. Our findings offer valuable insights onto the glyoxal pathway of CO2RR and the various multicarbon products that result from the further conversion of glyoxal.
研究领域:
化学
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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
CHINESE JOURNAL OF CATALYSIS
·
2025
·
IF 17.7
Zhenghao Mao,Wenjing Xu,Na Han,Yanguang Li
Aldehydes are valuable intermediates with widespread industrial applications, and their traditional synthesis relies on chemical oxidation that is often hazardous and environmentally unfriendly. Electrochemical oxidation offers a more sustainable and milder alternative; however, it faces challenges such as aldehyde overoxidation and susceptibility to base-catalyzed Cannizzaro disproportionation. Electrochemical glycerol oxidation to glyceraldehyde is a representative example, which typically requires precious metal-based electrocatalysts but still suffers from low selectivity and activity. Here, we report a metal-free oxidation strategy mediated by 2,2,6,6-tetramethylpiperidine-1-oxyl. By systematically investigating the redox thermodynamics and kinetics of TEMPO across a broad pH range, we construct a Pourbaix diagram and elucidate the relative kinetics of each reaction step. These insights allow us to explain the anomalously high apparent Faradaic efficiency (~200%) observed under acidic conditions, and identify neutral media as the optimal environment for selective glyceraldehyde production. Under optimized conditions, our system achieves a glyceraldehyde Faradaic efficiency exceeding 93% and a partial current density of 23.3 mA cm –2 at 0.57 V — more than doubling the performance of the best reported precious metal-based systems. Furthermore, the versatility of this strategy extends to the selective oxidation of other primary alcohols to their corresponding aldehydes with near-unity selectivity.
研究领域:
电化学
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有机合成
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催化化学
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绿色化学
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能源化学
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分子催化
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工业化学
✓ 已验证
产品关联
DOI
高影响因子
Biotechnology Journal
·
2024
·Vol. 19
·期 9
·2400360
·
IF 3.2
Yue Yan,Haodong Zhao,Dingyu Liu,Jie Zhang,Yuwan Liu,Huifeng Jiang
Global climate deterioration intensifies the demand for exploiting efficient CO 2 utilization approaches. Converting CO 2 to biorefinery feedstock affords an alternative strategy for third-generation biorefineries. However, upcycling CO 2 into complex chiral carbohydrates remains a major challenge. Previous attempts at sugar synthesis from CO 2 either produce mixtures with poor stereoselectivity or require ATP as a cofactor. Here, by redesigning glycolaldehyde synthase, the authors constructed a synthetic pathway for biorefinery feedstock D-xylulose from CO 2 that does not require ATP as a cofactor. The artificial D-xylulose pathway only requires a three-step enzyme cascade reaction to achieve the stereoselective synthesis of D-xylulose at a concentration of 1.2 g L −1 . Our research opens up an alternative route toward future production of chemicals and fuels from CO 2 .
研究领域:
生物技术
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生物化学
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环境科学
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化学工程
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产品关联
DOI
PubMed
高影响因子
Sustainable Energy & Fuels
·
2022
·Vol. 6
·期 10
·2602-2612
·
IF 6.813
Haosheng Xin,Haiyong Wang,Song Li,Xiaohong Hu,Chenguang Wang,Longlong Ma,Qiying Liu
Catalytic conversion of renewable cellulose, instead of fossil resources, to high-value ethylene glycol (EG) is of great significance for reducing considerable worries regarding the energy problem. However, the EG production from cellulose is dependent on Ni and Ru based catalysts. Herein, encapsulated Co@C catalyst was firstly applied for EG production from cellulose combined with tungstic acid (TA). The mixing of the two catalysts in different ratios was compared and well-controlled, and the highest 67.3% yield of EG can be achieved. TA is used mainly to promote both the cellulose hydrolysis and the retro-aldol reaction of glucose to glycolaldehyde. Co@C catalysts are responsible for the hydrogenation of glycolaldehyde to EG. Compared with traditional noble metals and composite catalysts, the inexpensive and easily synthesized Co@C catalysts could greatly reduce the cost of production of EG. The Co@C catalysts encapsulated with outside graphene layers can keep high stability for at least 6 runs.
研究领域:
化学工程
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催化
·
可再生能源
·
材料科学
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产品关联
DOI
高影响因子
Open Chemistry
·
2016
·Vol. 14
·期 1
·279-286
·
IF 0
Jian Feng,Wei Xiong,Hao Ding,Bai He
The hydrogenolysis of glycerol was performed over a Pt/C catalyst in combination with several alkali metal hydroxides and their salts. LiOH was found to be an effective promoter for the selective hydrogenolysis of glycerol to 1,2-propanediol. Hydroxyl ions are the main factor to promote the reaction process by dehydration of the glyceraldehyde intermediate. Lithium ions play a role in assisting the dehydrogenation of glycerol to glyceraldehyde, because they have the right size to coordinate with the alkoxide species. A possible surface reaction mechanism involving the participation of lithium ions was proposed to account for the results obtained in the study.
研究领域:
催化
·
化学工程
·
无机化学
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产品关联
DOI
FUEL
·
2024
·
IF 6.7
Xing Wei,Qingqiang Wang,Xunli Zhang,Ying Chen,Nan Jin,Yuchao Zhao
The process of converting glucose into formic acid (FA) has been explored as a promising route for using biomass as a renewable feedstock for green chemical manufacturing. However, the most commonly used batch-tank reactor systems currently suffer from several drawbacks, including extended processing time, limited product selectivity, and high energy consumption, while the underlying reaction paths have been poorly understood. In this work, a continuous flow microchannel reactor was employed for the glucose conversion catalyzed by H 5 PV 2 Mo 10 O 40 with O 2 as an oxidant. The influence of various parameters on the conversion rate of glucose and the FA yield was characterized. Experimental results indicated that with a residence time of less than 3 min, the glucose was completely converted, and the highest FA yield reached 82.40 %. Extensive examination on the apparent by-products revealed that most of them acted as intermediates to produce FA through various pathways, including glyoxal, glyceraldehyde and glycolaldehyde as key intermediates for the oxidation of glucose to FA. Furthermore, the density functional theory (DFT) method was used to determine the bond energies of different C–C bond cleavage modes of substrate glucose and fructose produced by the isomerization of glucose. Experimentally, the conversion of three main intermediates and some other possible intermediates and their FA yield were measured with different residence time. It was also found that the CO 2 was produced through the decarboxylation of α-hydroxy and α-carbonyl carboxylic acid compounds, while the aldehyde groups in the compounds were more likely converted to FA by the α-carbon bond cleavage. Finally, plausible reaction pathways were proposed for the process of glucose-to-FA catalyzed by HPA-2, providing useful guidance for the identification of side reaction pathways and further improvement of FA yield.
研究领域:
化学工程
·
绿色化学
·
催化
·
反应工程
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产品关联
DOI
高影响因子
ChemPhotoChem
·
2022
·Vol. 6
·期 8
·e202200067
·
IF 3.679
Yaoqiang Wang,Yu Jin,Zishuai Wang,Gang Xiao,Haijia Su
Graphical Cascading : A two-pot, light-dark cascade NADH regeneration procedure was developed. First, g-C 3 N 4 nanosheets photocatalyzed the conversion of triethanolamine (TEOA) to glycolaldehyde, which reduced NAD+ to NADH in the dark reaction step, thus avoiding the photo-deactivation of NADH. Photocatalytic regeneration of NAD(P)H is a green and promising method which utilizes clean solar energy. However, we found in this study that light exposure of NADH will cause the deactivation of the regenerated NADH. Therefore, we used ultrathin g-C 3 N 4 nanosheets as photocatalyst and developed a two-pot light-dark cascade procedure for NADH regeneration to avoid the light exposure and the deactivation of NADH. This two-pot procedure included a first light reaction step where triethanolamine was converted to glycolaldehyde through visible light photocatalysis which could reduce NAD + to NADH through a non-catalytic process in the followed dark reaction step. Using this procedure, the NADH productivity reached 1.625 mmol ⋅ h −1 ⋅ g −1 and was about 29 times higher that obtained in the one-pot method. The regenerated NADH using the two-pot procedure could act as cofactor of alcohol dehydrogenase to catalyze the reduction of acetaldehyde, illustrating the application potential of this procedure to aid enzyme catalyzed redox reactions.
研究领域:
化学
·
材料科学
·
生物技术
·
环境科学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）