FUEL
·
2021
·
IF 6.609
Ruru Zhou,Yuanyuan Jiang,Huaiyuan Zhao,Boyong Ye,Lina Wang,Zhaoyin Hou
Acetalization of glycerol with acetone could convert surplus glycerol into an important fuel additive (solketal). In this work, a stable solid acid catalyst was synthesized in a facile polycondensation of p -phenolsulfonic acid on KH560 modified SiO 2 (PSF/K-SiO 2 ) and used in the acetalization of glycerol at room temperature. Characterization results confirmed that PSF/K-SiO 2 possessed larger surface area and surface acidity than that of PSF resin (copolymer of p -phenolsulfonic acid and formaldehyde) and non-modified SiO 2 supported PSF resin (PSF/SiO 2 ). As a result, PSF/K-SiO 2 was extremely active and stable in the acetalization of glycerol. At 25 °C, the detected conversion of glycerol reached 86.3% with a 97.7% selectivity of solketal at 1.5 h. The best yield of solketal over PSF/K-SiO 2 could reach 93.1 g-solketal/g-cat/h, and PSF/K-SiO 2 could be recycled at least 5 times without obvious decrease in reactivity.
研究领域:
化学工程
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2021
·
IF 5.706
Qingting Zhang,Andreas Goldbach,Na Ta,Wenjie Shen
Hexagonal molybdates ( h-MoO 3 ) include abundant Mo vacancies that are charge-compensated by cations residing within one-dimensional channels. Hence, they present an intriguing structural motif for Mo catalysis which has been hardly explored for selective oxidation of olefins. We discovered that NH 4 + and Ag + -exchanged h-MoO 3 display surprisingly varied behavior during propylene oxidation. Acrolein and acrylonitrile are the main partial oxidation products with the latter forming due to NH 4 + consumption. The catalytic activity more than doubles upon introduction of Ag + which also enhances selectivity for the main products up to ∼60 %. Unexpectedly, the hexagonal frameworks transform into orthorhombic α-MoO 3 40−60 °C below their reported stability limits already. In addition, Ag 2 Mo 4 O 13 and Ag nanoparticles segregate in case of Ag + -containing h-MoO 3 frameworks. The resulting Ag/Ag 2 Mo 4 O 13 /α-MoO 3 composites catalyze propylene conversion into acrolein with even higher selectivity (∼80 %). Detailed analyses indicate that Ag 2 Mo 4 O 13 drives formation of this oxygenate over these composites.
研究领域:
催化化学
·
材料科学
·
无机化学
✓ 已验证
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2016
·
IF 5.267
Shuangshuang Jing,Xuefei Cao,Linxin Zhong,Xinwen Peng,Xiaoting Zhang,Sha Wang,Runcang Sun
Converting cellulose to renewable energies and chemicals is the most promising and sustainable route to solving the crisis of fossil fuel resources. Up to now, however, it is still a big challenge to effectively transform recalcitrant cellulose into targeted compounds. For the first time, this study proposes a new and highly effective catalysis system with a synergy effect to convert cellulose into formic acid and levulinic acid simultaneously by using in situ carbonic acid from CO2 as a green acid in the presence of CrCl3. The synergy effect of in situ carbonic acid and CrCl3 could highly effectively hydrolyze cellulose to glucose, isomerize glucose to fructose, dehydrate fructose to HMF, and rehydrate HMF to formic acid and levulinic acid in a one-pot way. Here, 49% formic acid and 32% levulinic acid could be obtained from cellulose at a moderate condition. Our results demonstrated that this new catalysis system is comparable to other catalysis systems, and in situ carbonic acid can be used as a low-cost acid to replace mineral acids such as H2SO4, HCl, and H3PO4 and organic acids such as C6H6O3S, H2C2O4, and Cl3CCOOH to constitute novel, highly effective, low-cost, and less environmental impact catalysis systems for producing formic acid and levulinic acid from cellulose.
研究领域:
生物化学
·
可再生能源
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
·
2024
·
IF 8
Lingyan Ma,Di Wu,Lianzhe Hu,Rui Xiao,Kanglin Pei,Wenjing Qi
Phenylglyoxylic acid (PGA) as styrene metabolite is an indicator of styrene occupational exposure. In this work, a novel anodic and cathodic dual-emitting electrochemiluminescence (ECL) ratiometric method for PGA detection is developed using persulfate (S 2 O 8 2- ) and silver metal organic frameworks (Ag-MOFs) amplification strategy. PGA can enhance anodic ECL intensity of Ru(bpy) 3 2+ /PGA system nearly 2 times and cathodic ECL intensity nearly 16 times. S 2 O 8 2- and Ag-MOFs as co-reactant accelerators promote redox reaction of PGA and enhance ECL intensity. Ag + can catalyze S 2 O 8 2- to produce SO 4 ·- , which can convert Ag + to Ag 2+ . Furthermore, SO 4 ·- can accelerate the transformation of Ag + generating more Ag 2+ . Compared with Ru(bpy) 3 2+ system, cathodic ECL intensity of Ru(bpy) 3 2+ /K 2 S 2 O 8 /Ag-MOFs/PGA system gets enhanced nearly 170 times and anodic ECL intensity gets enhanced nearly 6 times. First electro-reduction and then electro-oxidation using scanning potential direction of 0→− 1.3 V→1.4 V→0 also simultaneously enhanced cathodic and anodic ECL nearly 2 times. Thus this ECL ratiometric method for PGA detection has high sensitivity with LOD of 0.8 nM and rapid response once PGA is added in an instant (several seconds). More importantly, anodic and cathodic dual-emitting improves selectivity and avoid interference in complex detection.
研究领域:
分析化学
·
环境科学
·
职业健康
✓ 已验证
产品关联
DOI
高影响因子
ACS Catalysis
·
2023
·
IF 12.9
Yingying Cheng,Wenjing Xu,Jing Hou,Peng Kang
The electrosynthesis of multi-carbon chemicals such as glyoxylic acid (GX) and glycolic acid (GC) from oxalic acid (OA) offers a feasible pathway to achieve sustainable chemical production, especially when coupled with the electroreduction of CO2 to form OA. Here, we demonstrate a series of gallium tin oxide catalysts for selective, controlled OA electroreduction to GX and GC in acidic media. The product distribution can be tuned by changing the reaction temperatures. At room temperature using the GaSnOx/C catalyst, GX can be obtained with a GX Faradaic efficiency (FEGX) of 92.7% at −0.7 V vs RHE and a GX current density (jGX) of −100.2 mA cm–2. At a raised temperature of 80 °C using the GaSnOx/C catalyst, a GC Faradaic efficiency (FEGC) of 91.7% at −0.8 V vs RHE can be obtained. The accelerated OA electroreduction results from the Ga/Sn synergy in the catalysts. A proper Ga/Sn ratio not only enriches OA adsorption and enhances surface binding of intermediates, but also ensures catalyst stability in acidic media.
研究领域:
化学工程
·
材料科学
·
可持续化学
✓ 已验证
产品关联
DOI
高影响因子
Science Advances
·
2025
·Vol. 11
·期 27
·
IF 12.5
Haichao Li,Deqiang Li,Yuan He,Chaobing Luo,Wu Lan,Arthur J. Ragauskas,Tingting You,Feng Xu
Highly efficient conversion of lignin into value-added chemicals and materials is trapped in the inevitable cleavage of β-O-4 linkages and formation of highly condensed structures with deep colors during lignin isolation. Here, we develop a trifunctional choline chloride/glyoxylic acid (ChCl/GA) binary deep eutectic solvent with a π-π conjugate structure and moderate acidity for the fast isolation of light-colored lignin with near proto-structures (exceeding 88% of delignification ratio for 1 hour). The synergetic interaction of GA and ChCl substantially reduced Gibbs free energy of acetal reaction and thoroughly captured reactive intermediates, precisely activating the following key functions: stabilizing β-O-4 linkages, inhibiting condensation reaction, and shielding –OH groups. These enabled efficient isolation of uncondensed, abundant β-O-4 linkage (45.80/100 C9; 79% retention) and light-colored lignin. A near-theoretical yield of aromatic monomers upon depolymerization and high performances as adhesives for lignocellulosic bioplastics were achieved. This work unleashes the valorization potential of lignin by a relatively green and fast strategy for sustainable biorefineries.
研究领域:
化学工程
·
材料科学
·
绿色化学
·
生物技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
·
2018
·
IF 3.412
Cun-Duo Tang,Hong-Ling Shi,Jian-He Xu,Zhu-Jin Jiao,Fei Liu,Peng-Ju Ding,Hong-Fei Shi,Lun-Guang Yao,Yun-Chao Kan
d-Mandelate dehydrogenase (DMDH) has the potential to convert d-mandelic acid to phenylglyoxylic acid (PGA), which is a key building block in the field of chemical synthesis and is widely used to synthesize pharmaceutical intermediates or food additives. A novel NAD+-dependent d-mandelate dehydrogenase was cloned from Lactobacillus harbinensi (LhDMDH) by genome mining and expressed in Escherichia coli BL21. After being purified to homogeneity, the oxidation activity of LhDMDH toward d-mandelic acid was approximately 1200 U·mg–1, which was close to four times the activity of the probe. Meanwhile, the kcat/Km value of LhDMDH was 28.80 S–1·mM–1, which was distinctly higher than the probe. By coculturing two E. coli strains expressing LhDMDH and LcLDH, we developed a system for the efficient synthesis of PGA, achieving a 60% theoretical yield and 99% purity without adding coenzyme or cosubstrate. Our data supports the implementation of a promising strategy for the chiral resolution of racemic mandelic acid and the biosynthesis of PGA.
研究领域:
生物化学
·
生物技术
·
酶学
·
微生物学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Cunhao Du,Wenlu Sang,Chu Xu,Zhiyun Jiang,Jiajia Wang,Yuanyi Fang,Chengjie Zhu,Jakpa Wizi,Muhammad Asif Akram,Lixiao Ni,Shiyin Li
Artemisinin sustained-release microspheres (ASMs) have been shown to inhibit Microcystis aeruginosa ( M. aeruginosa ) blooms. Previous studies have focused on inhibitory mechanism of ASMs on the physiological level of M. aeruginosa , but the algal inhibitory mechanism of ASMs has not been comprehensively and profoundly revealed. The study proposed to reveal the toxicity mechanism of ASMs on M. aeruginosa based on transcriptomics and metabolomics. After exposure to 0.2 g·L −1 ASMs for 7 days, M. aeruginosa biomass was significantly inhibited, with an inhibition rate (IR) of 47 % on day 7. Transcriptomic and metabolomic results showed that: (1) 478 differentially expressed genes (DEGs) and 251 differential metabolites (DMs) were obtained; (2) ASMs inhibited photosynthesis by blocking photosynthetic pigment synthesis, destroying photoreaction centers and photosynthetic carbon reactions; (3) ASMs reduced L -glutamic acid content and blocked glutathione (GSH) synthesis, leading to an imbalance in the antioxidant system; (4) ASM disrupted nitrogen metabolism and the hindered synthesis of various amino acids; (5) ASMs inhibited glyoxylate cycle and TCA cycle. This study provides an important prerequisite for the practical application of ASMs and a new perspective for the management of harmful algal blooms (HABs).
研究领域:
环境科学
·
毒理学
·
分子生物学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
·
2019
·
IF 3.571
Cun-Duo Tang,Peng-Ju Ding,Hong-Ling Shi,Yuan-yuan Jia,Mao-zhi Zhou,Hui-lei Yu,Jian-He Xu,Lun-Guang Yao,Yun-Chao Kan
Phenylglyoxylic acid (PGA) are key building blocks and widely used to synthesize pharmaceutical intermediates or food additives. However, the existing synthetic methods for PGA generally involve toxic cyanide and complex processes. To explore an alternative method for PGA biosynthesis, we envisaged cascade biocatalysis for the one-pot synthesis of PGA from racemic mandelic acid. A novel mandelate racemase named ArMR showing higher expression level (216.9 U·mL–1 fermentation liquor) was cloned from Agrobacterium radiobacter and identified, and six recombinant Escherichia coli strains were engineered to coexpress three enzymes of mandelate racemase, d-mandelate dehydrogenase and l-lactate dehydrogenase, and transform racemic mandelic acid to PGA. Among them, the recombinant E. coli TCD 04, engineered to coexpress three enzymes of ArMR, LhDMDH, and LhLDH, can transform racemic mandelic acid (100 mM) to PGA with 98% conversion. Taken together, we provide a green approach for one-pot biosynthesis of PGA from racemic mandelic acid.
研究领域:
化学工程
·
生物技术
·
有机化学
·
酶学
✓ 已验证
产品关联
DOI
PubMed
高影响因子