GREEN CHEMISTRY
·
2015
·Vol. 17
·期 7
·3992-3999
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IF 8.02
Shujing Zhu,Xiaoqiang Ma,Erzheng Su,Dongzhi Wei
From an environmental perspective, utilizing nonconventional solvents (i.e. green solvents) with low ecological footprints is a highly beneficial alternative to using conventional organic solvents to form a reaction system. The nitrile hydratase (NHase, EC 4.2.1.84) catalyzed hydration of 2-amino-2,3-dimethylbutyronitrile (ADBN) to 2-amino-2,3-dimethylbutyramide (ADBA) in various green solvent–aqueous reaction systems was investigated in this study. After systematically optimizing the reaction conditions, the HFE-7100/H2O (v/v, 10%) biphasic system was ultimately identified as a promising reaction system for reducing product inhibition, avoiding substrate hydrolysis, and facilitating product separation and solvent recovery. The average ADBA yield of an entire batch reaction was 97.3%, which is obviously higher than those obtained with previously reported chemical or enzymatic methods. This is the first attempt to apply a fluorous solvent–aqueous biphasic system to a biocatalytic process, and the results suggest that the fluorous solvent employed in the biphasic system satisfies the requirements for green chemistry.
研究领域:
生物化学
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环境科学
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绿色化学
✓ 已验证
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2025
·
IF 3.9
Liuxing She,Lei Peng,Hang Yuan,Tianrong Zhu,Qiang Fu,Zaikun Wu
The absorption kinetics of CO2 into a novel nonaqueous mixture of 2-amino-2-methyl-1-propanol (AMP) and piperazine (PZ) was studied at atmospheric pressure. The effects of AMP/PZ molar ratio, total concentration, absorption temperature, and inlet flow rate were discussed. The results showed that the composite absorbent with an AMP/PZ ratio of 6:4 had a good effect on the CO2 absorption at 293 K. Unlike relevant reports at home and abroad, the solubility of CO2 in the 1-pentanol solution of AMP and PZ (AMP-PZ-Pentanol) was calculated based on a solution rule model and relevant data from Aspen Plus. The absorption kinetics of CO2 into nonaqueous composite absorbent was analyzed by a double stirred-cell absorber. It shows the enhancement factor increases with the increasing of total concentration but decreases with the increasing of absorption temperature. The absorption mechanism of CO2 in AMP-PZ-Pentanol was determined to be the formation of carbamate by FT-IR, 13C NMR, and XRD analysis. Based on the vapor–liquid equilibrium theory, the reaction heat of CO2 into the phase change absorbent was calculated to be 9.30 KJ mol–1. The results show that the composite absorbent has a lower reaction heat than any single component in it. The desorption experiment of saturated solution shows that the composite absorbent can be completely regenerated in a short period of time, which meets the industrial requirements for CO2 absorbents and will provide a theoretical basis for further industrial applications of this type of absorbent.
研究领域:
化学工程
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环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of CO2 Utilization
·
2022
·
IF 8.321
Mengmeng Ma,Yuchen Liu,Yuli Chen,Guohua Jing,Bihong Lv,Zuoming Zhou,Shihan Zhang
The large-scale deployment of non-aqueous amine solution for carbon dioxide (CO 2 ) capture is mainly limited by its high viscosity, even insoluble substances in saturated solution, which may result in equipment fouling and pipeline blockage. To avoid this problem, the polyamine 1,5-diamino-2-methyl-pentane (DA2MP) was screened as the main absorbent to ensure the high absorption load. While 2-amino-2-methyl-1-propanol (AMP) was used as the regulator to reduce the viscosity and eliminate insoluble substances, which dissolved in n-propanol (PrOH) to from the novel non-aqueous absorbent for CO 2 capture. The CO 2 absorption load of the novel absorbent was 0.95 mol·mol −1 , and the viscosity of saturated solution was only 15.00 mPa·s, remarkably lower than that of the solution without AMP regulation. The solution maintained 97% of its initial CO 2 absorption capacity after fourth regeneration cycle. The regulation mechanism was investigated using 13 C nuclear magnetic resonance (NMR) and quantum chemical calculations. It was proved that a strong and dense hydrogen bond network between DA2MP-carbamates was formed due to the self-deprotonation process, leading to insoluble products in the saturated DA2MP/PrOH solution. Through AMP regulation, there was another type of DA2MP-carbamates deprotonated by AMP formed in the solution with less hydrogen bond network, which could further react with PrOH to produce alkyl carbonates, achieving the elimination of insoluble products and reducing viscosity. Overall, the total regeneration energy consumption was 1.86 GJ·ton −1 CO 2 , only 50.27% of that of the benchmark monoethanolamine (MEA)-based solution, which would be a promising candidate for CO 2 capture.
研究领域:
化学工程
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED AND ENVIRONMENTAL MICROBIOLOGY
·
2017
·Vol. 83
·期 10
·
IF 3.807
Yaojie Gao,Gudan Xu,Pan Wu,Jin Liu,You-sheng Cai,Zixin Deng,Wenqing Chen
2′-Chloropentostatin (2′-Cl PTN, 2′-chloro-2′-deoxycoformycin) and 2′-amino-2′-deoxyadenosine (2′-amino dA) are two adenosine-derived nucleoside antibiotics coproduced by Actinomadura sp. strain ATCC 39365. 2′-Cl PTN is a potent adenosine deaminase (ADA) inhibitor featuring an intriguing 1,3-diazepine ring, as well as a chlorination at C-2′ of ribose, and 2′-amino dA is an adenosine analog showing bioactivity against RNA-type virus infection. However, the biosynthetic logic of them has remained poorly understood. Here, we report the identification of a single gene cluster (ada) essential for the biosynthesis of 2′-Cl PTN and 2′-amino dA. Further systematic genetic investigations suggest that 2′-Cl PTN and 2′-amino dA are biosynthesized by independent pathways. Moreover, we provide evidence that a predicted cation/H+ antiporter, AdaE, is involved in the chlorination step during 2′-Cl PTN biosynthesis. Notably, we demonstrate that 2′-amino dA biosynthesis is initiated by a Nudix hydrolase, AdaJ, catalyzing the hydrolysis of ATP. Finally, we reveal that the host ADA (designated ADA1), capable of converting adenosine/2′-amino dA to inosine/2′-amino dI, is not very sensitive to the powerful ADA inhibitor pentostatin. These findings provide a basis for the further rational pathway engineering of 2′-Cl PTN and 2′-amino dA production.IMPORTANCE 2′-Cl PTN/PTN and 2′-amino dA have captivated the great interests of scientists, owing to their unusual chemical structures and remarkable bioactivities. However, the precise logic for their biosynthesis has been elusive for decades. Actually, the identification and elucidation of their biosynthetic pathways not only enrich the biochemical repertoire of novel enzymatic reactions but may also lay solid foundations for the pathway engineering and combinatorial biosynthesis of this family of purine nucleoside antibiotics to generate novel hybrid analogs with improved features.
研究领域:
微生物学
·
分子生物学
·
药物化学
✓ 已验证
DOI
PubMed
高影响因子
Carbon Capture Science & Technology
·
2024
·
IF 10.4
Xiaobin Zhou,Yunqiong Tang,Chao Liu,Shengpeng Mo,Yinming Fan,Dunqiu Wang,Bihong Lv,Yanan Zhang,Yinian Zhu,Zongqiang Zhu,Guohua Jing
To tackle the prevalent challenges encountered with polyamine-based non-aqueous absorbents (NAAs), particularly the formation of viscous products and inferior regeneration performance, this study proposed an innovative synergistic regulation strategy that integrated 2-amino-2-methyl-1-propanol (AMP) and n-propanol (NPA). Accordingly, a novel tertiary tetraethylenepentamine (TEPA)-AMP-NPA (T-A-N) NAA was devised. The optimized T-A-N maintained complete homogeneity throughout the entire CO 2 absorption process and achieved an impressive CO 2 loading of 1.15 mol·mol −1 while maintaining a low viscosity of merely 22.47 mPa·s. Remarkably, its absorption capacity showed little decrement after four consecutive absorption-desorption cycles, underscoring its exceptional recyclability. Within the T-A-N system, AMP underwent a reaction with CO 2 , yielding AMP-carbamate and protonated AMP, while TEPA engaged in CO 2 absorption to form zwitterionic carbamates. During the desorption process, NPA served as a regeneration activator, facilitating the conversion of stable TEPA-carbamates into less stable alkyl carbonate intermediates, thereby enhancing the T-A-N's regeneration performance. Moreover, the T-A-N system addressed the issue of TEPA-carbamate self-aggregation into insoluble gelatinous substances by leveraging the synergistic enhancement effects between AMP derivatives and NPA. Specifically, these components effectively bound TEPA-carbamate species via robust electrostatic affinity and intermolecular hydrogen-bond interactions, inhibiting their self-aggregation and preventing the formation of insoluble products. Furthermore, T-A-N exhibited a significant reduction in both sensible and latent heat requirements, by 67 % and 82 % respectively, compared to 30 wt% MEA, highlighting its advantageous energy-saving potential for CO 2 capture. Overall, harnessing the synergistic enhancement effects of AMP and NPA was conducive to the development of polyamine-based NAAs that offered superior CO 2 capture reversibility, low energy consumption, and resistance to insoluble product formation.
研究领域:
化学工程
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
Desalination and Water Treatment
·
2015
·
IF 1.173
Ben Zhang,Juan Li,Xiaogai Lv,Yuanchen Cui,Ying Xu
Polyaspartic acid/2-amino-2-methyl-1,3-propanediol graft copolymer, a novel non-phosphorus scale and corrosion inhibitor, was synthesized and characterized by infrared spectroscopy. Its performance was evaluated by static scale inhibition method and dynamic corrosion testing. It was found that the graft copolymer showed excellent inhibition ability against CaCO3, CaSO4, and Ca3(PO4)2 scales and a definite inhibition corrosion performance as well. The inhibition efficiency was close to 99.9% against CaCO3, CaSO4, and Ca3(PO4)2 when the inhibitor was at an appropriate concentration. The inhibitor had still possessed higher antiscale efficiency against CaCO3 with increasing concentration of Ca2+ and heating time. In addition, The graft copolymer could change the structure of crystals CaCO3, CaSO4, and Ca3(PO4)2 by observation of scanning electron microscopy.
研究领域:
材料科学
·
化学工程
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Anteng Dai,Xu Chen,Hengyu Li,Zhangfeng Dong,Xiaoyun Chen,Qinghai Long,Bihong Lv,Zuoming Zhou,Guohua Jing
Solid-liquid biphasic solvents(SLBS) are considering as promising absorption for CO 2 chemical capture because of their potential energy-saving potential and easily separation of solid products. Nevertheless most of the SLB systems still with some defects, such as premature phase transition and viscous solid products. This work proposed a novel non-aqueous biphasic absorbent with controllable solid–liquid phase transition, composed of piperazine (PZ), 2-amino-2-methyl-1-propanol (AMP), and N-methylformamide (NMF). When NMF is 90 % by volume as solvent and the volume ratio of PZ and AMP is 3:1, the absorbent maintained a homogeneous phase with CO 2 loading below 0.729 mol/mol, which was about 60.6 % of the saturated loading (1.202 mol/mol). As the loading further increased, the solid products generated and the solution separated into solid–liquid two phases. And the solid product into the saturated solution was only 14 % of the total volume while contained about 93.29 % of total loading. The phase-transition mechanism was investigated by using 13 C NMR analysis and molecular simulations. Due to the higher reactivity of PZ with CO 2 compared to AMP, CO 2 initially reacted with PZ to form PZCOO − and PZH + . The enhanced polarity of the final products, PZ(COO − ) 2 and PZ(H + ) 2 , together with a marked increase in ESP difference, promotes the formation of small-volume, CO 2 -rich solids in the later stages of absorption. During this process, intermediate products (PZCOO − and PZH + ) interact with AMPCOO − and AMPH + , allowing early-stage dissolution of products in the solvent and ultimately producing easily separable solids with high CO 2 enrichment. The regeneration heat duty of the novel SLBS was estimated about 0.76 GJ/ton CO 2 , representing just 20.0 % of the industry standard for MEA (3.80 GJ/ton CO 2 ), which indicated extremely energy-saving advantage of the novel solvent.
研究领域:
化学工程
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Xiaoyi Gao,Xin Li,Siyi Cheng,Bihong Lv,Guohua Jing,Zuoming Zhou
The main issues in the application of biphasic amine absorbent include the inconvenient separation of the liquid–liquid biphase and the clogging that is associated with the solid–liquid mixture. A novel solid–liquid ‘phase controllable’ biphasic amine absorbent was therefore developed, in which the phase separation occurred only when the absorbent was near saturation. The absorbent, composed of triethylene tetramine (TETA), 2-amino-2-methyl-1-propanol (AMP), and N-methylformamide (NMF), turned into solid–liquid biphase under CO 2 loading of 0.85 mol mol −1 , which is close to saturation (0.92 mol mol −1 ). The solid phase comprised white powder that accounted for only 42 % of the total volume while absorbing 91 % of the total load. Turbidity and particle size tests showed that the phase separation was self-aggregating. The mechanisms of absorption and regulation were obtained using 13 C NMR and molecular simulation. During the absorption, CO 2 first combined with TETA to generate TETAH + CO 2 – /TETACO 2 – through the zwitterion mechanism, and then combined with AMP to generate AMPCO 2 – because of the lower reaction activity between CO 2 and AMP. The TETA-carbamate was found to greatly weakened the strength of the hydrogen bonds and the van der Waals forces between AMPH + and AMPCO 2 – , increasing the solubility of the intermediate products, and therefore achieved the purpose of controlling the phases separation inherent in the reaction.
研究领域:
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Shanlong An,Xin Huang,Nuo Li,Qiangwei Li,Tieyue Qi,Rujie Wang,Lidong Wang
2-amino-2-methyl-1-propanol (AMP) combines the advantages of the faster reaction rate of primary/secondary amines and the high absorption capacity of tertiary amines, making it a highly promising alternative to monoethanolamine (MEA). However, at high AMP concentrations, the absorption products are prone to solid crystallization, resulting in unstable operation of the carbon capture system. In this work, by adding a small amount of diethylenetriamine (DETA) to AMP, the crystallization of reaction products can be effectively controlled and AMP-DETA absorbent possesses a high absorption rate, low regeneration energy, and low metal corrosion rate. Wetted-wall column tests were performed to comprehensively evaluate the mass transfer kinetics and the effect of crucial conditions, and the diffusion coefficient, gas–liquid mass transfer coefficient, enhancement factor, and mass transfer resistance distribution were obtained. The effect of the addition of DETA on the solubility of HCO 3 − was verified. DETA carbamate was more likely to form intermolecular hydrogen bonds with HCO 3 − , thus reducing the formation of dimeric or multichain macromolecules between HCO 3 − molecules through hydrogen bonds and inhibiting the crystallization of high concentration HCO 3 − . HCO 3 − can accelerate the desorption rate by participating in the deprotonation of protonation amines. The results demonstrated that the average regeneration energy of the AMP–DETA absorption system was reduced by 21.2 % relative to that of 5 M MEA, and its metal corrosion rate was 0.07 mm/a, which was only 7.9 % of MEA under the same conditions. The results contribute to the industrial application of AMP–DETA.
研究领域:
化学工程
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Pan Xiao,Jingjing Xiao,Zhihong Xiao,Rukuan Liu,Zhiyong Zhang,Chuansheng Chen,Changzhu Li
Herein, a novel surfactant dihexyl (2-amino-2-(hydroxyimino)ethyl) phosphonate (DHAHEP) was synthesized by combining phosphonate and amidoxime groups in the same molecule, and used as a flotation collector for quartz vein-type wolframite. The Micro-flotation results showed that DHAHEP has excellent collection performance for wolframite, at pH 2 ∼ 4.5, the flotation recovery of DHAHEP for wolframite was over 90 %, while that for quartz was less than 60 %. The wolframite-quartz artificial mixed ores experiments demonstrated that at pH ∼ 4 and DHAHEP concentration of 8 × 10 -5 mol·L -1 , the flotation recovery of wolframite was 64.5 % and the grade was 48.9 %. Zeta potential and contact angle experiments elucidated that DHAHEP anchored on the wolframite surface mainly in the form of cations, increasing the hydrophobicity of the surface and thus separating the wolframite from quartz by flotation. FTIR, XPS, and DFT calculation further revealed that DHAHEP had an obvious flotation separation effect on quartz vein-type wolframite, it was mainly electrostatically adsorbed on the WO 4 2- sites of the wolframite surface in the form of cations, and also captured wolframite by forming chemical bonds with the Fe active sites through the phosphoryl and amidoxime groups in its molecular structure.
研究领域:
矿物加工工程
·
表面化学
✓ 已验证
产品关联
DOI
高影响因子
ENERGY
·
2023
·
IF 9
Xiaobin Zhou,Chao Liu,Jie Zhang,Yinming Fan,Yinian Zhu,Lihao Zhang,Shen Tang,Shengpeng Mo,Hongxiang Zhu,Zongqiang Zhu
Biphasic solvents are regarded as promising candidates for CO 2 capture but still suffer from the deficiency of inferior regenerability, which negatively affects their energy-saving potential. 2-Amino-2-methyl-1-propanol (AMP)-based absorbents have superior regenerability but poor phase-change performance. In this study, an effective strategy that using tetraethylenepentamine (TEPA) to regulate the phase change behavior of an AMP-pentamethyldiethylenetriamine (PMDETA) aqueous solution was proposed, aiming to develop a novel AMP-PMDETA-TEPA (A-P-T) biphasic solvent with good regenerability and excellent phase separation performance. The A-P-T biphasic solvent could realize a high CO 2 loading of 0.73 mol mol −1 and a high desorption efficiency of 75.3%. Its sensible heat requirement significantly decreased to 0.14 GJ·ton −1 CO 2 , 78.1% less than the monoethanolamine solution. The 13 C NMR characterization and quantum chemistry calculations indicated that with the introduction of TEPA, high polar TEPA-associated products were generated, which broke the original assimilation state of the A-P-T system and drove it to undergo phase change. Since the TEPA-associated products had a strong affinity to other CO 2 -captured products and H 2 O, they gathered together to form the CO 2 -rich phase. In contrast, less polar PMDETA showed a relatively weak affinity to the TEPA-associated products and was solely separated from the solution to form the CO 2 -lean phase.
研究领域:
化学工程
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环境科学
·
能源技术
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Zhifang Tu,Fei Han,Chao Liu,Yingxue Wang,Jianwen Wei,Xiaobin Zhou
Solid-liquid phase-change absorbents (SLPCAs) have a great potential to reduce the energy consumption of CO 2 capture. The main issue in the practical application of SLPCAs is the difficulty in the phase separation of gelatinous solid products. In this study, 2-amino-2-methyl-1-propanol (AMP) was used as a regulator to tune the physical form of the solid products of triethylenetetramine (TETA)-based SLPCAs. Experimental results showed that the AMP-regulated TETA-based SLPCAs successfully avoided the formation of gelatinous products (viscosity up to more than 1000 mPa·s) and yielded easily separated crystalline powders. Among the investigated SLPCAs, TETA/AMP/ N -methyl-2-pyrrolidone (NMP) (TETA:AMP = 2:8, 1 M) exhibited the best CO 2 capture performance with a high CO 2 loading of 0.94 mol·mol −1 and a high regeneration efficiency of 84.14 %. XRD, FT-IR and 13 C NMR analyses indicated that TETA/AMP/NMP absorbed CO 2 to form highly polar carbamate species and protonated amines, which could break the original assimilation state of the SLPCA system; thus, the polar products precipitated out from less polar NMP, leading to a phase change. The theoretical calculations revealed that in the absence of AMP, the TETA-derived products had a tendency to form gelatinous aggregation with large amounts of hydrogen bonds; with the introduction of AMP, the AMP-derived products tended to combine with the TETA-derived products via strong electrostatic attraction and Van der Waals force and effectively inhibited the aggregation formation. Since there was only one hydrogen bond forming between the AMP- and TETA-derived product molecules, the amount of hydrogen bonds was significantly reduced. Eventually, the TETA/AMP/NMP SLPCA avoided the formation of gelatinous products and yielded crystalline powder products.
研究领域:
化学工程
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）