Membranes
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2021
·Vol. 11
·期 2
·142
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IF 4.106
Junjie Yu,Kaifeng Gu,Binbin Yang,Kaizhen Wang,Yong Zhou,Congjie Gao
The work briefly introduces the nano-composite reverse osmosis (RO) membrane with more permeability and selective performance, and we adopted the phenyltrichlorosilane precursor with better chemical stability and greater spatial resistance. The phenyltrichlorosilane concentration was mainly discussed in this work. The in-situ hydrolysis of phenyltrichlorosilane and the occurrence of ammonia hydrolysis make it effectively incorporated into the polyamide film. The covalent bond and hydrogen bond of phenyltrichlorosilane and polyamide (PA) can be realized. The phenyl group can extend in the polyamide polymer network and give the film corresponding functions. There will be fewer non-selective defects between phenyltrichlorosilane and PA. Under the premise of maintaining the water-salt selectivity of the membrane, along with the increase of benzene trichlorosilane loading, the 300% pure water flux can be achieved and the desalination rate remains at 98.1–98.9%. This reverse osmosis (RO) is suitable for household water purification.Keywords:polyamide film;phenyltrichlorosilane;situ hydrolysis;ammonia hydrolysis
研究领域:
材料科学
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环境工程
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PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
·
IF 8.1
Ruizhuo Liu,Jian Cao,Zhongwei Zhao,Yongli Li
Solvent extraction with organophosphorus extractants has potential as a low-cost method for efficient Mo recovery for acidic leaching solutions. However, improved selectivity is required to obtain high-purity Mo products. In this study, various acidic organophosphorus extractants were compared, and 2-ethylhexylphosphonic acid mono-(2-ethylhexyl) ester (P507) was found to be optimal for efficient Mo extraction and Fe separation from acidic leaching solutions. Under the optimized conditions (40 vol% P507, 3:1 organic/aqueous, 20 °C, 5 min), the Mo and Fe extraction efficiencies reached 98.1 % and 35.2 %, respectively, with a separation factor of 90.1. The Mo/Fe separation efficiency was further improved using a two-stage countercurrent extraction method. The Mo extraction efficiency was attributed to coordination bonds (P = O → Mo) formed between Mo(VI) oxycations and P507 dimers, as well as covalent bonds (P O Mo) formed by substituting the hydrogen ions in P507. Increasing the H 2 SO 4 concentration in the leaching solution gradually transformed MoO 2 2+ into Mo 2 O 5 2+ dimers, which formed MoO 2 (HA 2 ) 2 and Mo 2 O 5 (HA 2 ) 2 metal complexes during the extraction process. HCl scrubbing of the loaded organic phase effectively removed Fe. For subsequent ammonia stripping of the HCl-scrubbed organic phase, the optimal ammonia concentration was 1.25 mol/L. Further increasing the ammonia concentration promoted the saponification reaction of ammonia with P507, thereby reducing the Mo stripping efficiency. In summary, using multistage countercurrent extraction, increasing the H 2 SO 4 concentration in the leaching solution, and scrubbing the loaded organic phase with HCl facilitate efficient Mo/Fe separation, providing a feasible approach for the preparation of high-purity ammonium molybdate with broad application prospects.
研究领域:
冶金化学
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环境工程
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DOI
高影响因子
Journal of Physical Chemistry C
·
2024
·
IF 3.3
Zhi-Qiang Wang,Wanjun Guo,Shengchao Jia,Yaxuan Jing,Shiting Li,Yong Guo,Xiaohui Liu,Xue-Qing Gong,Yanqin Wang
The selective production of primary amines through reductive amination has received increasing attention due to their extensive applications, while efficient reductive amination is still challenging. Herein, a novel strategy was developed to realize the efficient reductive amination of carbonyl compounds with NH3 via d–d orbital coupling strategies in RuCo alloys. The designed series of RuCo alloy catalysts not only exhibited excellent performance in conversion of various substrates but also demonstrated universal applicability across different supports. The key role of RuCo alloy is its unique ability to effectively catalyze the ammonolysis of a Schiff base, the rate-determining step in reductive amination. Theoretical studies reveal that the d–d orbital coupling strategies break the five d orbital equivalent contributions of metal (Co or Ru) atoms, and the d orbitals primarily contribute through the dz2 and dx2-y2 orbitals of Ru and the dz2 orbital of Co on the RuCo(001) surface, which significantly driving the homolytic NH3 dissociation during the ammonolysis of the Schiff base. Furthermore, stable Co–H covalent bond species and RuCo-NH2 half-ionic and half-covalent bond species on the RuCo(001) surface were generated with lower energy levels. This work not only achieves efficient reductive amination but also provides an atomic orbital-level understanding of the d–d orbital coupling strategies for heterogeneous catalysis.
研究领域:
催化化学
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材料科学
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理论化学
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DOI
高影响因子
ENZYME AND MICROBIAL TECHNOLOGY
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2024
·
IF 3.4
Jiangmei Zheng,Ruobin Sun,Dan Wu,Pengcheng Chen,Pu Zheng
Phenylalanine ammonia-lyase (PAL) plays a pivotal role in the biosynthesis of phenylalanine. PAL from Zea mays (ZmPAL2) exhibits a bi-function of direct deamination of L-phenylalanine (L-Phe) or L-tyrosine(-L-Tyr) to form trans -cinnamic acid or p -coumaric acid. trans -Cinnamic acid and p -coumaric acid are mainly used in flavors and fragrances, food additives, pharmaceutical and other fields. Here, the Activity of ZmPAL2 toward L-Phe or L-Tyr was improved by using semi-rational and rational designs. The catalytic efficiency ( k cat / K m ) of mutant PT10 (V258I/I459V/Q484N) against L-Phe was 30.8 μM −1 s −1 , a 4.5-fold increase compared to the parent, and the catalytic efficiency of mutant PA1 (F135H/I459L) to L-tyrosine exhibited 8.6 μM −1 s −1 , which was 1.6-fold of the parent. The yield of trans -cinnamic acid in PT10 reached 30.75 g/L with a conversion rate of 98%. Meanwhile, PA1 converted L-Tyr to yield 3.12 g/L of p -coumaric acid with a conversion rate of 95%. Suggesting these two engineered ZmPAL2 to be valuable biocatalysts for the synthesis of trans -cinnamic acid and p -coumaric acid. In addition, MD simulations revealed that the underlying mechanisms of the increased catalytic efficiency of both mutant PT10 and PA1 are attributed to the substrate remaining stable within the pocket and closer to the catalytically active site. This also provides a new perspective on engineered PAL.
研究领域:
生物化学
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分子生物学
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PubMed
高影响因子
RSC Advances
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2015
·Vol. 5
·期 28
·22289-22293
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IF 3.84
Qiyi Lu,Juanjuan Zhang,Yuanya Wu,Ruo Yuan,Shihong Chen
The cathodic electrochemiluminescence (ECL) behavior of the ammonolysis product of 3,4,9,10-perylenetetracarboxylic dianhydride (PTC–NH2) in aqueous solution with K2S2O8 as the co-reactant has been, for the first time reported, in this paper. The possible mechanisms have been investigated. Based on the fact that dopamine (DA) can efficiently quench the ECL intensity of PTC–NH2, DA was chosen as a template to investigate the application of PTC–NH2–S2O82− system in the sensor field. Under the optimal conditions, we achieved the detection of DA with the detection limit of 1.6 × 10−9 M. Due to the excellent ECL behavior, PTC–NH2 could be a new class of promising material for the construction of ECL sensors.
研究领域:
分析化学
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生物传感
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材料科学
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DOI
高影响因子
ACS Applied Materials & Interfaces
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2024
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IF 8.3
Qihui Huang,Hui Zheng,Xia Wang,Qi Fu,Tao Gong,Chang Liu,Huijuan Ma,Linmin Ye,Xinping Duan,Youzhu Yuan
Hexamethylene diamine, an important chemical intermediate for polyamides, can be synthesized through the two-step route of caprolactam (CPL) ammonolysis to 6-aminocapronitrile (ACN), followed by hydrogenation. This method has received increasing attention from academia and industry. However, studies on the catalyst structure–performance correlation in CPL ammonolysis are still sporadic. In this work, a series of anatase TiO2 with different oxygen vacancy concentrations was prepared by chemical reduction using NaBH4. The oxygen vacancy on TiO2 surface, presented as Ti3+ sites, substantially enhances the adsorption and activation of NH3, which are demonstrated as the key steps in ammonolysis. Owing to the synergistic effect of Ti3+ and Ti4+ species, the CPL conversion rate and ACN selectivity of 85 and 97%, respectively, are achieved within 250 h. Density functional theory calculations showed that the intermediates on oxygen vacancy-rich TiO2 had a more favorable adsorption energy compared to those on intact TiO2, which is in good agreement with the experimental results.
研究领域:
材料科学
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催化化学
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DOI
PubMed
高影响因子
Scientific Reports
·
2015
·Vol. 5
·期 1
·1-13
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IF 5.578
Cui Jiandong,Jia Shiru,Liang Longhao,Zhao Yamin,Feng Yuxiao
A novel enzyme immobilization approach was used to generate mesoporous enzymes-silica composite microparticles by co-entrapping gelatinized starch and cross-linked phenylalanine ammonia lyase (PAL) aggregates (CLEAs) containing gelatinized starch into biomemitic silica and subsequently removing the starch by α-amylase treatment. During the preparation process, the gelatinzed starch served as a pore-forming agent to create pores in CLEAs and biomimetic silica. The resulting mesoporous CLEAs-silica composite microparticles exhibited higher activity and stability than native PAL, conventional CLEAs and PAL encapsulated in biomimetic silica. Furthermore, the mesoporous CLEAs-silica composite microparticles displayed good reusability due to its suitable size and mechanical properties and had excellent stability for storage. The superior catalytic performances were attributed to the combinational unique structure from the intra-cross-linking among enzyme aggregates and hard mesoporous silica shell, which not only decreased the enzyme-support negative interaction and mass-transfer limitations, but also improved the mechanical properties and monodispersity. This approach will be highly beneficial for preparing various bioactive mesoporous composites with excellent catalytic performance.
研究领域:
生物化学
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材料科学
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DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2018
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IF 3.909
Wei Li,Yun Yang,Chong Qiao,Guolin Zhang,Yinggang Luo
Galanthamine (GAL), the well-known Amaryllidaceae alkaloid, is a clinically used drug for the treatment of Alzheimer's disease. L-Phenylalanine (Phe) and trans -cinnamic acid (CA) were enzymatically transformed into the catechol portion of GAL. Herein, a Phe ammonia-lyase-encoding gene LrPAL3 and a cinnamate 4-hydroxylase-encoding gene LrC4H were cloned from Lycoris radiata , a GAL-producing plant. LrPAL3 was overexpressed in Escherichia coli and purified to homogeneity. LrPAL3 catalyzes the forward deamination conversion of L-Phe into trans -CA. The 3-chloro- and 4-fluoro-L-Phe were deaminated to generate the corresponding 3-chloro- and 4-fluoro- trans -CA by LrPAL3. LrPAL3-catalyzed reverse hydroamination was confirmed by the conversion of trans -CA into L-Phe with exceptional regio- and stereo-selectivity. LrC4H was overexpressed in E. coli with tCamCPR , a cytochrome P450 reductase-encoding gene. LrC4H catalyzes the regioselective para -hydroxylation on trans -CA to form p -coumaric acid. The transcriptional levels of both LrPAL3 and LrC4H were positively associated with the GAL contents within the leaves and flowers of L. radiata , which suggested that their expression and function are co-regulated and involved in the biosynthesis of GAL. The present investigations on the biosynthetic genes of GAL will promote the development of synthetic biology platforms for this kind of important drug via metabolic engineering.
研究领域:
植物生物化学
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分子生物学
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药理学
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合成生物学
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PubMed
高影响因子
Polymer Chemistry
·
2018
·Vol. 9
·期 28
·3931-3943
·
IF 4.927
Yawei Sun,Qiuyan Wang,Shuying Zhang,Hao Li,Jinli Zhang,Daqing Li,Wei Li
A novel aromatic-doped polycaprolactone (Aro-PCL) material was synthesized through a facile PCL aminolysis-condensation polymerization incorporating the aromatic moiety to PCL chain and assessed by focusing on the dynamic aggregation and crystalline microdomains associated with the in vitro degradation properties, mechanical performance and biocompatibility. Characterizations by FTIR, NMR, UV-vis, DSC, WAXD, SAXS, POM, etc. illustrated that the incorporated aromatic and amine segments facilitated the formation of many low-oriented crystalline domains along the aliphatic chains. The results indicated that the evolution of mechanical performance is significantly associated with the chemical structure and the crystallization behavior of polymers. The Aro-PCL films possessed fast degradation rate, excellent biocompatibility and improved mechanical performance including augmented elongation at break, elastic modulus and radial strength. In particular, the Aro-PCL polymer films showed decrease in molecular weight at the beginning of hydrolytic degradation while maintaining mechanical support and stable mass. The Aro-PCL polymer has promising applications as a degradable biomaterial.
研究领域:
材料科学
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高分子化学
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生物医学工程
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生物材料
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DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2023
·
IF 16.5
Wanjun Guo,Zhi-Qiang Wang,Shuang Xiang,Yaxuan Jing,Xiaohui Liu,Yong Guo,Xue-Qing Gong,Yanqin Wang
ABSTRACT Owing to the wide application of primary amines, their selective production via reductive amination has become a crucial research topic. Various metal-supported catalysts (Pt, Ru, Rh, Ir, Co, Ni, etc. ) have been investigated, and metallic species have been recognized as active sites in recent years. Herein, we reveal for the first time that CoO species containing oxygen vacancies within a core-shell-structured Co@CoO catalyst accelerate the ammonolysis of Schiff bases, key intermediates in reductive amination, through NH 3 dissociation to hydride-like NH 2 δ – species, delivering an excellent reductive amination performance. The catalyst is highly stable and was utilized in 10 catalytic cycles for the amination of biomass-derived cyclopentanone (CPO) to cyclopentylamine (CPA) without deactivation. Various computational models in combination with spectroscopic measurements indicated that this catalyst not only drives the dissociation of H 2 to the active H δ – species, but also enables the homolytic cleavage of NH 3 to NH 2 δ – . D 2 isotopic tracing experiments provided further evidence of the direct involvement of hydride-like NH 2 δ – species in Schiff base ammonolysis. Theoretical calculations verified the stable co-adsorption of H δ – and NH 2 δ – , which allows the Schiff base to move freely on the surface of the CoO shell and participate extensively in molecular collisions, resulting in exceptional catalytic activity. This is the first study that demonstrates the potential of metal oxide catalysts for the production of primary amines via reductive amination.
研究领域:
催化
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化学工程
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材料科学
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物理化学
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DOI
高影响因子
Cell Host & Microbe
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2024
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IF 20.6
Haiyuan Shen,Liangliang Zhou,Hao Zhang,Yuanru Yang,Ling Jiang,Dongqing Wu,Hang Shu,Hejiao Zhang,Linxi Xie,Kaichen Zhou,Chen Cheng,Lei Yang,Jiali Jiang,Siya Wang,Yiran Han,Jiayi Zhu,Long Xu,Zhihua Liu,Hua Wang,Shi Yin
The gut microbiota and diet-induced changes in microbiome composition have been linked to various liver diseases, although the specific microbes and mechanisms remain understudied. Alcohol-related liver disease (ALD) is one such disease with limited therapeutic options due to its complex pathogenesis. We demonstrate that a diet rich in soluble dietary fiber increases the abundance of Bacteroides acidifaciens (B. acidifaciens) and alleviates alcohol-induced liver injury in mice. B. acidifaciens treatment alone ameliorates liver injury through a bile salt hydrolase that generates unconjugated bile acids to activate intestinal farnesoid X receptor (FXR) and its downstream target, fibroblast growth factor-15 (FGF15). FGF15 promotes hepatocyte expression of ornithine aminotransferase (OAT), which facilitates the metabolism of accumulated ornithine in the liver into glutamate, thereby providing sufficient glutamate for ammonia detoxification via the glutamine synthesis pathway. Collectively, these findings uncover a potential therapeutic strategy for ALD involving dietary fiber supplementation and B. acidifaciens.
研究领域:
胃肠病学
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肝病学
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微生物学
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营养学
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DOI
PubMed
高影响因子
JOURNAL OF FLUORESCENCE
·
2023
·Vol. 33
·期 4
·1305-1315
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IF 2.7
Wang Rui,Li Shumiao,Huang Hanjiang,Liu Botong,Gao Lu,Qu Meiru,Wei Yanying,Wei Jianfei
An environmentally friendly PET-based Carbon Dots (PET-CDs) with excellent fluorescence properties were prepared with waste PET bottle, pyromellitic acid and ammonia water as raw materials by one-step hydrothermal method. The preparation mechanism of PET-CDs was as follows: PET first underwent ammonolysis reaction to produce terephthalic acid diamide and ethylene glycol, and then dehydrated and carbonized with pyromellitic acid to form PET-CDs. The as-prepared PET-CDs exhibit excitation-independent emission properties in the range from 340 to 440 nm, and the fluorescence quantum yield is as high as 87.36%. In terms of structure, PET-CDs is a spherical structure with an average particle size of 2.0 nm, and its surface contains carboxyl and amino groups. The PET-CDs were dispersed in a PVA matrix to obtain an light blocking films(LBFs) for 250–450 nm light with excellent properties, and its transparency for 450–700 nm light is good. In addition, PET-CDs was used in the fields of LED, and it was found that the color coordinate for the LED assembled with PET-CDs and 395 nm LED chips is (0.55, 0.44) and the correlated color temperature is 2018 K.
研究领域:
材料科学
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环境科学
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纳米技术
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光电技术
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产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）